WorldWideScience

Sample records for surface pd atoms

  1. Ab initio thermodynamic evaluation of Pd atom interaction with CeO(2) surfaces.

    Science.gov (United States)

    Mayernick, Adam D; Janik, Michael J

    2009-08-28

    Palladium supported on ceria is an effective catalytic material for three-way automotive catalysis, catalytic combustion, and solid-oxide fuel cell (SOFC) anodes. The morphology, oxidation state, and particle size of Pd on ceria affect catalytic activity and are a function of experimental conditions. This work utilizes ab initio thermodynamics using density functional theory (DFT) (DFT+U) methods to evaluate the stability of Pd atoms, PdO(x) species, and small Pd particles in varying configurations on CeO(2) (111), (110), and (100) single crystal surfaces. Over specific oxygen partial pressure and temperature ranges, palladium incorporation to form a mixed surface oxide is thermodynamically favorable versus other single Pd atom states on each ceria surface. For example, Pd atoms may incorporate into Ce fluorite lattice positions in a Pd(4+) oxidation state on the CeO(2) (111) surface. The ceria support shifts the transition between formal Pd oxidation states (Pd(0), Pd(2+), Pd(4+)) relative to bulk palladium and stabilizes certain oxidized palladium species on each surface. We show that temperature, oxygen pressure, and cell potential in a SOFC can influence the stable states of palladium supported on ceria surfaces, providing insight into structural stability during catalytic operation.

  2. Atom condensation on an atomically smooth surface: Ir, Re, W, and Pd on Ir(111)

    International Nuclear Information System (INIS)

    Wang, S.C.; Ehrlich, G.

    1991-01-01

    The distribution of condensing metal atoms over the two types of sites present on an atomically smooth Ir(111) has been measured in a field ion microscope. For Ir, Re, W, and Pd from a thermal source, condensing on Ir(111) at ∼20 K, the atoms are randomly distributed, as expected if they condense at the first site struck

  3. The atomic structure of low-index surfaces of the intermetallic compound InPd

    Energy Technology Data Exchange (ETDEWEB)

    McGuirk, G. M.; Ledieu, J.; Gaudry, É.; Weerd, M.-C.; Fournée, V. de, E-mail: vincent.fournee@univ-lorraine.fr [Institut Jean Lamour (UMR 7198 CNRS-Université de Lorraine), Parc de Saurupt, F-54011 Nancy Cedex (France); Hahne, M.; Gille, P. [Department of Earth and Environmental Sciences, Crystallography Section, Ludwig-Maximilians-Universität München, Theresienstrasse 41, D-80333 München (Germany); Ivarsson, D. C. A.; Armbrüster, M. [Faculty of Natural Sciences, Institute of Chemistry, Materials for Innovative Energy Concepts, Technische Universität Chemnitz, D-09107 Chemnitz (Germany); Ardini, J.; Held, G. [Department of Chemistry, University of Reading, Reading RG6 6AD (United Kingdom); Diamond Light Source Ltd, Didcot OX11 0DE (United Kingdom); Maccherozzi, F. [Diamond Light Source Ltd, Didcot OX11 0DE (United Kingdom); Bayer, A. [Lehrstuhl für Physikalische Chemie II, Universität Erlangen-Nürnberg, Egerlandstraße 3, D-91058 Erlangen (Germany); Lowe, M. [Surface Science Research Centre and Department of Physics, The University of Liverpool, Liverpool L69 3BX (United Kingdom); Pussi, K. [Department of Mathematics and Physics, Lappeenranta University of Technology, P.O. Box 20, FIN-53851 Lappeenranta (Finland); Diehl, R. D. [Department of Physics, Penn State University, University Park, Pennsylvania 16802 (United States)

    2015-08-21

    The intermetallic compound InPd (CsCl type of crystal structure with a broad compositional range) is considered as a candidate catalyst for the steam reforming of methanol. Single crystals of this phase have been grown to study the structure of its three low-index surfaces under ultra-high vacuum conditions, using low energy electron diffraction (LEED), X-ray photoemission spectroscopy (XPS), and scanning tunneling microscopy (STM). During surface preparation, preferential sputtering leads to a depletion of In within the top few layers for all three surfaces. The near-surface regions remain slightly Pd-rich until annealing to ∼580 K. A transition occurs between 580 and 660 K where In segregates towards the surface and the near-surface regions become slightly In-rich above ∼660 K. This transition is accompanied by a sharpening of LEED patterns and formation of flat step-terrace morphology, as observed by STM. Several superstructures have been identified for the different surfaces associated with this process. Annealing to higher temperatures (≥750 K) leads to faceting via thermal etching as shown for the (110) surface, with a bulk In composition close to the In-rich limit of the existence domain of the cubic phase. The Pd-rich InPd(111) is found to be consistent with a Pd-terminated bulk truncation model as shown by dynamical LEED analysis while, after annealing at higher temperature, the In-rich InPd(111) is consistent with an In-terminated bulk truncation, in agreement with density functional theory (DFT) calculations of the relative surface energies. More complex surface structures are observed for the (100) surface. Additionally, individual grains of a polycrystalline sample are characterized by micro-spot XPS and LEED as well as low-energy electron microscopy. Results from both individual grains and “global” measurements are interpreted based on comparison to our single crystals findings, DFT calculations and previous literature.

  4. Ab Initio Density Functional Calculations and Infra-Red Study of CO Interaction with Pd Atoms on θ-Al2O3 (010) Surface.

    Science.gov (United States)

    Narula, Chaitanya K; Allard, Lawrence F; Wu, Zili

    2017-07-24

    The ab initio density functional theoretical studies show that energetics favor CO oxidation on single Pd atoms supported on θ-alumina. The diffuse reflectance infra-red spectroscopy (DRIFTS) results show that carbonates are formed as intermediates when single supported Pd atoms are exposed to a gaseous mixture of CO + O 2 . The rapid agglomeration of Pd atoms under CO oxidation conditions even at 6 °C leads to the presence of Pd particles along with single atoms during CO oxidation experiments. Thus, the observed CO oxidation has contributions from both single Pd atoms and Pd particles.

  5. Single Pd Atoms on θ-Al2O3 (010) Surface do not Catalyze NO Oxidation.

    Science.gov (United States)

    Narula, Chaitanya K; Allard, Lawrence F; Moses-DeBusk, Melanie; Stocks, G Malcom; Wu, Zili

    2017-04-03

    New convenient wet-chemistry synthetic routes have made it possible to explore catalytic activities of a variety of single supported atoms, however, the single supported atoms on inert substrates (e.g. alumina) are limited to adatoms and cations of Pt, Pd, and Ru. Previously, we have found that single supported Pt atoms are remarkable NO oxidation catalysts. In contrast, we report that Pd single atoms are completely inactive for NO oxidation. The diffuse reflectance infra-red spectroscopy (DRIFTS) results show the absence of nitrate formation on catalyst. To explain these results, we explored modified Langmuir-Hinshelwood type pathways that have been proposed for oxidation reactions on single supported atom. In the first pathway, we find that there is energy barrier for the release of NO 2 which prevent NO oxidation. In the second pathway, our results show that there is no driving force for the formation of O=N-O-O intermediate or nitrate on single supported Pd atoms. The decomposition of nitrate, if formed, is an endothermic event.

  6. Atomic Structure of Au−Pd Bimetallic Alloyed Nanoparticles

    KAUST Repository

    Ding, Yong

    2010-09-08

    Using a two-step seed-mediated growth method, we synthesized bimetallic nanoparticles (NPs) having a gold octahedron core and a palladium epitaxial shell with controlled Pd-shell thickness. The mismatch-release mechanism between the Au core and Pd shell of the NPs was systematically investigated by high-resolution transmission electron microscopy. In the NPs coated with a single atomic layer of Pd, the strain between the surface Pd layer and the Au core is released by Shockley partial dislocations (SPDs) accompanied by the formation of stacking faults. For NPs coated with more Pd (>2 nm), the stacking faults still exist, but no SPDs are found. This may be due to the diffusion of Au atoms into the Pd shell layers to eliminate the SPDs. At the same time, a long-range ordered L11 AuPd alloy phase has been identified in the interface area, supporting the assumption of the diffusion of Au into Pd to release the interface mismatch. With increasing numbers of Pd shell layers, the shape of the Au-Pd NP changes, step by step, from truncated-octahedral to cubic. After the bimetallic NPs were annealed at 523 K for 10 min, the SPDs at the surface of the NPs coated with a single atomic layer of Pd disappeared due to diffusion of the Au atoms into the surface layer, while the stacking faults and the L11 Au-Pd alloyed structure remained. When the annealing temperature was increased to 800 K, electron diffraction patterns and diffraction contrast images revealed that the NPs became a uniform Au-Pd alloy, and most of the stacking faults disappeared as a result of the annealing. Even so, some clues still support the existence of the L11 phase, which suggests that the L11 phase is a stable, long-range ordered structure in Au-Pd bimetallic NPs. © 2010 American Chemical Society.

  7. CO oxidation on PdO surfaces

    DEFF Research Database (Denmark)

    Hirvi, Janne T.; Kinnunen, Toni-Jani J.; Suvanto, Mika

    2010-01-01

    Density functional calculations were performed in order to investigate CO oxidation on two of the most stable bulk PdO surfaces. The most stable PdO(100) surface, with oxygen excess, is inert against CO adsorption, whereas strong adsorption on the stoichiometric PdO(101) surface leads to favorable...... oxidation via the Langmuir–Hinshelwood mechanism. The reaction with a surface oxygen atom has an activation energy of 0.66 eV, which is comparable to the lowest activation energies observed on metallic surfaces. However, the reaction rate may be limited by the coverage of molecular oxygen. Actually...... adsorption, following the Eley–Rideal mechanism and taking advantage of the reaction tunnel provided by the adjacent palladium atom, has an activation energy of only 0.24 eV. The reaction mechanism and activation energy for the palladium activated CO oxidation on the most stable PdO(100)–O surface...

  8. Atomic scale structure of the 5-fold surface of an AlPdMn quasicrystal: A quantitative X-Ray photoelectron diffraction analysis

    Energy Technology Data Exchange (ETDEWEB)

    Zheng, Jin-Cheng; Huan, C.H.A.; Wee, A.T.S.; Van Hove, M.A.; Fadley, C.S.; Shi, F.J.; Rotenberg, E.; Barman, S.R.; Paggel, J.J.; Horn, K.; Ebert, Ph.; Urban, K.

    2004-02-11

    The atomic scale structure of the 5-fold symmetric surface of an AlPdMn quasicrystal is investigated quantitatively by comparing x-ray photoelectron diffraction (XPD) simulations to experiment. The observed 5-fold symmetry of the diffraction patterns indicates that the surface is quasicrystalline with no hint of a reconstruction from the bulk structure. In analyzing the experimental data, many possible bulk terminations have been tested. Those few that fit best to the data have in common that they contain an Al-rich surface layer followed by a dense mixed Al/Pd/Mn layer. These best terminations, while not identical to each other, are suggested to form terraces coexisting on a real surface. Structural relaxations of the quasicrystal surface are also analyzed: mixing several best-fit terminations gives average best-fit interlayer spacing changes of Dd12 = -0.057 Angstrom, Dd24 = +0.159 Angstrom. These results are in good agreement with a prior structure determination by LEED on a sample that was prepared in a different manner.

  9. Controlling Hydrogen Activation, Spillover, and Desorption with Pd-Au Single-Atom Alloys.

    Science.gov (United States)

    Lucci, Felicia R; Darby, Matthew T; Mattera, Michael F G; Ivimey, Christopher J; Therrien, Andrew J; Michaelides, Angelos; Stamatakis, Michail; Sykes, E Charles H

    2016-02-04

    Key descriptors in hydrogenation catalysis are the nature of the active sites for H2 activation and the adsorption strength of H atoms to the surface. Using atomically resolved model systems of dilute Pd-Au surface alloys and density functional theory calculations, we determine key aspects of H2 activation, diffusion, and desorption. Pd monomers in a Au(111) surface catalyze the dissociative adsorption of H2 at temperatures as low as 85 K, a process previously expected to require contiguous Pd sites. H atoms preside at the Pd sites and desorb at temperatures significantly lower than those from pure Pd (175 versus 310 K). This facile H2 activation and weak adsorption of H atom intermediates are key requirements for active and selective hydrogenations. We also demonstrate weak adsorption of CO, a common catalyst poison, which is sufficient to force H atoms to spill over from Pd to Au sites, as evidenced by low-temperature H2 desorption.

  10. Surface studies on graphite furnace platforms covered with Pd, Rh and Ir as modifiers in graphite furnace atomic absorption spectrometry of tellurium

    Energy Technology Data Exchange (ETDEWEB)

    Pedro, Juana [Area de Química Analítica, Departamento de Química, Facultad de Ingeniería Química, Universidad Nacional del Litoral, Santiago del Estero 2829 (S3000GL.N), Santa Fe (Argentina); Stripekis, Jorge [Laboratorio de Análisis de Trazas, Departamento de Química Inorgánica, Analítica y Química Física, INQUIMAE, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, Ciudad Universitaria (1428), Buenos Aires (Argentina); Departamento de Ingeniería Química, Instituto Tecnológico de Buenos Aires, Av. Eduardo Madero 399 (1106), Buenos Aires (Argentina); Bonivardi, Adrian [Area de Química Analítica, Departamento de Química, Facultad de Ingeniería Química, Universidad Nacional del Litoral, Santiago del Estero 2829 (S3000GL.N), Santa Fe (Argentina); Tudino, Mabel, E-mail: tudino@qi.fcen.uba.ar [Laboratorio de Análisis de Trazas, Departamento de Química Inorgánica, Analítica y Química Física, INQUIMAE, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, Ciudad Universitaria (1428), Buenos Aires (Argentina)

    2015-05-01

    The main objective of this work is the study of correlations between the efficiency of the distribution of the permanent platinum group modifiers Pd, Rh and Ir over the graphite surface with the aim of improving analytical signal of tellurium. Modifier solution was deposited onto the platform and pyrolysed after drying. In the case of Pd, the physical vaporization/deposition technique was also tested. In order to analyze the differences amongst coverings (morphology, topology and distribution), the graphite surfaces were studied with scanning electron microscopy and energy dispersive X-ray microscopy. Micrographs for physical vaporization and pyrolytic deposition of Pd were also analyzed in order to explain the lack of signal obtained for tellurium with the first alternative. Similar micrographs were obtained for pyrolytic deposition of Ir and Rh and then, compared to those of Pd. Ir showed the most homogeneous distribution on the graphite surface and the tallest and sharpest transient. With the aim of improving the analytical signal of tellurium, the correlation between the surface studies and the tellurium transient signal (height, area and shape) is discussed. - Highlights: • Distribution of Rh, Pd and Ir onto graphite furnaces is evaluated by SEM and EDX • Micrographs and spectra showed that surface distribution could influence Te signal. • Ir showed the best signal together with the most homogeneous surface distribution. • Pd-PVD micrographs revealed the absence of graphite and no signal for Te.

  11. The Electrochemical Atomic Layer Deposition of Pt and Pd nanoparticles on Ni foam for the electrooxidation of alcohols

    CSIR Research Space (South Africa)

    Modibedi, RM

    2012-10-01

    Full Text Available Electrodeposition of Pt and Pd metal by surface limited redox replacement reactions was performed using the electrochemical atomic layer deposition. Carbon paper and Ni foam were used as substrates for metal deposition. Supported Pt and Pd...

  12. Alloying Au surface with Pd reduces the intrinsic activity in catalyzing CO oxidation

    KAUST Repository

    Qian, Kun

    2016-03-30

    © 2016. Various Au-Pd/SiO2 catalysts with a fixed Au loading but different Au:Pd molar ratios were prepared via deposition-precipitation method followed by H2 reduction. The structures were characterized and the catalytic activities in CO oxidation were evaluated. The formation of Au-Pd alloy particles was identified. The Au-Pd alloy particles exhibit enhanced dispersions on SiO2 than Au particles. Charge transfer from Pd to Au within Au-Pd alloy particles. Isolated Pd atoms dominate the surface of Au-Pd alloy particles with large Au:Pd molar ratios while contiguous Pd atoms dominate the surface of Au-Pd alloy particles with small Au:Pd molar ratios. Few synergetic effect of Au-Pd alloy occurs on catalyzing CO oxidation under employed reaction conditions. Alloying Au with Pd reduces the intrinsic activity in catalyzing CO oxidation, and contiguous Pd atoms on the Au-Pd alloy particles are capable of catalyzing CO oxidation while isolated Pd atoms are not. These results advance the fundamental understandings of Au-Pd alloy surfaces in catalyzing CO oxidation.

  13. Atom-surface potentials and atom interferometry

    International Nuclear Information System (INIS)

    Babb, J.F.

    1998-01-01

    Long-range atom-surface potentials characterize the physics of many actual systems and are now measurable spectroscopically in deflection of atomic beams in cavities or in reflection of atoms in atomic fountains. For a ground state, spherically symmetric atom the potential varies as -1/R 3 near the wall, where R is the atom-surface distance. For asymptotically large distances the potential is weaker and goes as -1/R 4 due to retardation arising from the finite speed of light. This diminished interaction can also be interpreted as a Casimir effect. The possibility of measuring atom-surface potentials using atomic interferometry is explored. The particular cases studied are the interactions of a ground-state alkali-metal atom and a dielectric or a conducting wall. Accurate descriptions of atom-surface potentials in theories of evanescent-wave atomic mirrors and evanescent wave-guided atoms are also discussed. (author)

  14. Towards ALD thin film stabilized single-atom Pd1 catalysts.

    Science.gov (United States)

    Piernavieja-Hermida, Mar; Lu, Zheng; White, Anderson; Low, Ke-Bin; Wu, Tianpin; Elam, Jeffrey W; Wu, Zili; Lei, Yu

    2016-08-18

    Supported precious metal single-atom catalysts have shown interesting activity and selectivity in recent studies. However, agglomeration of these highly mobile mononuclear surface species can eliminate their unique catalytic properties. Here we study a strategy for synthesizing thin film stabilized single-atom Pd1 catalysts using atomic layer deposition (ALD). The thermal stability of the Pd1 catalysts is significantly enhanced by creating a nanocavity thin film structure. In situ infrared spectroscopy and Pd K-edge X-ray absorption spectroscopy (XAS) revealed that the Pd1 was anchored on the surface through chlorine sites. The thin film stabilized Pd1 catalysts were thermally stable under both oxidation and reduction conditions. The catalytic performance in the methanol decomposition reaction is found to depend on the thickness of protecting layers. While Pd1 catalysts showed promising activity at low temperature in a methanol decomposition reaction, 14 cycle TiO2 protected Pd1 was less active at high temperature. Pd L3 edge XAS indicated that the low reactivity compared with Pd nanoparticles is due to the strong adsorption of carbon monoxide even at 250 °C. These results clearly show that the ALD nanocavities provide a basis for future design of single-atom catalysts that are highly efficient and stable.

  15. Strong paramagnon scattering in single atom Pd contacts

    DEFF Research Database (Denmark)

    Schendel, V.; Barreteau, Cyrille; Brandbyge, Mads

    2017-01-01

    Among all transition metals, palladium (Pd) has the highest density of states at the Fermi energy at low temperatures yet does not fulfill the Stoner criterion for ferromagnetism. However, close proximity to magnetism renders it a nearly ferromagnetic metal, which hosts paramagnons, strongly damp...... adatoms locally induce magnetic order, and transport through single cobalt atoms remains unaffected by paramagnon scattering, consistent with theory....... spin fluctuations. Here we compare the total and the differential conductance of monoatomic contacts consisting of single Pd and cobalt (Co) atoms between Pd electrodes. Transport measurements reveal a conductance for Co of 1G(0), while for Pd we obtain 2G(0). The differential conductance of monoatomic...

  16. Improving gold catalysis of nitroarene reduction with surface Pd

    Energy Technology Data Exchange (ETDEWEB)

    Pretzer, Lori A.; Heck, Kimberly N.; Kim, Sean S.; Fang, Yu-Lun; Zhao, Zhun; Guo, Neng; Wu, Tianpin; Miller, Jeffrey T.; Wong, Michael S.

    2016-04-01

    Nitroarene reduction reactions are commercialized catalytic processes that play a key role in the synthesisof many products including medicines, rubbers, dyes, and herbicides. Whereas bimetallic compositionshave been studied, a better understanding of the bimetallic structure effects may lead to improved indus-trial catalysts. In this work, the influence of surface palladium atoms supported on 3-nm Au nanoparticles(Pd-on-Au NPs) on catalytic activity for 4-nitrophenol reduction is explored. Batch reactor studies indi-cate Pd-on-Au NPs exhibit maximum catalytic activity at a Pd surface coverage of 150 sc%, with aninitial turnover frequency of ~3.7 mol-nitrophenol/mol-metalsurface/s, which was ~5.5× and ~13× moreactive than pure Au NPs and Pd NPs, respectively. Pd NPs, Au NPs, and Pd-on-Au NPs below 175 sc%show compensation behavior. Three-dimensional Pd surface ensembles (with ~4–5 atoms) previouslyidentified through X-ray adsorption spectroscopy provide the active sites responsible for the catalyticmaximum. These results demonstrate the ability to adjust systematically a structural feature (i.e., Pdsurface coverage) to yield a more active material.

  17. Preferential segregation of Pd atoms in the Ag-Pd bimetallic cluster: Density functional theory and molecular dynamics simulation

    Science.gov (United States)

    Kim, Hyun You; Kim, Hyoung Gyu; Ryu, Ji Hoon; Lee, Hyuck Mo

    2007-06-01

    Classical molecular dynamics simulations of the coalescence between an Ag cluster composed of 135 atoms and a Pd cluster of 16 atoms were performed at 500K . All Pd atoms penetrated into the Ag cluster and preferentially segregated at the subsurface layer. The density functional theory calculations revealed that the center site is the most stable position for Pd atoms. However, the energy barrier for further penetration of Pd atoms located at the subsurface was too high to overcome, and thus a metastable structure with Pd atoms segregated at the subsurface did not evolve.

  18. The synthesis of PdPt/carbon paper via surface limited redox replacement reactions for oxygen reduction reaction

    CSIR Research Space (South Africa)

    Motsoeneng, RG

    2015-09-01

    Full Text Available Surface-limited redox replacement reactions using the electrochemical atomic layer deposition (EC-ALD) technique were used to synthesize PdPt bimetallic electrocatalysts on carbon paper substrate. Electrocatalysts having different Pd:Pt ratio were...

  19. Controlled Synthesis of Pd/Pt Core Shell Nanoparticles Using Area-selective Atomic Layer Deposition

    OpenAIRE

    Cao, Kun; Zhu, Qianqian; Shan, Bin; Chen, Rong

    2015-01-01

    We report an atomic scale controllable synthesis of Pd/Pt core shell nanoparticles (NPs) via area-selective atomic layer deposition (ALD) on a modified surface. The method involves utilizing octadecyltrichlorosilane (ODTS) self-assembled monolayers (SAMs) to modify the surface. Take the usage of pinholes on SAMs as active sites for the initial core nucleation, and subsequent selective deposition of the second metal as the shell layer. Since new nucleation sites can be effectively blocked by s...

  20. Interaction of Pd single atoms with different CeO2 crystal planes: A first-principles study

    Science.gov (United States)

    He, Bingling; Wang, Jinlong; Ma, Dongwei; Tian, Zhixue; Jiang, Lijuan; Xu, Yan; Cheng, Sujun

    2018-03-01

    The adsorption of single Pd atoms on the various CeO2 surfaces, including (111), (110), and (100), has been studied based on the first-principles calculations. It is found that, according to the calculated adsorption energy, interaction strength between Pd and the three CeO2 surfaces follows the order of (100) > (110) > (111). Interestingly, the effect of the electron localization on the surface Ce ions due to the Pd adsorption on its adsorption stability is more significant for the (110) surface than that for the (111) and (100) surfaces. We also find that the formal oxidation states of Pd0, Pdδ+ (δ < 1) and Pd1+ may appear on the CeO2 (111) surface, and Pdδ+ (δ < 1) and Pd1+ could coexist on the CeO2 (100) surfaces. However, under suitable conditions the CeO2 (110) surface may be covered with Pd2+ ions. Present theoretical results clearly suggest that the interaction between Pd and CeO2 nanocrystals significantly depends on the crystal planes of CeO2. It is expected that our study will give useful insights into the effect of CeO2 crystal plane on the physicochemical and catalytic properties of CeO2 supported Pd catalyst.

  1. Atomically dispersed Pd catalysts in graphyne nanopore: formation and reactivity

    Science.gov (United States)

    Gu, Yongbing; Chen, Xianlang; Cao, Yongyong; Zhuang, Guilin; Zhong, Xing; Wang, Jianguo

    2017-07-01

    The formation of single-atom noble metal catalysts on carbon materials remains a challenge due to the weak interaction between metals and pristine carbon. By means of density functional theory (DFT) calculations, it is found that the atomically dispersed Pd in graphyne nanopore is much more stable than that of relative Pd clusters. The large diffusion barrier of Pd from the most stable hollow site to the bridge site confirms the kinetic stability of such structures. While CO adsorption causes the pulling of Pd from graphyne nanopore due to the low diffusion barrier, based on DFT calculations, which can be further confirmed by ab initio molecular dynamic simulations. Finally, CO oxidation on the reconstruction of Pd@graphyne exhibits an energy barrier of 0.62 eV in the rate-limiting step through the Langmuir-Hinshelwood mechanism. After the reaction, the catalyst can be restored to the original atomically dispersed state again. This study shows graphyne is an excellent support for an atomically dispersed or single-metal catalyst.

  2. Atomic displacements due to interstitial hydrogen in Cu and Pd

    Indian Academy of Sciences (India)

    c Indian Academy of Sciences. Vol. 69, No. 2. — journal of. August 2007 physics pp. 255–265. Atomic displacements due to interstitial hydrogen in Cu and Pd ..... Phys. 64, 1015 (1992). [7] Martin Fuchs and Matthias Scheffer, Comput. Phys. Commun. 119, 67 (1999). [8] Hitesh Sharma and S Prakash, Pramana – J. Phys.

  3. Catalytic activity of Pd-doped Cu nanoparticles for hydrogenation as a single-atom-alloy catalyst.

    Science.gov (United States)

    Cao, Xinrui; Fu, Qiang; Luo, Yi

    2014-05-14

    The single atom alloy of extended surfaces is known to provide remarkably enhanced catalytic performance toward heterogeneous hydrogenation. Here we demonstrate from first principles calculations that this approach can be extended to nanostructures, such as bimetallic nanoparticles. The catalytic properties of the single-Pd-doped Cu55 nanoparticles have been systemically examined for H2 dissociation as well as H atom adsorption and diffusion, following the concept of single atom alloy. It is found that doping a single Pd atom at the edge site of the Cu55 shell can considerably reduce the activation energy of H2 dissociation, while the single Pd atom doped at the top site or in the inner layers is much less effective. The H atom adsorption on Cu55 is slightly stronger than that on the Cu(111) surface; however, a larger nanoparticle that contains 147 atoms could effectively recover the weak binding of the H atoms. We have also investigated the H atom diffusion on the 55-atom nanoparticle and found that spillover of the produced H atoms could be a feasible process due to the low diffusion barriers. Our results have demonstrated that facile H2 dissociation and weak H atom adsorption could be combined at the nanoscale. Moreover, the effects of doping one more Pd atom on the H2 dissociation and H atom adsorption have also been investigated. We have found that both the doping Pd atoms in the most stable configuration could independently exhibit their catalytic activity, behaving as two single-atom-alloy catalysts.

  4. First principles analysis of hydrogen chemisorption on Pd-Re alloyed overlayers and alloyed surfaces

    DEFF Research Database (Denmark)

    Pallassana, Venkataraman; Neurock, Matthew; Hansen, Lars Bruno

    2000-01-01

    Gradient corrected periodic density functional theory (DFT-GGA) slab calculations were used to examine the chemisorption of atomic hydrogen on various Pd-Re alloyed overlayers and uniformly alloyed surfaces. Adsorption was examined at 33% surface coverage, where atomic hydrogen preferred the thre...

  5. Electronic and atomic disorder in icosahedral AlPdRe

    International Nuclear Information System (INIS)

    Rapp, Oe; Karkin, A A; Goshchitskii, B N; Voronin, V I; Srinivas, V; Poon, S J

    2008-01-01

    Relations between electronic and atomic disorder of i-AlPdRe have been investigated by studies of neutron irradiated and annealed samples. The advantage with this technique is that a single sample can be monitored over a significant range of varying electronic properties, without concern for any influence of varying impurities. X-ray diffraction, the electrical resistivity and its temperature dependence, and the magnetoresistance are studied. The results show that annealings of an irradiated sample lead to improvement of the atomic order, as reflected in increased intensities of the x-ray diffraction peaks, while electronic properties change in the direction of increasing electronic disorder towards a metal-insulator transition. The observed relation in quasicrystals that improved atomic structure is associated with stronger anomalies in transport properties is thus also seen in i-AlPdRe. In particular, the variation of the diffusion constant in the region of small values of the resistivity is found to be similar for annealed polygrain samples and for single grain samples with varying Pd concentration, as evaluated from literature data, indicating a similar development of electronic disorder in both sets of samples. However, the problem remains as to why the resistivity is small in single grain samples which are atomically well-ordered. The possibility of a strong sensitivity to concentration differences is pointed out

  6. Suppressing Isomerization of Phosphine-Protected Au9Cluster by Bond Stiffening Induced by a Single Pd Atom Substitution.

    Science.gov (United States)

    Yamazoe, Seiji; Matsuo, Shota; Muramatsu, Satoru; Takano, Shinjiro; Nitta, Kiyofumi; Tsukuda, Tatsuya

    2017-07-17

    The fluxional nature of small gold clusters has been exemplified by reversible isomerization between [Au 9 (PPh 3 ) 8 ] 3+ with a crown motif (Au 9 (C)) and that with a butterfly motif (Au 9 (B)) induced by association and dissociation with compact counteranions (NO 3 - , Cl - ). However, structural isomerization was suppressed by substitution of the central Au atom of the Au 9 core in [Au 9 (PPh 3 ) 8 ] 3+ with a Pd atom: [PdAu 8 (PPh 3 ) 8 ] 2+ with a crown motif (PdAu 8 (C)) did not isomerize to that with a butterfly motif (PdAu 8 (B)) upon association with the counteranions. Density functional theory calculation showed that the energy difference between PdAu 8 (C) and PdAu 8 (B) is comparable to that between Au 9 (C) and Au 9 (B), indicating that the relative stabilities of the isomers are not a direct cause for the suppression of isomerization. Temperature dependence of Debye-Waller factors obtained by X-ray absorption fine-structure analysis revealed that the intracluster bonds of PdAu 8 (C) were stiffer than the corresponding bonds in Au 9 (C). Natural bond orbital analysis suggested that the radial Pd-Au and lateral Au-Au bonds in PdAu 8 (C) are stiffened due to the increase in the ionic nature and decrease in electrostatic repulsion between the surface Au atoms, respectively. We conclude that the formation of stiffer metal-metal bonds by Pd atom doping inhibits the isomerization from PdAu 8 (C) to PdAu 8 (B).

  7. Cold atoms close to surfaces

    DEFF Research Database (Denmark)

    Krüger, Peter; Wildermuth, Stephan; Hofferberth, Sebastian

    2005-01-01

    Microscopic atom optical devices integrated on atom chips allow to precisely control and manipulate ultra-cold (T atoms and Bose-Einstein condensates (BECs) close to surfaces. The relevant energy scale of a BEC is extremely small (down to ... be utilized as a sensor for variations of the potential energy of the atoms close to the surface. Here we describe how to use trapped atoms as a measurement device and analyze the performance and flexibility of the field sensor. We demonstrate microscopic magnetic imaging with simultaneous high spatial...... variations of the current flow direction, resulting from local properties of the wire. These disorder potentials found near lithographically fabricated wires are two orders of magnitude smaller than those measured close to electroplated conductors....

  8. Helium atom scattering from surfaces

    CERN Document Server

    1992-01-01

    High resolution helium atom scattering can be applied to study a number of interesting properties of solid surfaces with great sensitivity and accuracy. This book treats in detail experimental and theoretical aspects ofthis method as well as all current applications in surface science. The individual chapters - all written by experts in the field - are devoted to the investigation of surface structure, defect shapes and concentrations, the interaction potential, collective and localized surface vibrations at low energies, phase transitions and surface diffusion. Over the past decade helium atom scattering has gained widespread recognitionwithin the surface science community. Points in its favour are comprehensiveunderstanding of the scattering theory and the availability of well-tested approximation to the rigorous theory. This book will be invaluable to surface scientists wishing to make an informed judgement on the actual and potential capabilities of this technique and its results.

  9. Friction of atomically stepped surfaces

    NARCIS (Netherlands)

    Dikken, R.J.; Thijsse, B.J.; Nicola, L.

    2017-01-01

    The friction behavior of atomically stepped metal surfaces under contact loading is studied using molecular dynamics simulations. While real rough metal surfaces involve roughness at multiple length scales, the focus of this paper is on understanding friction of the smallest scale of roughness:

  10. Polarization dependent Pd deposition structure on LiNbO3 {0001} surface

    Science.gov (United States)

    Kim, Seungchul; Rappe, Andrew M.

    2011-03-01

    We investigate effects of polarization orientation on atomic structure of palladium deposited on lithium niobate (LiNb O3) {0001} surface, using density functional theory (DFT) and kinetic Monte Carlo (kMC) simulations. Adsorption, diffusion, aggregation and clustering process -- include geometries, paths and energies -- of Pd clusters were calculated from DFT simulations. It has been observed that energy barriers of Pd motions on the negatively poled (c-) surface are much larger than those on the positively poled surface (c+), which indicates the Pd motions on the c- surface are much slower than that of c+ surface. We demonstrate, using kMC with kinetic parameters from DFT, very slow motion of Pd on c- surface leads dispersed small clusters or atoms while fast motion on c+ surface leads large clusters, indicating larger Pd-covered area on c- surface than c+ after Pd deposition. This work has been supported by US-DOE (grant DE-FG02-07ER15920), and by AROSR (FA9550-07-1-0397). Computational support was provided by HPCMO of the US-DoD.

  11. Theoretical studies of the work functions of Pd-based bimetallic surfaces

    Science.gov (United States)

    Ding, Zhao-Bin; Wu, Feng; Wang, Yue-Chao; Jiang, Hong

    2015-06-01

    Work functions of Pd-based bimetallic surfaces, including mainly M/Pd(111), Pd/M, and Pd/M/Pd(111) (M = 4d transition metals, Cu, Au, and Pt), are studied using density functional theory. We find that the work function of these bimetallic surfaces is significantly different from that of parent metals. Careful analysis based on Bader charges and electron density difference indicates that the variation of the work function in bimetallic surfaces can be mainly attributed to two factors: (1) charge transfer between the two different metals as a result of their different intrinsic electronegativity, and (2) the charge redistribution induced by chemical bonding between the top two layers. The first factor can be related to the contact potential, i.e., the work function difference between two metals in direct contact, and the second factor can be well characterized by the change in the charge spilling out into vacuum. We also find that the variation in the work functions of Pd/M/Pd(111) surfaces correlates very well with the variation of the d-band center of the surface Pd atom. The findings in this work can be used to provide general guidelines to design new bimetallic surfaces with desired electronic properties.

  12. Atomic structure of a decagonal Al-Pd-Mn phase

    Science.gov (United States)

    Mihalkovič, Marek; Roth, Johannes; Trebin, Hans-Rainer

    2017-12-01

    We present a detailed structure solution for the 16 -Å decagonal quasicrystal in the Al-Pd-Mn system by means of cluster decoration and ab initio energy minimization. It is based on structure models of the ɛ and other approximant phases. The ɛ phases can be represented as subsets of a hexagon-boat-star (HBS) tiling. The decagonal phase comprises further HBS tiles. We have constructed several fictitious HBS approximants and optimized their structures individually. All tiles are decorated by two types of atomic clusters: the pseudo-Mackay icosahedron (PMI) and the large bicapped pentagonal prism (LBPP). It turns out that, whereas the PMI clusters can be kept essentially unchanged, the LBPP clusters must be adjusted in occupancy with Al atoms depending on their positions in the various tiles. In this way we obtain cluster decorations for all tiles of the decagonal quasicrystal. The calculations were confirmed by evaluation of an effective tile Hamiltonian.

  13. Atomic Manipulation on Metal Surfaces

    Science.gov (United States)

    Ternes, Markus; Lutz, Christopher P.; Heinrich, Andreas J.

    Half a century ago, Nobel Laureate Richard Feynman asked in a now-famous lecture what would happen if we could precisely position individual atoms at will [R.P. Feynman, Eng. Sci. 23, 22 (1960)]. This dream became a reality some 30 years later when Eigler and Schweizer were the first to position individual Xe atoms at will with the probe tip of a low-temperature scanning tunneling microscope (STM) on a Ni surface [D.M. Eigler, E.K. Schweizer, Nature 344, 524 (1990)].

  14. Controlled Synthesis of Pd/Pt Core Shell Nanoparticles Using Area-selective Atomic Layer Deposition.

    Science.gov (United States)

    Cao, Kun; Zhu, Qianqian; Shan, Bin; Chen, Rong

    2015-02-16

    We report an atomic scale controllable synthesis of Pd/Pt core shell nanoparticles (NPs) via area-selective atomic layer deposition (ALD) on a modified surface. The method involves utilizing octadecyltrichlorosilane (ODTS) self-assembled monolayers (SAMs) to modify the surface. Take the usage of pinholes on SAMs as active sites for the initial core nucleation, and subsequent selective deposition of the second metal as the shell layer. Since new nucleation sites can be effectively blocked by surface ODTS SAMs in the second deposition stage, we demonstrate the successful growth of Pd/Pt and Pt/Pd NPs with uniform core shell structures and narrow size distribution. The size, shell thickness and composition of the NPs can be controlled precisely by varying the ALD cycles. Such core shell structures can be realized by using regular ALD recipes without special adjustment. This SAMs assisted area-selective ALD method of core shell structure fabrication greatly expands the applicability of ALD in fabricating novel structures and can be readily applied to the growth of NPs with other compositions.

  15. Experimental study on the surface characteristics of Pd-based bulk metallic glass

    International Nuclear Information System (INIS)

    Zhang, Xiang; Sun, Bingli; Zhao, Na; Li, Qian; Hou, Jianhua; Feng, Weina

    2014-01-01

    Highlights: • Wetting behavior of four polymer melts on Pd-based bulk metallic glass was investigated. • From results, in general, the contact angle of polymer on Pd-based BMG decreases with temperature increasing. • We find a critical temperature for each polymer, above this temperature, contact angle on Pd-based BMG does not decrease with temperature increasing. • Surface free energy of Pd-based BMG was estimated by Owens–Wendt method. - Abstract: The metallic glass has many unique and desirable physical and chemical characteristics for their long-range disordered atomic structure, among them the interfacial properties of the metallic glasses are crucial for their applications and manufacturing. In this work, the contact wetting angles between the polymer melts and Pd 40 Cu 30 Ni 10 P 20 bulk metallic glass (Pd-BMG) with four kinds of roughness were analyzed. Experiments show the order of four polymers wettability on Pd-BMG was PP > HDPE > COC > PC. The surface free energy of Pd-BMG was estimated by Owens–Wendt method using the contact angles of three testing liquids. Neumann method was also used to further evidence the surface free energy of Pd-BMG comparing with PTFE, mold steels NAK80 and LKM2343ESR. The results provide theoretical and technical supports for the fabrication of metallic glass micro mold and the parameter optimization of polymer micro injection molding

  16. Stability issues in Pd-based catalysts: the role of surface Pt in improving the stability and oxygen reduction reaction (ORR) activity.

    Science.gov (United States)

    Singh, R K; Rahul, R; Neergat, M

    2013-08-21

    Carbon-supported Pd and Pd3Co catalysts have been electrochemically characterized in 0.1 M HClO4 solution and we found that both catalysts were unstable. On repeated potential cycling, the electrochemical surface area of the catalysts decreases and the oxygen reduction reaction (ORR) activity suffers. To stabilize surface Pd atoms of both Pd and Pd3Co catalysts, we deposited Pt using adsorbed hydrogen on the catalytically active Pd sites. The Pt : Pd ratio of Pt-coated Pd and Pt-coated Pd3Co catalysts suggests half-a-monolayer coverage of Pt (two hydrogen atoms required for reducing a Pt(2+) ion). The Pt : Pd ratio of Pt-coated Pd3Co catalyst obtained from the simple geometrical hard sphere model, energy-dispersive X-ray spectroscopy (EDS) line scan and bulk EDS agrees very well with that calculated from the hydrogen desorption (H(des)) charge of Pd3Co. At the same time, the Pt : Pd ratio of Pt-coated Pd calculated from the H(des) charge of Pd catalyst is significantly lower than the ratio obtained from the other methods. Thus, the Pt : Pd ratio of the Pt-coated Pd catalyst estimated from the H(des) region of Pd is an underestimation of the composition. This suggests that Pd forms an electrochemically inactive species from the H(upd) region itself and Co in Pd3Co seems to stabilize Pd against oxidation by delaying the formation of electrochemically inactive species to higher potentials above the H(upd) region. The voltammograms along with the peroxide formation characteristics of the catalysts support the above observations. The deposited Pt on the surface of the Pd and Pd3Co catalysts masks active Pd sites from the electrochemical environment and even partial coverage with Pt improves the stability and ORR activity of the catalysts when compared to that of the respective Pt-free counterparts.

  17. 3D-nanoarchitectured Pd/Ni catalysts prepared by atomic layer deposition for the electrooxidation of formic acid

    Directory of Open Access Journals (Sweden)

    Loïc Assaud

    2014-02-01

    Full Text Available Three-dimensionally (3D nanoarchitectured palladium/nickel (Pd/Ni catalysts, which were prepared by atomic layer deposition (ALD on high-aspect-ratio nanoporous alumina templates are investigated with regard to the electrooxidation of formic acid in an acidic medium (0.5 M H2SO4. Both deposition processes, Ni and Pd, with various mass content ratios have been continuously monitored by using a quartz crystal microbalance. The morphology of the Pd/Ni systems has been studied by electron microscopy and shows a homogeneous deposition of granularly structured Pd onto the Ni substrate. X-ray diffraction analysis performed on Ni and NiO substrates revealed an amorphous structure, while the Pd coating crystallized into a fcc lattice with a preferential orientation along the [220]-direction. Surface chemistry analysis by X-ray photoelectron spectroscopy showed both metallic and oxide contributions for the Ni and Pd deposits. Cyclic voltammetry of the Pd/Ni nanocatalysts revealed that the electrooxidation of HCOOH proceeds through the direct dehydrogenation mechanism with the formation of active intermediates. High catalytic activities are measured for low masses of Pd coatings that were generated by a low number of ALD cycles, probably because of the cluster size effect, electronic interactions between Pd and Ni, or diffusion effects.

  18. IrPd nanoalloys: simulations, from surface segregation to local electronic properties

    Energy Technology Data Exchange (ETDEWEB)

    Andriamiharintsoa, T. H. [Institut de Physique et Chimie des Matériaux de Strasbourg CNRS-UDS UMR 7504 (France); Rakotomahevitra, A. [Institut pour la Maîtrise de l’Énergie, Faculté des sciences d’Antananarivo (Madagascar); Piccolo, L. [Institut de Recherches sur la Catalyse et l’Environnement de Lyon IRCELYON, UMR 5256 CNRS and Université Lyon 1 (France); Goyhenex, C., E-mail: christine.goyhenex@ipcms.unistra.fr [Institut de Physique et Chimie des Matériaux de Strasbourg CNRS-UDS UMR 7504 (France)

    2015-05-15

    Using semi-empirical modeling, namely tight-binding at different levels of accuracy, the chemical, crystallographic, and electronic structures of bimetallic IrPd nanoparticles are characterized. For the purpose, model cuboctahedral particles containing 561 atoms are considered. Atomistic simulations show that core–shell nanoparticles are highly stable, with a strong surface segregation of Pd, at least for one atomic shell thickness. Within self-consistent tight-binding calculations founded on the density functional theory, an accurate insight is given into the electronic structure of these materials which have a high potential as catalysts.

  19. PREFACE: Atom-surface scattering Atom-surface scattering

    Science.gov (United States)

    Miret-Artés, Salvador

    2010-08-01

    It has been a privilege and a real pleasure to organize this special issue or festschrift in the general field of atom-surface scattering (and its interaction) in honor of J R Manson. This is a good opportunity and an ideal place to express our deep gratitude to one of the leaders in this field for his fundamental and outstanding scientific contributions. J R Manson, or Dick to his friends and colleagues, is one of the founding fathers, together with N Cabrera and V Celli, of the 'Theory of surface scattering and detection of surface phonons'. This is the title of the very well-known first theoretical paper by Dick published in Physical Review Letters in 1969. My first meeting with Dick was around twenty years ago in Saclay. J Lapujoulade organized a small group seminar about selective adsorption resonances in metal vicinal surfaces. We discussed this important issue in surface physics and many other things as if we had always known each other. This familiarity and warm welcome struck me from the very beginning. During the coming years, I found this to be a very attractive aspect of his personality. During my stays in Göttingen, we had the opportunity to talk widely about science and life at lunch or dinner time, walking or cycling. During these nice meetings, he showed, with humility, an impressive cultural background. It is quite clear that his personal opinions about history, religion, politics, music, etc, come from considering and analyzing them as 'open dynamical systems'. In particular, with good food and better wine in a restaurant or at home, a happy cheerful soirée is guaranteed with him, or even with only a good beer or espresso, and an interesting conversation arises naturally. He likes to listen before speaking. Probably not many people know his interest in tractors. He has an incredible collection of very old tractors at home. In one of my visits to Clemson, he showed me the collection, explaining to me in great detail, their technical properties

  20. Surface composition and structure of nickel ultra-thin films deposited on Pd(111)

    Energy Technology Data Exchange (ETDEWEB)

    Carazzolle, M.F. [Universidade Estadual de Campinas, Instituto de Fisica ' Gleb Wataghin' , Departamento de Fisica Aplicada, 13083-970 Campinas, SP (Brazil); Maluf, S.S. [Universidade Federal de Sao Carlos, Departamento de Engenharia de Materiais, 13565-905 Sao Carlos, SP (Brazil); Siervo, A. de [Laboratorio Nacional de Luz Sincrotron, 13084-971 Campinas, SP (Brazil); Nascente, P.A.P. [Universidade Federal de Sao Carlos, Departamento de Engenharia de Materiais, 13565-905 Sao Carlos, SP (Brazil)], E-mail: nascente@power.ufscar.br; Landers, R. [Universidade Estadual de Campinas, Instituto de Fisica ' Gleb Wataghin' , Departamento de Fisica Aplicada, 13083-970 Campinas, SP (Brazil); Laboratorio Nacional de Luz Sincrotron, 13084-971 Campinas, SP (Brazil); Kleiman, G.G. [Universidade Estadual de Campinas, Instituto de Fisica ' Gleb Wataghin' , Departamento de Fisica Aplicada, 13083-970 Campinas, SP (Brazil)

    2007-05-15

    Ultra-thin nickel films deposited on the Pd(111) surface were characterized by X-ray photoelectron spectroscopy (XPS), low-energy electron diffraction (LEED), and X-ray photoelectron diffraction (XPD). Up to 3 ML coverage, a LEED (1 x 1) pattern with a diffuse background due to a random distribution of Ni atoms on the surface is observed. Annealing at 600 deg. C reduced the background drastically and sharp (1 x 1) spots appeared on the screen, but XPS showed no presence of nickel on the surface, indicating diffusion into the bulk. Annealing at 300 deg. C for 30 min yielded also a sharp (1 x 1) LEED pattern, and the XPS Ni/Pd intensity ratio decreased with annealing time. The comparison between experimental and theoretical XPD results indicated that the surface was covered partially by Ni islands and partially by a random Ni-Pd surface alloy.

  1. Can atom-surface potential measurements test atomic structure models?

    Science.gov (United States)

    Lonij, Vincent P A; Klauss, Catherine E; Holmgren, William F; Cronin, Alexander D

    2011-06-30

    van der Waals (vdW) atom-surface potentials can be excellent benchmarks for atomic structure calculations. This is especially true if measurements are made with two different types of atoms interacting with the same surface sample. Here we show theoretically how ratios of vdW potential strengths (e.g., C₃(K)/C₃(Na)) depend sensitively on the properties of each atom, yet these ratios are relatively insensitive to properties of the surface. We discuss how C₃ ratios depend on atomic core electrons by using a two-oscillator model to represent the contribution from atomic valence electrons and core electrons separately. We explain why certain pairs of atoms are preferable to study for future experimental tests of atomic structure calculations. A well chosen pair of atoms (e.g., K and Na) will have a C₃ ratio that is insensitive to the permittivity of the surface, whereas a poorly chosen pair (e.g., K and He) will have a ratio of C₃ values that depends more strongly on the permittivity of the surface.

  2. Atomic and molecular layer activation of dielectric surfaces

    Science.gov (United States)

    Senkevich, John Joseph

    Strong interaction between the material deposit and substrate is critical to stable deposits and interfaces. The work presented here focuses on the surface activation of dielectric surfaces and oxidized metal surfaces to promote the chemisorption of palladium (II) hexafluoroacetylacetonate (PdII (hfac)2). The goal is to develop reliable, robust metallization protocols, which enable strong interactions between the metal and substrate. SiO2, air exposed Ta, Trikon, and SiLK were activated with sulfur or phosphorus. Two types of activations were developed; one based on self-assembled chemistry, and the other a plasma-assisted process. Activation of the surface using self-assembly techniques was carried out using mercaptan-terminated silane and tetrasulfide silane. The resulting films were characterized by variable angle spectroscopic ellipsometry, contact angle goniometry, and X-ray photoelectron spectroscopy. Tetrasulfide silane sources films exhibit self-limiting behavior, even in the presence of water vapor; whereas mercaptan-terminated silane sourced films tend to be thicker. The surface activations using atomic layers of sulfur and phosphorus were carried out in a rf plasma chamber using hydrogen sulfide and phosphine sources, respectively. The activations were studied as functions of rf power, system pressure, and substrate material. Results show that higher rf powers and lower system pressures promote greater surface coverages by sulfur with a reduced oxidation state. The activated dielectrics show evidence of PdII(hfac)2 chemisorption, in contrast to non-activated surfaces. The binding energy shift of the Pd3d 5/2 XPS peak towards elemental Pd provides evidence for the dissociative chemisorption of PdII(hfac)2. The extent of dissociation depends on the substrate temperature and the activation method used. The conclusions of the work presented here have implications for metallization using highly polarizable transition metals. Specifically, it can be applied to

  3. Atomic layer deposition of Pd and Pt nanoparticles for catalysis: on the mechanisms of nanoparticle formation

    International Nuclear Information System (INIS)

    Mackus, Adriaan J M; Weber, Matthieu J; Thissen, Nick F W; Garcia-Alonso, Diana; Vervuurt, René H J; Assali, Simone; Bol, Ageeth A; Verheijen, Marcel A; Kessels, Wilhelmus M M

    2016-01-01

    The deposition of Pd and Pt nanoparticles by atomic layer deposition (ALD) has been studied extensively in recent years for the synthesis of nanoparticles for catalysis. For these applications, it is essential to synthesize nanoparticles with well-defined sizes and a high density on large-surface-area supports. Although the potential of ALD for synthesizing active nanocatalysts for various chemical reactions has been demonstrated, insight into how to control the nanoparticle properties (i.e. size, composition) by choosing suitable processing conditions is lacking. Furthermore, there is little understanding of the reaction mechanisms during the nucleation stage of metal ALD. In this work, nanoparticles synthesized with four different ALD processes (two for Pd and two for Pt) were extensively studied by transmission electron spectroscopy. Using these datasets as a starting point, the growth characteristics and reaction mechanisms of Pd and Pt ALD relevant for the synthesis of nanoparticles are discussed. The results reveal that ALD allows for the preparation of particles with control of the particle size, although it is also shown that the particle size distribution is strongly dependent on the processing conditions. Moreover, this paper discusses the opportunities and limitations of the use of ALD in the synthesis of nanocatalysts. (paper)

  4. Atomic probes of surface structure and dynamics

    International Nuclear Information System (INIS)

    Heller, E.J.; Jonsson, H.

    1992-01-01

    Progress for the period Sept. 15, 1992 to Sept. 14, 1993 is discussed. Semiclassical methods that will allow much faster and more accurate three-dimensional atom--surface scattering calculations, both elastic and inelastic, are being developed. The scattering of He atoms from buckyballs is being investigated as a test problem. Somewhat more detail is given on studies of He atom scattering from defective Pt surfaces. Molecular dynamics simulations of He + and Ar + ion sputtering of Pt surfaces are also being done. He atom scattering from Xe overlayers on metal surfaces and the thermalized dissociation of H 2 on Cu(110) are being studied. (R.W.R.) 64 refs

  5. A Theoretical Investigation on CO Oxidation by Single-Atom Catalysts M1/γ-Al2O3(M=Pd, Fe, Co, and Ni).

    Science.gov (United States)

    Yang, Tao; Fukuda, Ryoichi; Hosokawa, Saburo; Tanaka, Tsunehiro; Sakaki, Shigeyoshi; Ehara, Masahiro

    2017-04-07

    Single-atom catalysts have attracted much interest recently because of their excellent stability, high catalytic activity, and remarkable atom efficiency. Inspired by the recent experimental discovery of a highly efficient single-atom catalyst Pd 1 /γ-Al 2 O 3 , we conducted a comprehensive DFT study on geometries, stabilities and CO oxidation catalytic activities of M 1 /γ-Al 2 O 3 (M=Pd, Fe, Co, and Ni) by using slab-model. One of the most important results here is that Ni 1 /Al 2 O 3 catalyst exhibits higher activity in CO oxidation than Pd 1 /Al 2 O 3 . The CO oxidation occurs through the Mars van Krevelen mechanism, the rate-determining step of which is the generation of CO 2 from CO through abstraction of surface oxygen. The projected density of states (PDOS) of 2 p orbitals of the surface O, the structure of CO-adsorbed surface, charge polarization of CO and charge transfer from CO to surface are important factors for these catalysts. Although the binding energies of Fe and Co with Al 2 O 3 are very large, those of Pd and Ni are small, indicating that the neighboring O atom is not strongly bound to Pd and Ni, which leads to an enhancement of the reactivity of the O atom toward CO. The metal oxidation state is suggested to be one of the crucial factors for the observed catalytic activity.

  6. Development of an inter-atomic potential for the Pd-H binary system.

    Energy Technology Data Exchange (ETDEWEB)

    Zimmerman, Jonathan A.; Hoyt, Jeffrey John (McMaster University, Hamilton, Ontario, Canada); Leonard, Francois Leonard; Griffin, Joshua D.; Zhou, Xiao Wang

    2007-09-01

    Ongoing research at Sandia National Laboratories has been in the area of developing models and simulation methods that can be used to uncover and illuminate the material defects created during He bubble growth in aging bulk metal tritides. Previous efforts have used molecular dynamics calculations to examine the physical mechanisms by which growing He bubbles in a Pd metal lattice create material defects. However, these efforts focused only on the growth of He bubbles in pure Pd and not on bubble growth in the material of interest, palladium tritide (PdT), or its non-radioactive isotope palladium hydride (PdH). The reason for this is that existing inter-atomic potentials do not adequately describe the thermodynamics of the Pd-H system, which includes a miscibility gap that leads to phase separation of the dilute (alpha) and concentrated (beta) alloys of H in Pd at room temperature. This document will report the results of research to either find or develop inter-atomic potentials for the Pd-H and Pd-T systems, including our efforts to use experimental data and density functional theory calculations to create an inter-atomic potential for this unique metal alloy system.

  7. Effect of preparation method on the surface characteristics and activity of the Pd/OMS-2 catalysts for the oxidation of carbon monoxide, toluene, and ethyl acetate

    Science.gov (United States)

    Liu, Lisha; Song, Yong; Fu, Zhidan; Ye, Qing; Cheng, Shuiyuan; Kang, Tianfang; Dai, Hongxing

    2017-02-01

    The cryptomelane-type manganese oxide octahedral molecular sieve (OMS-2)-supported Pd (0.5 wt% Pd/OMS-2-DP, 0.5 wt% Pd/OMS-2-PI, and 0.5 wt% Pd/OMS-2-EX) catalysts were prepared by the deposition-precipitation, pre-incorporation, and ion-exchanging strategies, respectively. It is shown that the preparation method exerted an important effect on the physicochemical property of the sample. Among the OMS-2-supported Pd catalysts, 0.5 wt% Pd/OMS-2-DP possessed the highest surface (Mn2+ + Mn3+)/Mn4+ atomic ratio and the highest surface Pd loading and acid sites. The 0.5 wt% Pd/OMS-2 catalysts outperformed the Pd-free counterpart, among which 0.5 wt% Pd/OMS-2-DP presented the best catalytic activity (T50% and T90% were 25 and 55 °C for CO oxidation, 240 and 285 °C for toluene oxidation, and 160 and 200 °C for ethyl acetate oxidation, respectively). We believe that the high Pd surface loading, high surface atomic ratio of (Mn2+ + Mn3+)/Mn4+, and good low-temperature reducibility, good oxygen mobility, and high acidity were responsible for the excellent performance of the 0.5 wt% Pd/OMS-2-DP catalyst.

  8. Nanoporous PdZr surface alloy as highly active non-platinum electrocatalyst toward oxygen reduction reaction with unique structure stability and methanol-tolerance

    Science.gov (United States)

    Duan, Huimei; Xu, Caixia

    2016-06-01

    Nanoporous (NP) PdZr alloy with controllable bimetallic ratio is successfully fabricated by a simple dealloying method. By leaching out the more reactive Al from PdZrAl precursor alloy, NP-PdZr alloy with smaller ligament size was generated, characterized by the nanoscaled interconnected network skeleton and hollow channels extending in all three dimensions. Upon voltammetric scan in acid solution, the dissolution of surface Zr atoms generates the highly active Pd-Zr surface alloy with a nearly pure Pd surface and Pd-Zr alloy core. The NP-Pd80Zr20 surface alloy exhibits markedly enhanced specific and mass activities as well as higher catalytic stability toward oxygen reduction reaction (ORR) compared with NP-Pd and the state-of-the-art Pt/C catalysts. In addition, the NP-Pd80Zr20 surface alloy shows a better selectivity for ORR than methanol in the 0.1 M HClO4 and 0.1 M methanol mixed solution. X-ray photoelectron spectroscopy and density functional theory calculations both demonstrate that the weakened Pd-O bond and improved ORR performances in turn depend on the downshifted d-band center of Pd due to the alloying Pd with Zr (20 at.%). The as-made NP-PdZr alloy holds prospective applications as a cathode electrocatalyst in fuel-cell-related technologies with the advantages of superior overall ORR performances, unique structure stability, and easy preparation.

  9. Effect of preparation method on the surface characteristics and activity of the Pd/OMS-2 catalysts for the oxidation of carbon monoxide, toluene, and ethyl acetate

    Energy Technology Data Exchange (ETDEWEB)

    Liu, Lisha; Song, Yong; Fu, Zhidan [Key Laboratory of Beijing on Regional Air Pollution Control, Department of Environmental Science, College of Environmental and Energy Engineering, Beijing University of Technology, Beijing 100124 (China); Ye, Qing, E-mail: yeqing@bjut.edu.cn [Key Laboratory of Beijing on Regional Air Pollution Control, Department of Environmental Science, College of Environmental and Energy Engineering, Beijing University of Technology, Beijing 100124 (China); Cheng, Shuiyuan; Kang, Tianfang [Key Laboratory of Beijing on Regional Air Pollution Control, Department of Environmental Science, College of Environmental and Energy Engineering, Beijing University of Technology, Beijing 100124 (China); Dai, Hongxing, E-mail: hxdai@bjut.edu.cn [Beijing Key Laboratory for Green Catalysis and Separation, Key Laboratory of Beijing on Regional Air Pollution Control, Department of Chemistry and Chemical Engineering, College of Environmental and Energy Engineering, Beijing University of Technology, Beijing 100124 (China)

    2017-02-28

    Highlights: • The framework-structured of cryptomelane-type manganese oxide octahedral molecular sieve (OMS-2) has a 2 × 2 square tunnel. • Preparation route has an important impact on physicochemical property of the product. • Pd/OMS-2-DP via the deposition-precipitation route shows excellent catalytic activity. • Pd surface loading, surface atomic ratio of Mn ions, lattice oxygen mobility, oxygen vacancy, reducibility and acidity govern activity. - Abstract: The cryptomelane-type manganese oxide octahedral molecular sieve (OMS-2)-supported Pd (0.5 wt% Pd/OMS-2-DP, 0.5 wt% Pd/OMS-2-PI, and 0.5 wt% Pd/OMS-2-EX) catalysts were prepared by the deposition-precipitation, pre-incorporation, and ion-exchanging strategies, respectively. It is shown that the preparation method exerted an important effect on the physicochemical property of the sample. Among the OMS-2-supported Pd catalysts, 0.5 wt% Pd/OMS-2-DP possessed the highest surface (Mn{sup 2+} + Mn{sup 3+})/Mn{sup 4+} atomic ratio and the highest surface Pd loading and acid sites. The 0.5 wt% Pd/OMS-2 catalysts outperformed the Pd-free counterpart, among which 0.5 wt% Pd/OMS-2-DP presented the best catalytic activity (T{sub 50%} and T{sub 90%} were 25 and 55 °C for CO oxidation, 240 and 285 °C for toluene oxidation, and 160 and 200 °C for ethyl acetate oxidation, respectively). We believe that the high Pd surface loading, high surface atomic ratio of (Mn{sup 2+} + Mn{sup 3+})/Mn{sup 4+}, and good low-temperature reducibility, good oxygen mobility, and high acidity were responsible for the excellent performance of the 0.5 wt% Pd/OMS-2-DP catalyst.

  10. Effect of preparation method on the surface characteristics and activity of the Pd/OMS-2 catalysts for the oxidation of carbon monoxide, toluene, and ethyl acetate

    International Nuclear Information System (INIS)

    Liu, Lisha; Song, Yong; Fu, Zhidan; Ye, Qing; Cheng, Shuiyuan; Kang, Tianfang; Dai, Hongxing

    2017-01-01

    Highlights: • The framework-structured of cryptomelane-type manganese oxide octahedral molecular sieve (OMS-2) has a 2 × 2 square tunnel. • Preparation route has an important impact on physicochemical property of the product. • Pd/OMS-2-DP via the deposition-precipitation route shows excellent catalytic activity. • Pd surface loading, surface atomic ratio of Mn ions, lattice oxygen mobility, oxygen vacancy, reducibility and acidity govern activity. - Abstract: The cryptomelane-type manganese oxide octahedral molecular sieve (OMS-2)-supported Pd (0.5 wt% Pd/OMS-2-DP, 0.5 wt% Pd/OMS-2-PI, and 0.5 wt% Pd/OMS-2-EX) catalysts were prepared by the deposition-precipitation, pre-incorporation, and ion-exchanging strategies, respectively. It is shown that the preparation method exerted an important effect on the physicochemical property of the sample. Among the OMS-2-supported Pd catalysts, 0.5 wt% Pd/OMS-2-DP possessed the highest surface (Mn 2+ + Mn 3+ )/Mn 4+ atomic ratio and the highest surface Pd loading and acid sites. The 0.5 wt% Pd/OMS-2 catalysts outperformed the Pd-free counterpart, among which 0.5 wt% Pd/OMS-2-DP presented the best catalytic activity (T 50% and T 90% were 25 and 55 °C for CO oxidation, 240 and 285 °C for toluene oxidation, and 160 and 200 °C for ethyl acetate oxidation, respectively). We believe that the high Pd surface loading, high surface atomic ratio of (Mn 2+ + Mn 3+ )/Mn 4+ , and good low-temperature reducibility, good oxygen mobility, and high acidity were responsible for the excellent performance of the 0.5 wt% Pd/OMS-2-DP catalyst.

  11. Electro-deposition of Pd on carbon paper and Ni foam via surface limited redox-replacement reaction for oxygen reduction reaction

    CSIR Research Space (South Africa)

    Modibedi, RM

    2014-05-01

    Full Text Available Pd nanostructured catalysts were electrodeposited by surface-limited redox replacement reactions usingthe electrochemical atomic layer deposition technique. Carbon paper and Ni foam were used as substratesfor the electrodeposition of the metal...

  12. DFT study of Hg adsorption on M-substituted Pd(1 1 1) and PdM/γ-Al2O3(1 1 0) (M = Au, Ag, Cu) surfaces

    Science.gov (United States)

    Wang, Jiancheng; Yu, Huafeng; Geng, Lu; Liu, Jianwen; Han, Lina; Chang, Liping; Feng, Gang; Ling, Lixia

    2015-11-01

    The adsorption of Hgn (n = 1-3) on the Au-, Ag-, Cu-substituted Pd(1 1 1) surfaces as well as the PdM/γ-Al2O3(1 1 0) (M = Au, Ag, Cu) surfaces has been investigated using spin-polarized density functional theory calculations. It is found that M-substituted Pd(1 1 1) surfaces show as good Hg adsorption capacity as the perfect Pd(1 1 1) at low Hg coverage, while the Hg adsorption capacity is only slightly weakened at high Hg coverage. On the basis of stepwise adsorption energies analysis, it is concluded that M-substituted Pd(1 1 1) surfaces can contribute to the binding of Hg atom on the surfaces at high Hg coverage. The electronic properties of the second metal atoms are the main factor contributes to the Hg adsorption capacity. Gas phase Pd2 shows better Hg adsorption capacity than Pd2/γ-Al2O3, while PdM/γ-Al2O3 can adsorb Hg more efficiently than bare PdM clusters. It suggests that the γ-Al2O3 support can enhance the activity of PdM for Hg adsorption and reduces the activity of Pd2. It is also found that Pd is the main active composition responsible for the interaction of mercury with the surface for PdM/γ-Al2O3 sorbent. Taking Hg adsorption capacity and economic costs into account, Cu addition is a comparatively good candidate for Hg capture.

  13. Slab model studies of water adsorption and decomposition on clean and X- (X = C, N and O) contaminated Pd(111) surfaces.

    Science.gov (United States)

    Cao, Yilin; Chen, Zhao-Xu

    2007-02-14

    To explore the effect of surface contaminants on water chemistry at metallic surfaces, adsorption and decomposition of water monomers on clean and X/Pd(111)(X = C, N and O) surfaces are investigated based on density functional theory calculations. It is revealed that H(2)O binds to Pd(111) surface primarily through the mixing of its 1b(1) with the Pd 4d(z(2)) state. A charge accumulation between the oxygen atom of water and the bound Pd atom is calculated, which is found to be relevant to the H(2)O-Pd interaction. Water adsorption results in a reduction of surface work function and the polarization of the X 2p states. The O-H bond scission of H(2)O on the clean Pd(111) is an energy unfavorable process. In the case of X-assisted O-H bond breaking on X/Pd(111) surfaces, however, the reaction barrier tends to be lower than that on the clean surface and decreases from C/Pd(111) to O/Pd(111). In particular, water decomposition is found to become feasible on O/Pd(111), in agreement with the experimental observations. The calculated barrier is demonstrated to be correlated linearly with the density of X 2p states at the Fermi level. A thorough energy analysis demonstrates that the following geometrical and electronic factors favor the barrier reduction on X/Pd(111) with respect to water decomposition on clean Pd(111): (i) the less deformed structure of water in TS; (ii) the decreased bonding competition between the fragments OH and H. The remarkable decrease of the barrier on O/Pd(111) is revealed to be due to the largest stabilization of the split H atom and the least deformation of water in the TS.

  14. Hydrogen adsorption on bimetallic PdAu(111) surface alloys

    DEFF Research Database (Denmark)

    Takehiro, Naoki; Liu, Ping; Bergbreiter, Andreas

    2014-01-01

    The adsorption of hydrogen on structurally well defined PdAu-Pd(111) monolayer surface alloys was investigated in a combined experimental and theoretical study, aiming at a quantitative understanding of the adsorption and desorption properties of individual PdAu nanostructures. Combining...... the structural information obtained by high resolution scanning tunneling microscopy (STM), in particular on the abundance of specific adsorption ensembles at different Pd surface concentrations, with information on the adsorption properties derived from temperature programmed desorption (TPD) spectroscopy...... and high resolution electron energy loss spectroscopy (HREELS) provides conclusions on the minimum ensemble size for dissociative adsorption of hydrogen and on the adsorption energies on different sites active for adsorption. Density functional theory (DFT) based calculations give detailed insight...

  15. Surface, segregation profile for Ni50Pd50(100)

    DEFF Research Database (Denmark)

    Christensen, Asbjørn; Ruban, Andrei; Skriver, Hans Lomholt

    1997-01-01

    A recent dynamical LEED study [G.N. Derry, C.B. McVey, P.J. Rous, Surf. Sci. 326 (1995) 59] reported an oscillatory surface segregation profile in the Ni50Pd50(100) system with the surface layer enriched by Pd. We have performed ab-initio total-energy calculations for the surface of this alloy...... system using the coherent potential approximation and obtain an oscillatory segregation profile, in agreement with experiments. We discuss the energetic origin of the oscillatory segregation profile in terms of effective cluster interactions. We include relaxation effects by means of the semi...

  16. The vibrational spectrum of the atoms in the grain boundaries of nanocrystalline Pd

    Energy Technology Data Exchange (ETDEWEB)

    Stuhr, U. [Paul Scherrer Inst. (PSI), Villigen (Switzerland); Wipf, H.; Hahn, H. [Technische Hochschule Darmstadt (Germany); Natter, H.; Hemperlmann, R. [Universitaet des Saarlandes, Saarbruecken (Germany); Andersen, K. [Institut Max von Laue - Paul Langevin (ILL), 38 - Grenoble (France)

    1997-09-01

    The vibrational excitations of the atoms in nanocrystalline Pd was investigated by neutron-time-of-flight spectroscopy. Hydrogen was used as a probe for the vibrations in the grain boundaries. The separation between the H and Pd vibrations was done by spin analysis. The results show that in the grain boundary the density of states of low energy excitations ({<=}5 meV) is drastically increased. (author) 3 figs., 3 refs.

  17. Structural characterization of Pt-Pd and Pd-Pt core-shell nanoclusters at atomic resolution.

    Science.gov (United States)

    Sanchez, Sergio I; Small, Matthew W; Zuo, Jian-min; Nuzzo, Ralph G

    2009-06-24

    We describe the results of a study at atomic resolution of the structures exhibited by polymer-capped monometallic and bimetallic Pt and Pd nanoclusters--models for nanoscale material electrocatalysts--as carried out using an aberration-corrected scanning transmission electron microscope (STEM). The coupling of sub-nanometer resolution with Z-contrast measurements provides unprecedented insights into the atomic structures and relative elemental speciation of Pt and Pd within these clusters. The work further defines the nature of deeply quenched states that prevent facile conversions of core-shell motifs to equilibrium alloys and the nature of nonidealities such as twinning (icosahedral cores) and atomic segregation that these structures can embed. The nature of the facet structure present in these model systems is revealed by theory directed modeling in which experimental intensity profiles obtained in Z-contrast measurements at atomic resolution are compared to simulated intensity profiles using theoretically predicted cluster geometries. These comparisons show close correspondences between experiment and model and highlight striking structural complexities in these systems that are compositionally sensitive and subject to amplification by subsequent cluster growth processes. The work demonstrates an empowering competency in nanomaterials research for STEM measurements carried out using aberration corrected microscopes, approaches that hold considerable promise for characterizing the structure of these and other important catalytic materials systems at the atomic scale.

  18. Calculation of the vibration properties of the Pd/Au (111 ordered surface alloy in its stable domain

    Directory of Open Access Journals (Sweden)

    Tigrine R.

    2012-06-01

    Full Text Available In the present paper, a calculation is presented for the vibration properties of the ordered surface alloy alloy Au(111 − (√3×√3R30° − Pd, which is a stable system in the temperature range of 500K to 600K. This surface alloy is formed by depositing Pd atoms onto the Au(111surface, and annealing at higher temperatures. The matching theory is applied to calculate the surface phonons and local vibration densities of states (LDOS for the clean Au (111 surface, and for the Au(111 − (√3×√3R30° − Pd surface alloy. Our theoretical results for the surface phonon branches of the clean Au (111 surface compare favorably with previous ab initio results and experimental data. In contrast, there are no previous results for the vibrational LDOS for the atomic Au site in a clean Au (111 surface, or results for the surface phonons and vibration spectra for the surface alloy. The surface phonons are calculated for the clean Au (111 surface and the ordered surface alloy along three directions of high symmetry, namely, ΓΜ¯, MML:MK¯ $overline {Gamma {m M}} ,{m{ }}overline {{m{MK}}} $ , and KΓ¯ $overline {KGamma } $ . The phonon branches are strongly modified from the Au (111 surface to the surface alloy. In particular a remarkable change takes place for the LDOS between the clean Au (111 surface and the surface alloy, which may find its origin in the charge transfer from Au atoms to Pd atoms.

  19. DFT study of Hg adsorption on M-substituted Pd(1 1 1) and PdM/γ-Al{sub 2}O{sub 3}(1 1 0) (M = Au, Ag, Cu) surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Jiancheng; Yu, Huafeng [Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024 (China); Geng, Lu [College of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan 030024 (China); Liu, Jianwen [National Supercomputing Center in Shenzhen, Shenzhen 518055 (China); Han, Lina, E-mail: hanlina@tyut.edu.cn [College of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan 030024 (China); Chang, Liping [Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024 (China); Feng, Gang, E-mail: fengg.sshy@sinopec.com [Shanghai Research Institute of Petrochemical Technology SINOPEC, Shanghai 201208 (China); College of Chemistry, Nanchang University, Nanchang, Jiangxi 330031 (China); Ling, Lixia [Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024 (China)

    2015-11-15

    Graphical abstract: - Highlights: • M-substituted Pd surfaces show good Hg adsorption capacity at low Hg coverage. • γ-Al{sub 2}O{sub 3} can enhance the activity of bimetallic PdM for Hg adsorption. • Pd is the main active composition of PdM/γ-Al{sub 2}O{sub 3} sorbent for Hg adsorption. • Cu addition is a better than Au and Ag for the Pd-based Hg adsorbents. - Abstract: The adsorption of Hg{sub n} (n = 1–3) on the Au-, Ag-, Cu-substituted Pd(1 1 1) surfaces as well as the PdM/γ-Al{sub 2}O{sub 3}(1 1 0) (M = Au, Ag, Cu) surfaces has been investigated using spin-polarized density functional theory calculations. It is found that M-substituted Pd(1 1 1) surfaces show as good Hg adsorption capacity as the perfect Pd(1 1 1) at low Hg coverage, while the Hg adsorption capacity is only slightly weakened at high Hg coverage. On the basis of stepwise adsorption energies analysis, it is concluded that M-substituted Pd(1 1 1) surfaces can contribute to the binding of Hg atom on the surfaces at high Hg coverage. The electronic properties of the second metal atoms are the main factor contributes to the Hg adsorption capacity. Gas phase Pd{sub 2} shows better Hg adsorption capacity than Pd{sub 2}/γ-Al{sub 2}O{sub 3}, while PdM/γ-Al{sub 2}O{sub 3} can adsorb Hg more efficiently than bare PdM clusters. It suggests that the γ-Al{sub 2}O{sub 3} support can enhance the activity of PdM for Hg adsorption and reduces the activity of Pd{sub 2}. It is also found that Pd is the main active composition responsible for the interaction of mercury with the surface for PdM/γ-Al{sub 2}O{sub 3} sorbent. Taking Hg adsorption capacity and economic costs into account, Cu addition is a comparatively good candidate for Hg capture.

  20. Adsorption of Ni, Pd, Pt, Cu, Ag and Au on the Fe3O4(111) surface

    Science.gov (United States)

    Yu, Xiaohu; Tian, Xinxin; Wang, Shengguang

    2014-10-01

    The interaction of Group 10 and 11 transition metals with the magnetite (111) surface has been investigated using the GGA + U density functional theory and periodic slab surface models. It was found that these transition metals adsorb stronger on an oxygen-terminated magnetite (111) surface than on an iron-terminated surface. On an oxygen-terminated surface, the adsorption strength is in the order of Ni > Pt Cu > Pd > Ag Au. In contrast, the order on an iron-terminated surface is Ni > Pt Cu > Au > Pd Ag. The adsorption strength was found to correlate well with the average lengths of metal-oxygen bonds. The magnetite (111) surfaces largely modify the electronic structures of the transition metals. Compared to their density of states in bulk structures, the atomically adsorbed transition metals have narrower d bands, and their d-band centers are closer to the Fermi levels. This implies the higher activities of the atomically adsorbed transition metals.

  1. Atomic displacements due to interstitial hydrogen in Cu and Pd

    Indian Academy of Sciences (India)

    Abstract. The density functional theory (DFT) is used to study the atomic interac- tions in transition metal-based interstitial alloys. The strain field is calculated in the discrete lattice model using Kanzaki method. The total energy and hence atomic forces between interstitial hydrogen and transition metal hosts are calculated ...

  2. Atomic clusters and atomic surfaces in icosahedral quasicrystals.

    Science.gov (United States)

    Quiquandon, Marianne; Portier, Richard; Gratias, Denis

    2014-05-01

    This paper presents the basic tools commonly used to describe the atomic structures of quasicrystals with a specific focus on the icosahedral phases. After a brief recall of the main properties of quasiperiodic objects, two simple physical rules are discussed that lead one to eventually obtain a surprisingly small number of atomic structures as ideal quasiperiodic models for real quasicrystals. This is due to the fact that the atomic surfaces (ASs) used to describe all known icosahedral phases are located on high-symmetry special points in six-dimensional space. The first rule is maximizing the density using simple polyhedral ASs that leads to two possible sets of ASs according to the value of the six-dimensional lattice parameter A between 0.63 and 0.79 nm. The second rule is maximizing the number of complete orbits of high symmetry to construct as large as possible atomic clusters similar to those observed in complex intermetallic structures and approximant phases. The practical use of these two rules together is demonstrated on two typical examples of icosahedral phases, i-AlMnSi and i-CdRE (RE = Gd, Ho, Tm).

  3. Effects of atomic and magnetic order on electronic transport in Pd-richPd-Fe alloys

    Czech Academy of Sciences Publication Activity Database

    Kudrnovský, Josef; Drchal, Václav; Khmelevskyi, S.; Turek, Ilja

    2011-01-01

    Roč. 84, č. 21 (2011), "214436-1"-"214436-8" ISSN 1098-0121 R&D Projects: GA ČR(CZ) GAP204/11/1228 Institutional research plan: CEZ:AV0Z10100520; CEZ:AV0Z20410507 Keywords : residual resistivity * anisotropic magnetoresistance * anomalous Hall effect * PdFe-alloys * spin-orbit coupling * theory Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 3.691, year: 2011

  4. High-temperature stability of Au/Pd/Cu and Au/Pd(P)/Cu surface finishes

    Science.gov (United States)

    Ho, C. E.; Hsieh, W. Z.; Lee, P. T.; Huang, Y. H.; Kuo, T. T.

    2018-03-01

    Thermal reliability of Au/Pd/Cu and Au/Pd(4-6 wt.% P)/Cu trilayers in the isothermal annealing at 180 °C were investigated by X-ray photoelectron spectroscopy (XPS), time-of-flight secondary ion mass spectrometry (TOF-SIMS), and transmission electron microscopy (TEM). The pure Pd film possessed a nanocrystalline structure with numerous grain boundaries, thereby facilitating the interdiffusion between Au and Cu. Out-diffusion of Cu through Pd and Au grain boundaries yielded a significant amount of Cu oxides (CuO and Cu2O) over the Au surface and gave rise to void formation in the Cu film. By contrast, the Pd(P) film was amorphous and served as a good diffusion barrier against Cu diffusion. The results of this study indicated that amorphous Pd(P) possessed better oxidation resistance and thermal reliability than crystalline Pd.

  5. Controlled decoration of Pd on Ni(OH)2 nanoparticles by atomic layer deposition for high ethanol oxidation activity

    Science.gov (United States)

    Jiang, Yiwu; Chen, Jinwei; Zhang, Jie; Zeng, Yaping; Wang, Yichun; Zhou, Feilong; Kiani, Maryam; Wang, Ruilin

    2017-10-01

    A new catalysts electrode was prepared by in situ controllable deposition of Pd shell layer on the gas diffusion layer (GDL) supported Ni(OH)2 nanoparticles using atomic layer deposition (ALD) technology. High resolution transmission electron microscope confirmed that the Ni(OH)2 core was coated by several atomic layers of Pd. The core-shell Ni(OH)2@Pd catalysts with different thickness of Pd shell are easily prepared by controlling ALD cycle. Electrochemical tests showed that the 100-Ni(OH)2@Pd/GDL catalyst prepared via 100 ALD cycles presented the highest catalytic activity for ethanol electro-oxidation reaction (EOR). The peaking current density of Ni(OH)2@Pd/GDL was 1439 mA mgPd-1, which was about 2.75 times as high as that of Pd/GDL (522 mA mgPd-1). The shift in binding energy of the XPS peak of Pd in Ni(OH)2@Pd catalyst confirmed the strong interaction between the Pd shell and the Ni(OH)2 core. We suggested that the high catalytic activity of Ni(OH)2@Pd/GDL catalyst layer may be due to following factors: high Pd dispersion arising from the core-shell structure, high Pd utilization because of the in situ deposition of Pd on catalyst layer and the interaction between the Pd shell and the Ni(OH)2 core. Herein, the ALD technology exhibits a promising application prospect for preparing core-shell structure and precisely controlling shell thickness of nano-composite as an electro-catalyst toward EOR.

  6. Atomically flat single terminated oxide substrate surfaces

    Science.gov (United States)

    Biswas, Abhijit; Yang, Chan-Ho; Ramesh, Ramamoorthy; Jeong, Yoon H.

    2017-05-01

    Scientific interest in atomically controlled layer-by-layer fabrication of transition metal oxide thin films and heterostructures has increased intensely in recent decades for basic physics reasons as well as for technological applications. This trend has to do, in part, with the coming post-Moore era, and functional oxide electronics could be regarded as a viable alternative for the current semiconductor electronics. Furthermore, the interface of transition metal oxides is exposing many new emergent phenomena and is increasingly becoming a playground for testing new ideas in condensed matter physics. To achieve high quality epitaxial thin films and heterostructures of transition metal oxides with atomically controlled interfaces, one critical requirement is the use of atomically flat single terminated oxide substrates since the atomic arrangements and the reaction chemistry of the topmost surface layer of substrates determine the growth and consequent properties of the overlying films. Achieving the atomically flat and chemically single terminated surface state of commercially available substrates, however, requires judicious efforts because the surface of as-received substrates is of chemically mixed nature and also often polar. In this review, we summarize the surface treatment procedures to accomplish atomically flat surfaces with single terminating layer for various metal oxide substrates. We particularly focus on the substrates with lattice constant ranging from 4.00 Å to 3.70 Å, as the lattice constant of most perovskite materials falls into this range. For materials outside the range, one can utilize the substrates to induce compressive or tensile strain on the films and explore new states not available in bulk. The substrates covered in this review, which have been chosen with commercial availability and, most importantly, experimental practicality as a criterion, are KTaO3, REScO3 (RE = Rare-earth elements), SrTiO3, La0.18Sr0.82Al0.59Ta0.41O3 (LSAT), Nd

  7. Spin fluctuation effects on the conductance through a single Pd atom contact

    International Nuclear Information System (INIS)

    Romero, M A; Goldberg, E C; Gomez-Carrillo, S C; Bolcatto, P G

    2009-01-01

    A controversy about the conductance through single atoms still exists. There are many experiments where values lower than the quantum unity G 0 = 2e 2 /h have been found associated to Kondo regimes with high Kondo temperatures. Specifically in the Pd single atom contact, conductance values close to G 0 /2 at room temperature have been reported. In this work we propose a theoretical analysis of a break junction of Pd where the charge fluctuation in the single atom contact is limited to the most probable one: d 10 ↔d 9 . The projected density of states and the characteristics of the electron transport are calculated by using a realistic description of the interacting system. A Kondo regime is found where the conductance values and their dependence on temperature are in good agreement with the experimental trends observed in the conduction of single molecule transistors based on transition metal coordination complexes.

  8. Melting phenomena: effect of composition for 55-atom Ag-Pd bimetallic clusters.

    Science.gov (United States)

    Cheng, Daojian; Wang, Wenchuan; Huang, Shiping

    2008-05-14

    Understanding the composition effect on the melting processes of bimetallic clusters is important for their applications. Here, we report the relationship between the melting point and the metal composition for the 55-atom icosahedral Ag-Pd bimetallic clusters by canonical Monte Carlo simulations, using the second-moment approximation of the tight-binding potentials (TB-SMA) for the metal-metal interactions. Abnormal melting phenomena for the systems of interest are found. Our simulation results reveal that the dependence of the melting point on the composition is not a monotonic change, but experiences three different stages. The melting temperatures of the Ag-Pd bimetallic clusters increase monotonically with the concentration of the Ag atoms first. Then, they reach a plateau presenting almost a constant value. Finally, they decrease sharply at a specific composition. The main reason for this change can be explained in terms of the relative stability of the Ag-Pd bimetallic clusters at different compositions. The results suggest that the more stable the cluster, the higher the melting point for the 55-atom icosahedral Ag-Pd bimetallic clusters at different compositions.

  9. Surface electronic properties of discontinuous Pd films during hydrogen exposure

    International Nuclear Information System (INIS)

    Zhao, Ming; Nagata, Shinji; Shikama, Tatsuo; Inouye, Aichi; Yamamoto, Shunya; Yoshikawa, Masahito

    2011-01-01

    This paper explored the change in the surface resistance of the discontinuous palladium (Pd) films during hydrogen exposure. In our experiments, we observed a remarkable rise in the electrical resistance of the discontinuous film which consists of nano-sized particles, when it was exposed to thin hydrogen. By studying the resistance change ratio before and after hydrogen exposure, we have found that it demonstrates an inverse exponential relationship with the ratio of on-film particle radius to the inter island separation. This suggests that the change in the film resistance under hydrogen exposure is primarily associated with the variation of surface work function which is caused by the hydrogen absorption on the Pd surface. (author)

  10. Surface Plasmon Polaritons Probed with Cold Atoms

    DEFF Research Database (Denmark)

    Kawalec, Tomasz; Sierant, Aleksandra; Panas, Roman

    2017-01-01

    We report on an optical mirror for cold rubidium atoms based on a repulsive dipole potential created by means of a modified recordable digital versatile disc. Using the mirror, we have determined the absolute value of the surface plasmon polariton (SPP) intensity, reaching 90 times the intensity...

  11. Controllable irregular phenomenon induced by Ag atomic segregation on the melting of (AgPd)561 bimetallic clusters

    Science.gov (United States)

    Li, Guojian; Wang, Qiang; Liu, Tie; Wang, Kai; Wu, Chun; He, Jicheng

    2012-08-01

    This paper studies the melting of Ag-Pd bimetallic clusters with different Ag concentrations and atomic distributions by using molecular dynamics simulation with a general embedded-atom method. The melting of a cluster with 45 % Ag atoms distributing in the core was compared with that of 45 %, 15 % Ag on the surface and 15 % Ag in the core. It is found that the energy variation with the increasing temperature is strongly related to the Ag atomic segregation, due to the reason that there is a competition between the decreased energy induced by the atomic segregation and the increased energy as the temperature increases. The melting of the Ag-core clusters with different Ag concentrations from 5 to 55 % Ag was further explored. It is found that the irregular variation of energy occurred that the atomic energy increases, keeps unchanged or decreases with the increase of the temperature. Furthermore, the irregular phenomena of the melting were induced by the Ag concentrations. This gives a new method to tune the melting in bimetallic clusters.

  12. Atom diffraction reveals the impact of atomic core electrons on atom-surface potentials.

    Science.gov (United States)

    Lonij, Vincent P A; Klauss, Catherine E; Holmgren, William F; Cronin, Alexander D

    2010-12-03

    We measured ratios of van der Waals potential coefficients (C3) for different atoms (Li, Na, K, and Rb) interacting with the same surface by studying atom diffraction from a nanograting. These measurements are a sensitive test of atomic structure calculations because C3 ratios are strongly influenced by core electrons and only weakly influenced by the permittivity and geometry of the surface. Our measurement uncertainty of 2% in the ratio C(3)(K)/C(3)(Na) is close to the uncertainty of the best theoretical predictions, and some of these predictions are inconsistent with our measurement.

  13. Mechanistic insight into the enhanced photocatalytic activity of single-atom Pt, Pd or Au-embedded g-C3N4

    Science.gov (United States)

    Tong, Tong; Zhu, Bicheng; Jiang, Chuanjia; Cheng, Bei; Yu, Jiaguo

    2018-03-01

    Single atoms of platinum (Pt), palladium (Pd) or gold (Au) trapped by two-dimensional graphitic carbon nitride (g-C3N4) exhibit superior photocatalytic performance. However, the underlying mechanism of single-atom noble metal/g-C3N4 photocatalytic system is still unclear. Herein, the structural, electronic and optical properties of single-atom Pt, Pd and Au loaded on bilayer g-C3N4 (BL-g-C3N4) substrate were investigated by density functional theory (DFT) simulations. The results indicate that single-atom Pt/Pd/Au loading can significantly narrow the band gap of g-C3N4 and thus increase its light absorption in the visible-light region. Rather than being adsorbed on the surface, Pt and Pd atoms tend to be embedded into g-C3N4 interlayer and act as bridges to facilitate the interlayer charge carrier transfer due to the effects of conduction band offset. In particular, an internal electric field is generated in Pt/BL-g-C3N4, which is further beneficial for separating charge carrier of photoexcited g-C3N4. By contrast, Au can only be adsorbed on the g-C3N4 surface (in the six-fold cavity) and deliver a limited amount of charge carrier excited in the N-conjugated aromatic pore of g-C3N4 surface. Our finding is conducive to understanding the interactive relationship between single-atom noble metal co-catalysts and g-C3N4 and to the design of high-efficiency photocatalyst.

  14. Catalytic Conversion of Short-Chain Alcohols on Atomically Dispersed Au and Pd Supported on Nanoscale Metal Oxides

    Science.gov (United States)

    Wang, Chongyang

    Au and Pd from Group IB and Group VIII, respectively, for methanol and ethanol alcohol reforming reactions employing a novel ZnZrOx composite oxide as a platform catalyst support. Comprehensive study of Au catalyst has deepened our understanding of atomically dispersed Au anchored on various supports through oxygen bonds as the active sites for alcohol reforming reactions, and showed the support effect to be indirect, serving as the carrier and stabilizer of the gold species. For Pd, the Zn species of the composite oxide is necessary to modify the Pd catalyst and the PdZn alloy gives it the desired Au-like properties. Full characterization of the catalysts used here by ICP, XPS, XRD, FTIR and STEM imaging was conducted throughout the thesis to identify the stable species and correlate the catalyst performance with its composition and morphology. Surface acidity titration by isopropanol temperature-programmed desorption/mass spectrometry (IPA-TPD/MS) and pyridine-IR adsorption/desorption was conducted in parallel to temperature-programmed surface reaction (TPSR) studies and products from isothermal steady-state reactions were monitored online by mass spectrometry.

  15. Pd adsorption on Si(1 1 3) surface: STM and XPS study

    International Nuclear Information System (INIS)

    Hara, Shinsuke; Yoshimura, Masamichi; Ueda, Kazuyuki

    2008-01-01

    Pd-induced surface structures on Si(1 1 3) have been studied by scanning tunneling microscopy (STM) and X-ray photoelectron spectroscopy (XPS). In the initial process of the Pd adsorption below 0.10 ML, Pd silicide (Pd 2 Si) clusters are observed to form randomly on the surface. By increasing the Pd coverage to 0.10 ML, the clusters cover the entire surface, and an amorphous layer is formed. After annealing the Si(1 1 3)-Pd surface at 600 deg. C, various types of islands and chain protrusions appears. The agglomeration, coalescence and crystallization of these islands are observed by using high temperature (HT-) STM. It is also found by XPS that the islands correspond to Pd 2 Si structure. On the basis of these results, evolution of Pd-induced structures at high temperatures is in detail discussed

  16. Triboelectric Hydrogen Gas Sensor with Pd Functionalized Surface

    Directory of Open Access Journals (Sweden)

    Sung-Ho Shin

    2016-10-01

    Full Text Available Palladium (Pd-based hydrogen (H2 gas sensors have been widely investigated thanks to its fast reaction and high sensitivity to hydrogen. Various sensing mechanisms have been adopted for H2 gas sensors; however, all the sensors must be powered through an external battery. We report here an H2 gas sensor that can detect H2 by measuring the output voltages generated during contact electrification between two friction surfaces. When the H2 sensor, composed of Pd-coated ITO (indium tin oxide and PET (polyethylene Terephthalate film, is exposed to H2, its output voltage is varied in proportion to H2 concentration because the work function (WF of Pd-coated surface changes, altering triboelectric charging behavior. Specifically, the output voltage of the sensor is gradually increased as exposing H2 concentration increases. Reproducible and sensitive sensor response was observed up 1% H2 exposure. The approach introduced here can easily be adopted to development of triboelectric gas sensors detecting other gas species.

  17. Comparison of bacterial cells and amine-functionalized abiotic surfaces as support for Pd nanoparticle synthesis

    DEFF Research Database (Denmark)

    De Corte, Simon; Bechstein, Stefanie; Lokanathan, Arcot R.

    2013-01-01

    An increasing demand for catalytic Pd nanoparticles has motivated the search for sustainable production methods. An innovative approach uses bacterial cells as support material for synthesizing Pd nanoparticles by reduction of Pd(II) with e.g. hydrogen or formate. Nevertheless, drawbacks...... nanoparticles, and that abiotic surfaces could support the Pd particle synthesis as efficiently as bacteria. In this study, we explore the possibility of replacing bacteria with amine-functionalized materials, and we compare different functionalization strategies. Pd nanoparticles formed on the support...... on these surfaces was higher than for Pd particles formed on Shewanella oneidensis cells. Smaller Pd nanoparticles generally have better catalytic properties, and previous studies have shown that the particle size can be lowered by increasing the amount of support material used during Pd particle formation. However...

  18. Effects of single metal atom (Pt, Pd, Rh and Ru) adsorption on the photocatalytic properties of anatase TiO2

    Science.gov (United States)

    Jin, Cui; Dai, Ying; Wei, Wei; Ma, Xiangchao; Li, Mengmeng; Huang, Baibiao

    2017-12-01

    The effects of single metal atom (Pt, Pd, Rh and Ru) adsorption on the photocatalytic properties of anatase TiO2 are investigated by means of the first-principles calculations based on density functional theory (DFT). Our results show that the most stable adsorption site for single metal atom on anatase TiO2 (101) surface is the bridge site formed by two twofold coordinated oxygen (O2c) atoms at the step edge. Due to the charge transfer from metal atoms to anatase TiO2 (101) surface, the work function of adsorbed surface is significantly smaller than the clean one, indicating enhanced surface activity. Fukui functions are highly localized around the isolated metal atoms, indicating that single metal atoms on anatase TiO2 (101) surface serve as the active reduction and oxidation sites in the photocatalytic process. Photo-induced electrons in the electronically excited TiO2 photocatalyst can be transferred to target species through the deposited single atoms. The band structures of host TiO2 are almost unchanged upon the adsorption, and the metal induced states are located in the band gap of the host. Remarkably, due to the metal atoms adsorption, the upward shift of conduction band edge will improve the reducing capacity of anatase TiO2. Moreover, when single metal atoms are adsorbed, potential energy of topmost surface Ti atoms turns to get close to the vacuum level, which significantly facilitates the electron transfer for hydrogen evolution. Results in this work provide new insights into improving the photocatalytic performance by single metal atoms adsorption.

  19. Phonon lineshapes in atom-surface scattering

    Energy Technology Data Exchange (ETDEWEB)

    MartInez-Casado, R [Department of Chemistry, Imperial College London, South Kensington, London SW7 2AZ (United Kingdom); Sanz, A S; Miret-Artes, S [Instituto de Fisica Fundamental, Consejo Superior de Investigaciones CientIficas, Serrano 123, E-28006 Madrid (Spain)

    2010-08-04

    Phonon lineshapes in atom-surface scattering are obtained from a simple stochastic model based on the so-called Caldeira-Leggett Hamiltonian. In this single-bath model, the excited phonon resulting from a creation or annihilation event is coupled to a thermal bath consisting of an infinite number of harmonic oscillators, namely the bath phonons. The diagonalization of the corresponding Hamiltonian leads to a renormalization of the phonon frequencies in terms of the phonon friction or damping coefficient. Moreover, when there are adsorbates on the surface, this single-bath model can be extended to a two-bath model accounting for the effect induced by the adsorbates on the phonon lineshapes as well as their corresponding lineshapes.

  20. Mechanism of yttrium atom formation in electrothermal atomization from metallic and metal-carbide surfaces of a heated graphite atomizer in atomic absorption spectrometry

    International Nuclear Information System (INIS)

    Wahab, H.S.; Chakrabarti, C.L.

    1981-01-01

    Mechanism of Y atom formation from pyrocoated graphite, tantalum and tungsten metal surfaces of a graphite tube atomizer has been studied and a mechanism for the formation for Y atoms is proposed for the first time. (author)

  1. Self-excitation of Rydberg atoms at a metal surface

    DEFF Research Database (Denmark)

    Bordo, Vladimir

    2017-01-01

    field of the metal surface acts as an active device that supports sustained atomic dipole oscillations, which generate, in their turn, an electromagnetic field. This phenomenon does not exploit stimulated emission and therefore does not require population inversion in atoms. An experiment with Rydberg......The novel effect of self-excitation of an atomic beam propagating above a metal surface is predicted and a theory is developed. Its underlying mechanism is positive feedback provided by the reflective surface for the atomic polarization. Under certain conditions the atomic beam flying in the near...... atoms in which this effect should be most pronounced is proposed and the necessary estimates are given....

  2. Isolation and Structural Characterization of a Mackay 55-Metal-Atom Two-Shell Icosahedron of Pseudo-Ih Symmetry, Pd55L12(μ3-CO)20 (L = PR3, R = Isopropyl): Comparative Analysis with Interior Two-Shell Icosahedral Geometries in Capped Three-Shell Pd145, Pt-Centered Four-Shell Pd-Pt M165, and Four-Shell Au133 Nanoclusters.

    Science.gov (United States)

    Erickson, Jeremiah D; Mednikov, Evgueni G; Ivanov, Sergei A; Dahl, Lawrence F

    2016-02-10

    We present the first successful isolation and crystallographic characterization of a Mackay 55-metal-atom two-shell icosahedron, Pd55L12(μ3-CO)20 (L = PPr(i)3) (1). Its two-shell icosahedron of pseudo-Ih symmetry (without isopropyl substituents) enables a structural/bonding comparison with interior 55-metal-atom two-shell icosahedral geometries observed within the multi-shell capped 145-metal-atom three-shell Pd145(CO)72(PEt3)30 and 165-metal-atom four-shell Pt-centered (μ12-Pt)Pd164-xPtx(CO)72(PPh3)20 (x ≈ 7) nanoclusters, and within the recently reported four-shell Au133(SC6H4-p-Bu(t))52 nanocluster. DFT calculations carried out on a Pd55(CO)20(PH3)12 model analogue, with triisopropyl phosphine substituents replaced by H atoms, revealed a positive +0.84 e charge for the entire Pd55 core, with a highly positive second-shell Pd42 surface of +1.93 e.

  3. Field emission techniques for studying surface reactions: applying them to NO-H2 interaction with Pd tips.

    Science.gov (United States)

    Visart de Bocarmé, T; Kruse, Norbert

    2011-05-01

    The adsorption of NO and its reaction with H(2) over Pd tips were investigated by means of field ion microscopy (FIM) and pulsed field desorption mass spectrometry (PFDMS) in the 10(-3)Pa pressure range and at sample temperatures between 400 and 600K. By varying the H(2) partial pressure while keeping the other control parameters constant, the NO+H(2) reaction over Pd crystallites is shown to exhibit a strong hysteresis effect. The hysteresis region narrows with increase in temperature and the H(2) pressures delimiting this hysteresis decrease as well. Abrupt transformations of the micrographs are observed by FIM from bright to dark patterns and vice versa. These transformations define the hysteresis region. The collected data allow establishing a novel kinetic phase diagram of the NO+H(2)/Pd system within the range of temperatures and pressures indicated. The observed features are correlated with a local chemical analysis by means of field pulses. NO(+) seems to be the dominating imaging species under all conditions. At high relative H(2) pressures (the "hydrogen-side"), H atoms seem to diffuse subsurface. This process is blocked at lower H(2) pressure (the "NO-side") due to NO(ad) and O(ad) accumulation on the surface. Probe-hole measurements with field pulses indicate that the Pd surface undergoes oxidation as revealed by the occurrence of PdO(2)(+) species in the mass spectra. Copyright © 2010 Elsevier B.V. All rights reserved.

  4. Photoionization microscopy of hydrogen atom near a metal surface

    International Nuclear Information System (INIS)

    Yang Hai-Feng; Wang Lei; Liu Xiao-Jun; Liu Hong-Ping

    2011-01-01

    We have studied the ionization of Rydberg hydrogen atom near a metal surface with a semiclassical analysis of photoionization microscopy. Interference patterns of the electron radial distribution are calculated at different scaled energies above the classical saddle point and at various atom—surface distances. We find that different types of trajectories contribute predominantly to different manifolds in a certain interference pattern. As the scaled energy increases, the structure of the interference pattern evolves smoothly and more types of trajectories emerge. As the atom approaches the metal surface closer, there are more types of trajectories contributing to the interference pattern as well. When the Rydberg atom comes very close to the metal surface or the scaled energy approaches the zero field ionization energy, the potential induced by the metal surface will make atomic system chaotic. The results also show that atoms near a metal surface exhibit similar properties like the atoms in the parallel electric and magnetic fields. (atomic and molecular physics)

  5. Ethanol decomposition on a Pd(110) surface: a density functional theory investigation.

    Science.gov (United States)

    Guo, Wenyue; Li, Ming; Lu, Xiaoqing; Zhu, Houyu; Li, Yang; Li, Shaoren; Zhao, Lianming

    2013-02-14

    Ethanol decomposition on Pd(110) is comprehensively investigated using self-consistent periodic density functional theory. Geometries and energies for all the intermediates involved are analyzed, and the decomposition network is mapped out to illustrate the reaction mechanism. On Pd(110), the most stable adsorption of the involved species tends to follow the gas-phase bond order rules, wherein C is tetravalent and O is divalent with the missing H atoms replaced by metal atoms. The most likely decomposition pathway of ethanol on Pd(110) is CH(3)CH(2)OH → CH(3)CH(2)O → CH(3)CHO → CH(3)CO → CH(3) + CO → CO + H + CH(4) + C, in which the initial dehydrogenation is the rate-limited step. No C-O scission pathway is identified. Comparing with ethanol decomposition on Pd(111) [Langmuir, 2010, 26, 1879-1888], Pd(110) characterizes relatively high activity and different selectivity. Two crucial factors controlling the variations of reactivity and selectivity from Pd(111) to Pd(110), i.e., the local electronic effect of the metals and the geometrical effect of the relevant transition states, are identified. Four distinct Brønsted-Evans-Polanyi (BEP) relations are identified for the three types of bond scission (C-H, C-O, and C-C) if we consider Pd(111) and Pd(110) as a whole, one for C-H bond scission, one for C-O bond scission, and two for C-C bond scission.

  6. Changes in red blood cell membrane structure in G6PD deficiency: an atomic force microscopy study.

    Science.gov (United States)

    Tang, Jia; Jiang, Chengrui; Xiao, Xiao; Fang, Zishui; Li, Lei; Han, Luhao; Mei, Anqi; Feng, Yi; Guo, Yibin; Li, Hongyi; Jiang, Weiying

    2015-04-15

    Glucose-6-phosphate dehydrogenase deficiency affects over 400 million people worldwide. The hemolytic anemia in G6PD deficiency is usually triggered by oxidative stress, but the mechanism remains uncertain. We have used atomic force microscopy for studying changes in red blood cell membrane and providing new insights on the mechanism. G6PD activity assay and molecular genetic tests were used for molecular diagnosis. AFM was used to investigate alterations in the ultrastructure of G6PD deficient RBC membranes, the influence of different primaquine concentrations, and the protective effects of vitamin C. Nine variants were identified from 33 G6PD deficient individuals. AFM imaging and quantitative analysis showed that G6PD deficient erythrocytes became heterogeneous and roughness measurements of erythrocyte membranes are increased. G6PD enzyme activity and different mutations may relate with roughness parameters. Furthermore, primaquine induces an increased roughness and height of erythrocyte membrane. Meanwhile, primaquine induces damages to erythrocytes which could be prevented by vitamin C treatment in normal RBCs but not in G6PD deficient erythrocytes. Our research may give valuable information about the status of G6PD deficient patients and explore the mechanism of hemolytic anemia. Copyright © 2015 Elsevier B.V. All rights reserved.

  7. The magnetic properties of Ce/Pd surface alloys investigated using DFT

    KAUST Repository

    Shuttleworth, I.G.

    2014-06-01

    The surface alloys that form between Ce and Pd(1 1 1), Pd(1 0 0) and both unreconstructed and missing-row type Pd(1 1 0) at low Ce coverage ( θCe=19ML) have shown permanent magnetism that is mediated in part by an RKKY-like delocalized Ce 6s-Pd 5s interaction. The Pd 4d states are significantly affected by alloying and their behavior cannot be explained by a purely spin-dependent Hamiltonian. Experimental observations of changes to the Pd 4d states are explained and the implications of Ce/Pd magnetism in reforming catalysis are discussed. © 2014 Elsevier B.V. All rights reserved.

  8. Facile preparation of dendritic Ag-Pd bimetallic nanostructures on the surface of Cu foil for application as a SERS-substrate

    Science.gov (United States)

    Yi, Zao; Tan, Xiulan; Niu, Gao; Xu, Xibin; Li, Xibo; Ye, Xin; Luo, Jiangshan; Luo, Binchi; Wu, Weidong; Tang, Yongjian; Yi, Yougen

    2012-05-01

    Dendritic Ag-Pd bimetallic nanostructures have been synthesized on the surface of Cu foil via a multi-stage galvanic replacement reaction (MGRR) of Ag dendrites in a Na2PdCl4 solution. After five stages of replacement reaction, one obtained structures with protruding Ag-Pd flakes; these will mature into many porous structures with a few Ag atoms that are left over dendrites. The dendritic Ag-Pd bimetallic nanostructures were characterized by transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HRTEM), field emission scanning electron microscopy (FESEM), energy-dispersive X-ray (EDX), selected area electron diffraction (SAED) and X-ray photoelectron spectroscopy (XPS). The morphology of the products strongly depended on the stage of galvanic replacement reaction and reaction temperature. The morphology and composition-dependent surface-enhanced Raman scattering (SERS) of the as-synthesized Ag-Pd bimetallic nanostructures were investigated. The effectiveness of these dendritic Ag-Pd bimetallic nanostructures on the surface of Cu foil as substrates toward SERS detection was evaluated by using rhodamine 6G (R6G) as a probe molecule. The results indicate that as-synthesized dendritic Ag-Pd bimetallic nanostructures are good candidates for SERS spectroscopy.

  9. Peptide-Directed PdAu Nanoscale Surface Segregation: Toward Controlled Bimetallic Architecture for Catalytic Materials.

    Science.gov (United States)

    Bedford, Nicholas M; Showalter, Allison R; Woehl, Taylor J; Hughes, Zak E; Lee, Sungsik; Reinhart, Benjamin; Ertem, S Piril; Coughlin, E Bryan; Ren, Yang; Walsh, Tiffany R; Bunker, Bruce A

    2016-09-27

    Bimetallic nanoparticles are of immense scientific and technological interest given the synergistic properties observed when two different metallic species are mixed at the nanoscale. This is particularly prevalent in catalysis, where bimetallic nanoparticles often exhibit improved catalytic activity and durability over their monometallic counterparts. Yet despite intense research efforts, little is understood regarding how to optimize bimetallic surface composition and structure synthetically using rational design principles. Recently, it has been demonstrated that peptide-enabled routes for nanoparticle synthesis result in materials with sequence-dependent catalytic properties, providing an opportunity for rational design through sequence manipulation. In this study, bimetallic PdAu nanoparticles are synthesized with a small set of peptides containing known Pd and Au binding motifs. The resulting nanoparticles were extensively characterized using high-resolution scanning transmission electron microscopy, X-ray absorption spectroscopy, and high-energy X-ray diffraction coupled to atomic pair distribution function analysis. Structural information obtained from synchrotron radiation methods was then used to generate model nanoparticle configurations using reverse Monte Carlo simulations, which illustrate sequence dependence in both surface structure and surface composition. Replica exchange with solute tempering molecular dynamics simulations were also used to predict the modes of peptide binding on monometallic surfaces, indicating that different sequences bind to the metal interfaces via different mechanisms. As a testbed reaction, electrocatalytic methanol oxidation experiments were performed, wherein differences in catalytic activity are clearly observed in materials with identical bimetallic composition. Taken together, this study indicates that peptides could be used to arrive at bimetallic surfaces with enhanced catalytic properties, which could be leveraged

  10. Simulations of atomic trajectories near a dielectric surface

    Energy Technology Data Exchange (ETDEWEB)

    Stern, N P; Alton, D J; Kimble, H J, E-mail: hjkimble@caltech.edu [Norman Bridge Laboratory of Physics 12-33, California Institute of Technology, Pasadena, CA 91125 (United States)

    2011-08-15

    We present a semiclassical model of an atom moving in the evanescent field of a microtoroidal resonator. Atoms falling through whispering-gallery modes can achieve strong, coherent coupling with the cavity at distances of approximately 100 nm from the surface; in this regime, surface-induced Casmir-Polder level shifts become significant for atomic motion and detection. Atomic transit events detected in recent experiments are analyzed with our simulation, which is extended to consider atom trapping in the evanescent field of a microtoroid.

  11. Hydrogen storage and stability properties of Pd-Pt solid-solution nanoparticles revealed via atomic and electronic structure.

    Science.gov (United States)

    Kumara, Loku Singgappulige Rosantha; Sakata, Osami; Kobayashi, Hirokazu; Song, Chulho; Kohara, Shinji; Ina, Toshiaki; Yoshimoto, Toshiki; Yoshioka, Satoru; Matsumura, Syo; Kitagawa, Hiroshi

    2017-11-06

    Bimetallic Pd 1-x Pt x solid-solution nanoparticles (NPs) display charging/discharging of hydrogen gas, which has relevance for fuel cell technologies; however, the constituent elements are immiscible in the bulk phase. We examined these material systems using high-energy synchrotron X-ray diffraction, X-ray absorption fine structure and hard X-ray photoelectron spectroscopy techniques. Recent studies have demonstrated the hydrogen storage properties and catalytic activities of Pd-Pt alloys; however, comprehensive details of their structural and electronic functionality at the atomic scale have yet to be reported. Three-dimensional atomic-scale structure results obtained from the pair distribution function (PDF) and reverse Monte Carlo (RMC) methods suggest the formation of a highly disordered structure with a high cavity-volume-fraction for low-Pt content NPs. The NP conduction band features, as extracted from X-ray absorption near-edge spectra at the Pd and Pt L III -edge, suggest that the Pd conduction band is filled by Pt valence electrons. This behaviour is consistent with observations of the hydrogen storage capacity of these NPs. The broadening of the valence band width and the down-shift of the d-band centre away from the Fermi level upon Pt substitution also provided evidence for enhanced stability of the hydride (ΔH) features of the Pd 1-x Pt x solid-solution NPs with a Pt content of 8-21 atomic percent.

  12. Soft-landing deposition of radioactive probe atoms on surfaces

    NARCIS (Netherlands)

    Laurens, C.R; Rosu, M.F; Pleiter, F; Niesen, L

    1999-01-01

    We present a method to deposit a wide range of radioactive probe atoms on surfaces, without introducing lattice damage or contaminating the surface with other elements or isotopes. In this method, the probe atoms are mass-separated using an isotope separa-tor, decelerated to 5 eV, and directly

  13. The effect of alloying on shake-up satellites: The case of Pd in SbPd{sub 2} and InPd{sub 2} surface alloys

    Energy Technology Data Exchange (ETDEWEB)

    Pancotti, A. [Instituto de Fisica ' Gleb Wataghin-Universidade Estadual de Campinas, Caixa Postal 6165, 13083-970 Campinas, SP (Brazil)], E-mail: pancotti@ifi.unicamp.br; Siervo, A. de [Laboratorio Nacional de Luz Sincrotron, Caixa Postal 6192, 13084-971 Campinas, SP (Brazil); Carazzolle, M.F. [Instituto de Fisica ' Gleb Wataghin-Universidade Estadual de Campinas, Caixa Postal 6165, 13083-970 Campinas, SP (Brazil); Landers, R. [Instituto de Fisica ' Gleb Wataghin-Universidade Estadual de Campinas, Caixa Postal 6165, 13083-970 Campinas, SP (Brazil); Laboratorio Nacional de Luz Sincrotron, Caixa Postal 6192, 13084-971 Campinas, SP (Brazil); Kleiman, G.G. [Instituto de Fisica ' Gleb Wataghin-Universidade Estadual de Campinas, Caixa Postal 6165, 13083-970 Campinas, SP (Brazil)

    2007-05-15

    A well-known final state effect in photoemission is that of the 'shake-up' satellite in core level and valence band spectra from Pd in the bulk metals. The satellite is explained in terms of the existence of two Pd final state configurations, 4d{sup 9}5s{sup 1} and 4d{sup 10}5s{sup 2}. The present paper is a preliminary report of studies of the suppression of the shake-up satellite in surface alloys of Pd with the 'sp metals', In and Sb, on Pd(1 1 1), whose surface structure was determined as being ({radical}3 x {radical}3)R30 deg. from LEED and X-ray photoelectron diffraction (XPD). Although satellite suppression has been reported for bulk alloys, no such report has been made for a metallic surface alloy system. From the satellite suppression and the related spectra asymmetry reduction, as well as the small binding energy shifts, we are able to interpret the results in terms of valence band splitting.

  14. A DFT study and micro-kinetic analysis of acetylene selective hydrogenation on Pd-doped Cu(111) surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Ma, Ling-Ling [Department of Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Nankai University, Tianjin 300071 (China); Lv, Cun-Qin, E-mail: lcq173@126.com [College of Chemistry and Environmental Engineering, Shanxi Datong University, Datong 037009, Shanxi Province (China); Wang, Gui-Chang, E-mail: wangguichang@nankai.edu.cn [Department of Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Nankai University, Tianjin 300071 (China)

    2017-07-15

    Semi-hydrogenation of acetylene in a hydrogen-rich stream is an industrially important process. Inspired by the recent experiments that Cu(111) surface doped by a small number of Pd atoms can exhibit excellent catalytic performance toward the dissociation of H{sub 2} molecule as well as the high selective hydrogenation of acetylene as compared with pure Cu and Pd metal alone at low-temperature, here we performed systematic first-principles calculations to investigate the corresponding reaction mechanism related to the acetylene hydrogenation processes on single atom alloys (SAAs) and monolayer Pd/Cu(111) (i.e.,1.00 ML Pd/Cu(111)) model catalysts in detail, and to explore the possible factors controlling the high selectivity on SAAs. Our results clearly demonstrate that the SAA catalyst has higher selectivity for the ethylene formation than that of 1.00 ML Pd/Cu(111), and lower activity for the acetylene conversion compared with that of 1.00 ML Pd/Cu(111). The relatively high selectivity on SAA is mainly due to the facile desorption of ethylene and moderate activity in the dissociation of molecular H{sub 2}. The main factor which lowers the selectivity towards the ethylene formation on 1.00 ML Pd/Cu(111) is that this system has a higher capacity to promote the breaking of C−H/C−C bonds, which leads to the formation of carbonaceous deposits and polymers such as benzene, and thus reduces the selectivity for the ethylene formation. Meanwhile, it was found that the desorption energy of ethylene on these two surfaces was smaller than the energy barrier of further hydrogenation, which results in the absence of ethane on these two systems. Micro-kinetic model analysis provides a further valuable insight into the evidence for the key factors controlling the catalytic activity and selectivity towards the selective hydrogenation of acetylene. Our findings may help people to design a highly selective hydrogenation catalyst by controlling the balance between the H{sub 2

  15. A DFT study and micro-kinetic analysis of acetylene selective hydrogenation on Pd-doped Cu(111) surfaces

    Science.gov (United States)

    Ma, Ling-Ling; Lv, Cun-Qin; Wang, Gui-Chang

    2017-07-01

    Semi-hydrogenation of acetylene in a hydrogen-rich stream is an industrially important process. Inspired by the recent experiments that Cu(111) surface doped by a small number of Pd atoms can exhibit excellent catalytic performance toward the dissociation of H2 molecule as well as the high selective hydrogenation of acetylene as compared with pure Cu and Pd metal alone at low-temperature, here we performed systematic first-principles calculations to investigate the corresponding reaction mechanism related to the acetylene hydrogenation processes on single atom alloys (SAAs) and monolayer Pd/Cu(111) (i.e.,1.00 ML Pd/Cu(111)) model catalysts in detail, and to explore the possible factors controlling the high selectivity on SAAs. Our results clearly demonstrate that the SAA catalyst has higher selectivity for the ethylene formation than that of 1.00 ML Pd/Cu(111), and lower activity for the acetylene conversion compared with that of 1.00 ML Pd/Cu(111). The relatively high selectivity on SAA is mainly due to the facile desorption of ethylene and moderate activity in the dissociation of molecular H2. The main factor which lowers the selectivity towards the ethylene formation on 1.00 ML Pd/Cu(111) is that this system has a higher capacity to promote the breaking of Csbnd H/Csbnd C bonds, which leads to the formation of carbonaceous deposits and polymers such as benzene, and thus reduces the selectivity for the ethylene formation. Meanwhile, it was found that the desorption energy of ethylene on these two surfaces was smaller than the energy barrier of further hydrogenation, which results in the absence of ethane on these two systems. Micro-kinetic model analysis provides a further valuable insight into the evidence for the key factors controlling the catalytic activity and selectivity towards the selective hydrogenation of acetylene. Our findings may help people to design a highly selective hydrogenation catalyst by controlling the balance between the H2 dissociation and

  16. Au@Pd Bimetallic Nanocatalyst for Carbon-Halogen Bond Cleavage: An Old Story with New Insight into How the Activity of Pd is Influenced by Au.

    Science.gov (United States)

    Liu, Rui; Chen, Hui-Min; Fang, Li-Ping; Xu, Cuihong; He, Zuoliang; Lai, Yujian; Zhao, Huachao; Bekana, Deribachew; Liu, Jing-Fu

    2018-03-21

    AuPd bimetallic nanocatalysts exhibit superior catalytic performance in the cleavage of carbon-halogen bonds (C-X) in the hazardous halogenated pollutants. A better understanding of how Au atoms promote the reactivity of Pd sites rather than vaguely interpreting as bimetallic effect and determining which type of Pd sites are necessary for these reactions are crucial factors for the design of atomically precise nanocatalysts that make full use of both the Pd and Au atoms. Herein, we systematically manipulated the coordination number of Pd-Pd, d-orbital occupation state, and the Au-Pd interface of the Pd reactive centers and studied the structure-activity relationship of Au-Pd in the catalyzed cleavage of C-X bonds. It is revealed that Au enhanced the activity of Pd atoms primarily by increasing the occupation state of Pd d-orbitals. Meanwhile, among the Pd sites formed on the Au surface, five to seven contiguous Pd atoms, three or four adjacent Pd atoms, and isolated Pd atoms were found to be the most active in the cleavage of C-Cl, C-Br, and C-I bonds, respectively. Besides, neighboring Au atoms directly contribute to the weakening of the C-Br/C-I bond. This work provides new insight into the rational design of bimetallic metal catalysts with specific catalytic properties.

  17. Use of surface area computations to describe atom-atom interactions.

    Science.gov (United States)

    de La Cruz, X; Calvo, M

    2001-06-01

    Accessible surface (ASA) and atomic contact (ACA) areas are powerful tools for protein structure analysis. However, their use for analysis purposes could be extended if a relationship between them and protein stability could be found. At present, this is the case only for ASAs, which have been used to assess the contribution of the hydrophobic effect to protein stability. In the present work we study whether there is a relationship between atomic contact areas and the free energy associated to atom-atom interactions. We utilise a model in which the contribution of atomic interactions to protein stability is expressed as a linear function of the accessible surface area buried between atom pairs. We assess the validity of this hypothesis, using a set of 124 lysozyme mutants (Matthews, 1995, Adv Protein Chem, 249-278) for which both the X-ray structure and the experimental stability are known. We tested this assumption for residue representations with increasing numbers of atom types. Our results indicate that for simple residue representations, with only 4 to 5 atom types, there is not a clear linear relationship between stability and buried accessible area. However, this relationship is observed for representations with 6 to 9 atom types, where gross heterogeneities in the atom type definition are eliminated. Finally, we also study a version of the linear model in which the atom- atom interactions are represented utilising a simple function for the buried accessible area, which may be useful for protein structure prediction studies.

  18. Electronegativity determination of individual surface atoms by atomic force microscopy

    Czech Academy of Sciences Publication Activity Database

    Onoda, J.; Ondráček, Martin; Jelínek, Pavel; Sugimoto, Y.

    2017-01-01

    Roč. 8, Apr (2017), 1-6, č. článku 15155. ISSN 2041-1723 R&D Projects: GA ČR(CZ) GC14-16963J Institutional support: RVO:68378271 Keywords : AFM * DFT * electronegativity * surface science Subject RIV: BM - Solid Matter Physics ; Magnetism OBOR OECD: Condensed matter physics (including formerly solid state physics, supercond.) Impact factor: 12.124, year: 2016

  19. Atomization of Impinging Droplets on Superheated Superhydrophobic Surfaces

    Science.gov (United States)

    Emerson, Preston; Crockett, Julie; Maynes, Daniel

    2017-11-01

    Water droplets impinging smooth superheated surfaces may be characterized by dynamic vapor bubbles rising to the surface, popping, and causing a spray of tiny droplets to erupt from the droplet. This spray is called secondary atomization. Here, atomization is quantified experimentally for water droplets impinging superheated superhydrophobic surfaces. Smooth hydrophobic and superhydrophobic surfaces with varying rib and post microstructuring were explored. Each surface was placed on an aluminum heating block, and impingement events were captured with a high speed camera at 3000 fps. For consistency among tests, all events were normalized by the maximum atomization found over a range of temperatures on a smooth hydrophobic surface. An estimate of the level of atomization during an impingement event was created by quantifying the volume of fluid present in the atomization spray. Droplet diameter and Weber number were held constant, and atomization was found for a range of temperatures through the lifetime of the impinging droplet. The Leidenfrost temperature was also determined and defined to be the lowest temperature at which atomization ceases to occur. Both atomization and Leidenfrost temperature increase with decreasing pitch (distance between microstructures).

  20. Multiple atomic scale solid surface interconnects for atom circuits and molecule logic gates

    International Nuclear Information System (INIS)

    Joachim, C; Martrou, D; Gauthier, S; Rezeq, M; Troadec, C; Jie Deng; Chandrasekhar, N

    2010-01-01

    The scientific and technical challenges involved in building the planar electrical connection of an atomic scale circuit to N electrodes (N > 2) are discussed. The practical, laboratory scale approach explored today to assemble a multi-access atomic scale precision interconnection machine is presented. Depending on the surface electronic properties of the targeted substrates, two types of machines are considered: on moderate surface band gap materials, scanning tunneling microscopy can be combined with scanning electron microscopy to provide an efficient navigation system, while on wide surface band gap materials, atomic force microscopy can be used in conjunction with optical microscopy. The size of the planar part of the circuit should be minimized on moderate band gap surfaces to avoid current leakage, while this requirement does not apply to wide band gap surfaces. These constraints impose different methods of connection, which are thoroughly discussed, in particular regarding the recent progress in single atom and molecule manipulations on a surface.

  1. Stable structures and potential energy surface of the metallic clusters: Ni, Cu, Ag, Au, Pd, and Pt

    Science.gov (United States)

    Wu, Xia; Sun, Yan

    2017-06-01

    Metallic clusters have been widely studied due to their special electrical, optical, and catalytic properties. The many-body Gupta potential is applied to describe the interatomic interaction of Ni, Cu, Ag, Au, Pd, and Pt clusters, and their global minimal structures within 100 atoms are optimized using dynamic lattice searching (DLS) method. The configurational distribution of global minima is analyzed, and the geometrical difference among these clusters is demonstrated. Results show that the dominant motif of Ni and Cu clusters is the icosahedron, and in Ag and Au clusters the number of decahedra is slightly larger than that of the icosahedra. However, more face-centered cubic (fcc), stacking fault fcc, and amorphous structures are formed in Au clusters than in Ag clusters. Furthermore, the main motif of Pd and Pt clusters is the decahedron. In particular, Ni98 adopts a Leary tetrahedral motif, and Pt54 is a central vacant icosahedron. The difference related to the potential parameters of these metallic clusters is further investigated by energy analysis. Moreover, the potential energy surfaces (PES) of 38-atom metallic clusters is characterized in terms of conformational analysis. It was found that the sequence of the number of local minima on the PES from large to low is Ni, Cu, Ag, Pt, Pd, and Au.

  2. Electric field sensing near the surface microstructure of an atom chip using cold Rydberg atoms

    Science.gov (United States)

    Martin, J. D. D.

    2013-05-01

    Rydberg atoms may enable hybrid systems that combine the benefits of gas-phase atoms with those of solid-state devices. However, these hybrid systems will require atoms to be located near a heterogeneous surface with exposed metal electrodes and dielectric insulators, which are sources of uncontrollable and unwanted electric fields. With this motivation, we have measured the electric fields near the heterogeneous metal-dielectric surface of an atom chip using cold Rydberg atoms. We have also developed a technique for reducing the influence of dc and low-frequency electric fields on Rydberg atom transitions, while retaining their sensitivity to high-frequency resonant fields. Work performed in collaboration with J. D. Carter, L. A. Jones, and O. Cherry and supported by NSERC.

  3. First-principles theory of the temperature and compositional dependence of atomic short-range order in disordered Cu-Pd alloys

    Science.gov (United States)

    Chepulskii, R. V.; Staunton, J. B.; Bruno, Ezio; Ginatempo, B.; Johnson, D. D.

    2002-02-01

    We combine the first-principles, Korringa-Kohn-Rostoker coherent potential approximation based calculations of compositional fluctuations with a statistical mechanical ring approximation to study the temperature (T) and composition (c) dependence of the atomic short-range order (SRO) in disordered, face-centred cubic, Cu-Pd alloys. The fourfold splitting of SRO peaks around the equivalent X(0,1,0) points in reciprocal space is obtained in a wide T-c region. Such splitting is shown to be an ``energy'' effect caused by the absolute minima of the Fourier transform of the effective atomic interactions and related previously to the existence of nested sheets of the disordered alloy's Fermi surface. However, we find that the T dependence of the SRO peak position is mostly an ``entropy'' effect. Both the calculated T and c dependences of the SRO peaks position are in good correspondence with the experimental data. The real-space effective atomic interactions and SRO parameters indicate the tendency for longer-period structures with increasing Pd concentration, as observed.

  4. Perpendicular magnetic anisotropy of ultrathin FeCo alloy films on Pd(0 0 1) surface: First principles study

    International Nuclear Information System (INIS)

    Kim, Dongyoo; Hong, Jisang

    2009-01-01

    Using the full potential linearized augmented plane wave (FLAPW) method, thickness dependent magnetic anisotropy of ultrathin FeCo alloy films in the range of 1 monolayer (ML) to 5 ML coverage on Pd(0 0 1) surface has been explored. We have found that the FeCo alloy films have close to half metallic state and well-known surface enhancement in thin film magnetism is observed in Fe atom, whereas the Co has rather stable magnetic moment. However, the largest magnetic moment in Fe and Co is found at 1 ML thickness. Interestingly, it has been observed that the interface magnetic moments of Fe and Co are almost the same as those of surface elements. The similar trend exists in orbital magnetic moment. This indicates that the strong hybridization between interface FeCo alloy and Pd gives rise to the large magnetic moment. Theoretically calculated magnetic anisotropy shows that the 1 ML FeCo alloy has in-plane magnetization, but the spin reorientation transition (SRT) from in-plane to perpendicular magnetization is observed above 2 ML thickness with huge magnetic anisotropy energy. The maximum magnetic anisotropy energy for perpendicular magnetization is as large as 0.3 meV/atom at 3 ML film thickness with saturation magnetization of 2.36μ B . Besides, the calculated X-ray magnetic circular dichroism (XMCD) has been presented.

  5. Single atom self-diffusion on nickel surfaces

    International Nuclear Information System (INIS)

    Tung, R.T.; Graham, W.R.

    1980-01-01

    Results of a field ion microscope study of single atom self-diffusion on Ni(311), (331), (110), (111) and (100) planes are presented, including detailed information on the self-diffusion parameters on (311), (331), and (110) surfaces, and activation energies for diffusion on the (111), and (100) surfaces. Evidence is presented for the existence of two types of adsorption site and surface site geometry for single nickel atoms on the (111) surface. The presence of adsorbed hydrogen on the (110), (311), and (331) surfaces is shown to lower the onset temperature for self-diffusion on these planes. (orig.)

  6. Atomic forces between noble gas atoms, alkali ions, and halogen ions for surface interactions

    Science.gov (United States)

    Wilson, J. W.; Outlaw, R. A.; Heinbockel, J. H.

    1988-01-01

    The components of the physical forces between noble gas atoms, alkali ions, and halogen ions are analyzed and a data base developed from analysis of the two-body potential data, the alkali-halide molecular data, and the noble gas crystal and salt crystal data. A satisfactory global fit to this molecular and crystal data is then reproduced by the model to within several percent. Surface potentials are evaluated for noble gas atoms on noble gas surfaces and salt crystal surfaces with surface tension neglected. Within this context, the noble gas surface potentials on noble gas and salt crystals are considered to be accurate to within several percent.

  7. Synthesis and crystal structure of a new Cu3Au-type ternary phase in the Au-In-Pd system: distribution of atoms over crystallographic positions.

    Science.gov (United States)

    Ptashkina, Evgeniya A; Kabanova, Elizaveta G; Tursina, Anna I; Yatsenko, Alexandr V; Kuznetsov, Victor N

    2018-03-01

    A new Cu 3 Au-type ternary phase (τ phase) is found in the AuPd-rich part of the Au-In-Pd system. It has a broad homogeneity range based on extensive (Pd,Au) and (In,Au) replacement, with the composition varying between Au 17.7 In 25.3 Pd 57.0 and Au 50.8 In 16.2 Pd 33.0 . The occupancies of the crystallographic positions were studied by single-crystal X-ray diffraction for three samples of different composition. The sites with m-3m symmetry are occupied by atoms with a smaller scattering power than the atoms located on 4/mmm sites. Two extreme structure models were refined. Within the first, the occupation type changes from (Au,In,Pd) 3 (Pd,In) to (Au,Pd) 3 (In,Pd,Au) with an increase in the Au gross content. For the second model, the occupation type (Au,In,Pd) 3 (Pd,Au) remains essentially unchanged for all Au concentrations. Although the diffraction data do not allow the choice of one of these models, the latter model, where Au substitutes In on 4/mmm sites, seems to be preferable, since it agrees with the fact that the homogeneity range of the τ phase is inclined to the Au corner and provides the same occupation type for all the studied samples of different compositions.

  8. Modeling noncontact atomic force microscopy resolution on corrugated surfaces

    Directory of Open Access Journals (Sweden)

    Kristen M. Burson

    2012-03-01

    Full Text Available Key developments in NC-AFM have generally involved atomically flat crystalline surfaces. However, many surfaces of technological interest are not atomically flat. We discuss the experimental difficulties in obtaining high-resolution images of rough surfaces, with amorphous SiO2 as a specific case. We develop a quasi-1-D minimal model for noncontact atomic force microscopy, based on van der Waals interactions between a spherical tip and the surface, explicitly accounting for the corrugated substrate (modeled as a sinusoid. The model results show an attenuation of the topographic contours by ~30% for tip distances within 5 Å of the surface. Results also indicate a deviation from the Hamaker force law for a sphere interacting with a flat surface.

  9. SASP - Symposium on atomic, cluster and surface physics '94

    International Nuclear Information System (INIS)

    Maerk, T.D.; Schrittwieser, R.; Smith, D.

    1994-01-01

    This international symposium (Founding Chairman: W. Lindinger, Innsbruck) is one in a continuing biennial series of conferences which seeks to promote the growth of scientific knowledge and its effective exchange among scientists in the field of atomic, molecular, cluster and surface physics and related areas. The symposium deals in particular with interactions between ions, electrons, photons, atoms, molecules, and clusters and their interactions with surfaces. (author)

  10. Scanning tuneeling microscopy studies of fivefold surfaces of icosahedral Al-Pd-Mn quasicrystals and of thin silver films on those surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Unal, Baris [Iowa State Univ., Ames, IA (United States)

    2008-01-01

    their top planes. Hence, we name them as Pd+(with Pd) and Pd-(without Pd). Based on their planer structure and the step height, it can be said that these two families can be viable surface terminations. However, besides the Pd content, these two sets differ in terms of relative densities of their top planes as well as the gap separating the layer from the nearest atomic plane. The experimental data and other arguments lead to the conclusion that the Pd- family is favored over the Pd+. This has an important implication on the interpretation of local motifs seen in the high resolution STM images. In other words, the dark stars are not formed by cut-Bergmans rather they are formed by cut-Mackays.

  11. First principles investigation of the activity of thin film Pt, Pd and Au surface alloys for oxygen reduction

    DEFF Research Database (Denmark)

    Tripkovic, Vladimir; Hansen, Heine Anton; Rossmeisl, Jan

    2015-01-01

    active binary thin films are near-surface alloys of Pt with subsurface Pd and certain PdAu and PtAu thin films with surface and/or subsurface Au. The most active ternary thin films are with pure metal Pt or Pd skins with some degree of Au in the surface and/or subsurface layer and the near-surface alloys...... driving force for surface segregation, diffusion to defects or surface self-assembling. On the basis of stability and activity analysis we conclude that the near surface alloy of Pd in Pt and some PdAu binary and PtPdAu ternary thin films with a controlled amount of Au are the best catalysts for oxygen...

  12. Photodesorption of Na atoms from rough Na surfaces

    DEFF Research Database (Denmark)

    Balzer, Frank; Gerlach, R.; Manson, J.R.

    1997-01-01

    We investigate the desorption of Na atoms from large Na clusters deposited on dielectric surfaces. High-resolution translational energy distributions of the desorbing atoms are determined by three independent methods, two-photon laser-induced fluorescence, as well as single-photon and resonance......-enhanced two-photon ionization techniques. Upon variation of surface temperature and for different substrates (mica vs lithium fluoride) clear non-Maxwellian time-of-flight distributions are observed with a cos θ angular dependence and most probable kinetic energies below that expected of atoms desorbing from...... atoms are scattered by surface vibrations. Recent experiments providing time constants for the decay of the optical excitations in the clusters support this model. The excellent agreement between experiment and theory indicates the importance of both absorption of the laser photons via direct excitation...

  13. Photodesorption of Na atoms from rough Na surfaces

    DEFF Research Database (Denmark)

    Balzer, Frank; Gerlach, R.; Manson, J.R.

    1997-01-01

    atoms are scattered by surface vibrations. Recent experiments providing time constants for the decay of the optical excitations in the clusters support this model. The excellent agreement between experiment and theory indicates the importance of both absorption of the laser photons via direct excitation......We investigate the desorption of Na atoms from large Na clusters deposited on dielectric surfaces. High-resolution translational energy distributions of the desorbing atoms are determined by three independent methods, two-photon laser-induced fluorescence, as well as single-photon and resonance......-enhanced two-photon ionization techniques. Upon variation of surface temperature and for different substrates (mica vs lithium fluoride) clear non-Maxwellian time-of-flight distributions are observed with a cos θ angular dependence and most probable kinetic energies below that expected of atoms desorbing from...

  14. Origin and shape evolution of core-shell nanoparticles in Au-Pd: from few atoms to high Miller index facets

    Energy Technology Data Exchange (ETDEWEB)

    Bhattarai, Nabraj; Casillas, Gilberto; Khanal, Subarna; Velazquez Salazar, J. Jesus; Ponce, Arturo; Jose-Yacaman, Miguel, E-mail: miguel.yacaman@utsa.edu [University of Texas at San Antonio, Department of Physics and Astronomy (United States)

    2013-06-15

    Au-Pd core-shell nanocubes and triangular nanoparticles were systematically synthesized from a few Pd layers up to fully grown morphologies by a modified seed-mediated growth method. The shape evolution of Au-Pd core-shell nanoparticles from single crystal and singly twinned seed to final concave nanocube and triangular plates are presented at atomic level by Cs-corrected scanning transmission electron microscopy (STEM). The growth mechanism of both morphologies was studied throughout different sizes. It was found that the concave nanocubes grew from octahedral Au seeds due to fast growth along Left-Pointing-Angle-Bracket 111 Right-Pointing-Angle-Bracket directions; while the triangular nanoparticles grew from singly twinned Au seeds, growing twice as fast in Left-Pointing-Angle-Bracket 110 Right-Pointing-Angle-Bracket directions along the twin boundary; compared to the Left-Pointing-Angle-Bracket 111 Right-Pointing-Angle-Bracket direction perpendicular to the twin boundary. Both the concave nanocubes and triangular nanoparticles presented high index facet (HIF) surfaces that will increase the catalytic activity of different reactions.

  15. Low energy atomic and molecular collision with graphite surface

    International Nuclear Information System (INIS)

    Bercu, M.; Grecu, V. V.

    2002-01-01

    The interaction of atomic and molecular species of hydrogen with basal plane of graphite has been investigated by means of atomic cluster models of 10, 24 and 48 carbon atoms using Hartree-Fock - Linear Combination of Atomic Orbitals (HF-LCAO) theory at the ab-initio and semiempirical level of approximation. The last approach was based on an original package developed for carbon clusters. Atomic migration between consecutive basal planes was described by cluster models of two sheets of carbon atoms. Our contribution presents the theoretical results about atomic and molecular interactions with graphite. It was found for H atom bonding energy the value 2.6 eV, using the largest cluster model. The migration of H atoms above the surface and between consecutive basal planes was simulated by extended calculations of potential energy in each point of a mesh containing 450 points describing a local surface of 0.25 nm 2 . A 3D interpolation approach gives the image of a hypersurface potential energy projection at a given distance to the graphite surface. The semi-quantitative results have indicated two significant facts related to atomic species migration. The first is that H atom has the smallest displacement barrier along C-C bonds at a distance of 1.3 A from the basal plane. In the case of absorbed atoms between graphite basal planes an almost free motion channel has been found parallel to the surface. The interaction potential barrier for H atom collision with graphite surface at the center of the carbon ring has been calculated neglecting surface vibration modes and found to be 5.9 eV . The hyperfine interaction between the electron of hydrogen and the proton has been taken as a measure of the interaction between the incident atom and the target local states. The isotropic hyperfine constant obtained at the level of the semiempiric calculations was found to be 402 Gs at the equilibrium position of H atom above a C atom at a distance of 1.3 A. The corresponding value

  16. Surface Adsorption in Nonpolarizable Atomic Models.

    Science.gov (United States)

    Whitmer, Jonathan K; Joshi, Abhijeet A; Carlton, Rebecca J; Abbott, Nicholas L; de Pablo, Juan J

    2014-12-09

    Many ionic solutions exhibit species-dependent properties, including surface tension and the salting-out of proteins. These effects may be loosely quantified in terms of the Hofmeister series, first identified in the context of protein solubility. Here, our interest is to develop atomistic models capable of capturing Hofmeister effects rigorously. Importantly, we aim to capture this dependence in computationally cheap "hard" ionic models, which do not exhibit dynamic polarization. To do this, we have performed an investigation detailing the effects of the water model on these properties. Though incredibly important, the role of water models in simulation of ionic solutions and biological systems is essentially unexplored. We quantify this via the ion-dependent surface attraction of the halide series (Cl, Br, I) and, in so doing, determine the relative importance of various hypothesized contributions to ionic surface free energies. Importantly, we demonstrate surface adsorption can result in hard ionic models combined with a thermodynamically accurate representation of the water molecule (TIP4Q). The effect observed in simulations of iodide is commensurate with previous calculations of the surface potential of mean force in rigid molecular dynamics and polarizable density-functional models. Our calculations are direct simulation evidence of the subtle but sensitive role of water thermodynamics in atomistic simulations.

  17. Measuring Forces between Oxide Surfaces Using the Atomic Force Microscope

    DEFF Research Database (Denmark)

    Pedersen, Henrik Guldberg; Høj, Jakob Weiland

    1996-01-01

    The interactions between colloidal particles play a major role in processing of ceramics, especially in casting processes. With the Atomic Force Microscope (AFM) it is possible to measure the inter-action force between a small oxide particle (a few micron) and a surface as function of surface...

  18. Studies of isotopic defined hydrogen beams scattering from Pd single-crystal surfaces

    International Nuclear Information System (INIS)

    Varlam, Mihai; Steflea, Dumitru

    2001-01-01

    An experimental investigation of hydrogen isotopes interaction with Pd single-crystal surface has been carried out using molecular beam technique. The energy dependence of the sticking probability and its relation with the trapping probability into the precursor state is studied by integrating the scattered angular distribution of hydrogen Isotopic defined beams from Pd (111) surface in the 40-400 K surface temperature range. The dependence has been evaluated by defining hydrogen molecular beams with different isotopic concentration - from the natural one to the 5% D/(D+H) ratio - and for different incident energies. The beam was directed onto a single-crystal Pd (111) surface. In the paper, we report the experimental results and some considerations related to it. (authors)

  19. Studies of isotopic defined hydrogen beams scattering from Pd single-crystal surfaces

    International Nuclear Information System (INIS)

    Varlam, Mihai; Steflea, Dumitru

    1999-01-01

    An experimental investigation of hydrogen isotopes interaction with Pd single-crystal surfaces has been carried out using molecular beam technique. The energy dependence of the sticking probability and its relation with the trapping probability into the precursor state is studied by integrating the scattered angular distribution of hydrogen isotopic defined beams from Pd (111) surfaces in the 40 - 400 K surface temperature range. The dependence has been evaluated by defining hydrogen molecular beams with different isotopic concentration - from the natural one until 5% D/(D + H) and different incident energies and directed onto a single - crystal Pd (111) surface. In the paper, we report the experimental results and some considerations related to them. (authors)

  20. Theoretical investigation of bulk ordering and surface segregation in Ag-Pd and other isoelectornic alloys

    Science.gov (United States)

    Ruban, A. V.; Simak, S. I.; Korzhavyi, P. A.; Johansson, B.

    2007-02-01

    Bulk ordering in Ag-Pd and other isoelectronic alloys is investigated theoretically by a number of first-principles techniques. The electronic structure and total energy have been calculated by the Green’s function Korringa-Kohn-Rostocker and full-potential plane wave methods. The effective cluster interactions of the Ising-type Hamiltonian have been obtained by the screened generalized perturbation method. They reveal a complex concentration-dependent ordering behavior in these alloys due to band filling and Fermi surface effects. In particular we show that long-period superstructures are gradually stabilized by a great number of relatively weak long-range effective pair- and three-site interactions, which can be seen as “collective” effect. A similar complex concentration dependence is also found for surfaces of Ag-Pd alloys. The surface composition of the (111) and (100) surface of Ag75Pd25 , Ag50Pd50 , and Ag33Pd67 alloys have been then investigated by the surface Green’s function technique and the screened generalized perturbation method for the effective interactions of the Ising-type Hamiltonian and the grand canonical Monte Carlo method for statistical thermodynamic simulations at finite temperatures. We compare our results with experimental data and other theoretical calculations.

  1. Design of Pd-Based Bimetallic Catalysts for ORR: A DFT Calculation Study

    Directory of Open Access Journals (Sweden)

    Lihui Ou

    2015-01-01

    Full Text Available Developing Pd-lean catalysts for oxygen reduction reaction (ORR is the key for large-scale application of proton exchange membrane fuel cells (PEMFCs. In the present paper, we have proposed a multiple-descriptor strategy for designing efficient and durable ORR Pd-based alloy catalysts. We demonstrated that an ideal Pd-based bimetallic alloy catalyst for ORR should possess simultaneously negative alloy formation energy, negative surface segregation energy of Pd, and a lower oxygen binding ability than pure Pt. By performing detailed DFT calculations on the thermodynamics, surface chemistry and electronic properties of Pd-M alloys, Pd-V, Pd-Fe, Pd-Zn, Pd-Nb, and Pd-Ta, are identified theoretically to have stable Pd segregated surface and improved ORR activity. Factors affecting these properties are analyzed. The alloy formation energy of Pd with transition metals M can be mainly determined by their electron interaction. This may be the origin of the negative alloy formation energy for Pd-M alloys. The surface segregation energy of Pd is primarily determined by the surface energy and the atomic radius of M. The metals M which have smaller atomic radius and higher surface energy would tend to favor the surface segregation of Pd in corresponding Pd-M alloys.

  2. Measurement of near neighbor separations of surface atoms

    International Nuclear Information System (INIS)

    Cohen, P.I.

    Two techniques are being developed to measure the nearest neighbor distances of atoms at the surfaces of solids. Both measures extended fine structure in the excitation probability of core level electrons which are excited by an incident electron beam. This is an important problem because the structures of most surface systems are as yet unknown, even though the location of surface atoms is the basis for any quantitative understanding of the chemistry and physics of surfaces and interfaces. These methods would allow any laboratory to make in situ determinations of surface structure in conjunction with most other laboratory probes of surfaces. Each of these two techniques has different advantages; further, the combination of the two will increase confidence in the results by reducing systematic error in the data analysis

  3. Electronic state of europium atoms on surface of oxidized tungsten

    CERN Document Server

    Davydov, S Y

    2001-01-01

    The energy scheme of the europium atoms adsorption system on the tungsten surface, coated with the oxygen monolayer, is considered. The evaluations of the europium adatoms charged state on the oxidized tungsten surface are performed. It is established, that europium, adsorbed at the oxidized tungsten surface, is a positive ion with the charge close to the unit. The zonal scheme of the Eu-O/W adsorption system for the europium low and high concentrations is proposed

  4. Surface spectroscopy using inelastic scattering of He atoms

    International Nuclear Information System (INIS)

    Doak, R.B.

    1986-01-01

    A low energy (∼0 meV) neutral helium atomic beam has been scattered from crystal surfaces. Energy gain and face phonons may be measured by time-of-flight analysis of single phonon scattering dominates, allowing the frequency and wave vector of individual surface phonons to be determined and their dispersion relations plotted. Resonant interaction with bound states of the helium in the surface potential well is found to greatly affect the inelastic scattering cross-sections. 23 references, 27 figures

  5. Monitoring of Pd in airborne particulates by solid sampling high-resolution continuum source electrothermal atomic absorption spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Atilgan, Semin [Istanbul Technical University, Faculty of Science and Letters, Department of Chemistry, 34469, Maslak, Istanbul (Turkey); Akman, Suleyman, E-mail: akmans@itu.edu.tr [Istanbul Technical University, Faculty of Science and Letters, Department of Chemistry, 34469, Maslak, Istanbul (Turkey); Baysal, Asli [Istanbul Technical University, Faculty of Science and Letters, Department of Chemistry, 34469, Maslak, Istanbul (Turkey); Bakircioglu, Yasemin [Trakya University, Faculty of Science and Letters, Department of Chemistry, 22030, Edirne (Turkey); Szigeti, Tamas; Ovari, Mihaly; Zaray, Gyula [Eoetvoes Lorand University, Institute of Chemistry, Department of Analytical Chemistry, P.O. Box 32, H-1518 Budapest (Hungary)

    2012-04-15

    An analytical method has been developed for determination of palladium in PM2.5 fractions of urban airborne particulate matter by solid sampling high-resolution continuum source electrothermal atomic absorption spectrometry. For the optimization of the experimental conditions, a road dust certified reference material (BCR-723) was used. The influence of pyrolysis and atomization temperatures, the amount of sample introduced into the graphite furnace and the addition of acids, surfactants and modifiers on the analytical signal of Pd were investigated. The limit of detection, calculated based on three times the standard deviations of analytical signals obtained during the atomization of 10 blank filter pieces, was 0.07 pg/m{sup 3}. Since the amount of solid certified reference material introduced into the graphite furnace was about 50-2000 times lower than those required in order to obtain the certified value, the precision was relatively poor. This analytical method was applied for investigation of urban airborne particulate matter collected onto quartz fiber filters by high-volume aerosol samplers in the city center of Istanbul (Turkey) and Budapest (Hungary). The measured Pd concentrations changed in the range of 0.22-0.64 and 0.25-0.86 pg/m{sup 3} in Istanbul and Budapest, respectively. - Highlights: Black-Right-Pointing-Pointer Method development for palladium determination in air samples using solid sampling technique. Black-Right-Pointing-Pointer Analysis by solid sampling electrothermal atomic absorption spectrometry (HR CS ETAAS). Black-Right-Pointing-Pointer Monitoring of Pd in Istanbul and Budapest PM2.5 urban aerosols during one year. Black-Right-Pointing-Pointer Statistical analysis of results.

  6. First-principles study of the interactions of hydrogen with low-index surfaces of PdCu ordered alloy

    Directory of Open Access Journals (Sweden)

    Min Tang

    2017-12-01

    Full Text Available PdCu catalysts play a key role in several hydrogen-involved processes. Among these reactions, the interaction of hydrogen with PdCu essentially determines the catalytic performance. However, the response of PdCu to surrounding hydrogen has been poorly investigated, especially for specific facets of PdCu at different environment. In this work, taking temperature and hydrogen pressure into account, we studied the hydrogen-surface interactions for four low-index surfaces of PdCu through first-principles calculations. It was found that H-PdCu adsorption strong relies on the facets, hydrogen coverage, and reaction environment (temperature and H-pressure. Our work highlights the importance of the environment on the nature of catalyst surfaces and reactions and offers a plausible way to investigate the interactions between gas and the surfaces of nanocatalysts in real reactions.

  7. The influence of surface oxygen and hydroxyl groups on the dehydrogenation of ethylene, acetic acid and hydrogenated vinyl acetate on pure Pd(1 0 0): A DFT study

    Energy Technology Data Exchange (ETDEWEB)

    Huang, Yanping [Key Laboratory for Green Chemical Technology of Ministry of Education, R& D Center for Petrochemical Technology, Tianjin University, Tianjin (China); Collaborative Innovation Center of Chemical Science and Engineering, Tianjin 300072 (China); Dong, Xiuqin [Key Laboratory for Green Chemical Technology of Ministry of Education, R& D Center for Petrochemical Technology, Tianjin University, Tianjin (China); Yu, Yingzhe, E-mail: yzhyu@tju.edu.cn [Key Laboratory for Green Chemical Technology of Ministry of Education, R& D Center for Petrochemical Technology, Tianjin University, Tianjin (China); Zhang, Minhua, E-mail: mhzhangtj@163.com [Key Laboratory for Green Chemical Technology of Ministry of Education, R& D Center for Petrochemical Technology, Tianjin University, Tianjin (China)

    2016-12-01

    Highlights: • All dehydrogenation reactions in vinyl acetate synthesis on Pd(1 0 0) were studied. • The energy barriers of the transition state of the three reactions were calculated. • The influence of surface Os and OHs on all dehydrogenation actions was discussed. - Abstract: On the basis of a Langmuir–Hinshelwood-type mechanism, the dehydrogenation of ethylene, acetic acid and hydrogenated vinyl acetate (VAH) on pure Pd(1 0 0) with surface oxygen atoms (Os) and hydroxyl groups (OHs) was studied with density functional theory (DFT) method. Our calculation results show that both Os and OHs can consistently reduce the activation energies of dehydrogenation of ethylene, acetic acid and VAH to some degree with only one exception that OHs somehow increase the activation energy of VAH. Based on Langmuir–Hinshelwood mechanism, the three dehydrogenation reactions in presence of surface Os and OHs are almost consistently favored, compared with the corresponding processes on clean Pd(1 0 0) surfaces, and thus a Langmuir–Hinshelwood-type mechanism may not be excluded beforehand when investigating the microscopic performance of the oxygen-assisted vinyl acetate synthesis on Pd(1 0 0) catalysts.

  8. Activation of C-H bond in methane by Pd atom from the bonding evolution theory perspective.

    Science.gov (United States)

    Nizovtsev, Anton S

    2013-08-15

    We report detailed study focused on the electron density redistribution during the simple oxidative addition reaction being the crucial stage of various catalytic processes. The bonding evolution theory based on the electron localization function and Thom's catastrophe theory shows that activation of methane's C-H bond by Pd atom consist of six elementary steps. The important feature revealed is the pronounced reorganization of Pd's outer core maxima corresponding to N-shell electrons of metal. Electronic rearrangements identified in this model reaction are likely to be the case in the more complex reactions of the same type involving transition metal compounds and, in principle, can be observed by modern ultrafast spectroscopy and diffraction techniques. Copyright © 2013 Wiley Periodicals, Inc.

  9. Classical theory of atom-surface scattering: The rainbow effect

    Science.gov (United States)

    Miret-Artés, Salvador; Pollak, Eli

    2012-07-01

    The scattering of heavy atoms and molecules from surfaces is oftentimes dominated by classical mechanics. A large body of experiments have gathered data on the angular distributions of the scattered species, their energy loss distribution, sticking probability, dependence on surface temperature and more. For many years these phenomena have been considered theoretically in the framework of the “washboard model” in which the interaction of the incident particle with the surface is described in terms of hard wall potentials. Although this class of models has helped in elucidating some of the features it left open many questions such as: true potentials are clearly not hard wall potentials, it does not provide a realistic framework for phonon scattering, and it cannot explain the incident angle and incident energy dependence of rainbow scattering, nor can it provide a consistent theory for sticking. In recent years we have been developing a classical perturbation theory approach which has provided new insight into the dynamics of atom-surface scattering. The theory includes both surface corrugation as well as interaction with surface phonons in terms of harmonic baths which are linearly coupled to the system coordinates. This model has been successful in elucidating many new features of rainbow scattering in terms of frictions and bath fluctuations or noise. It has also given new insight into the origins of asymmetry in atomic scattering from surfaces. New phenomena deduced from the theory include friction induced rainbows, energy loss rainbows, a theory of super-rainbows, and more. In this review we present the classical theory of atom-surface scattering as well as extensions and implications for semiclassical scattering and the further development of a quantum theory of surface scattering. Special emphasis is given to the inversion of scattering data into information on the particle-surface interactions.

  10. Theory of inelastic effects in resonant atom-surface scattering

    International Nuclear Information System (INIS)

    Evans, D.K.

    1983-01-01

    The progress of theoretical and experimental developments in atom-surface scattering is briefly reviewed. The formal theory of atom-surface resonant scattering is reviewed and expanded, with both S and T matrix approaches being explained. The two-potential formalism is shown to be useful for dealing with the problem in question. A detailed theory based on the S-matrix and the two-potential formalism is presented. This theory takes account of interactions between the incident atoms and the surface phonons, with resonant effects being displayed explicitly. The Debye-Waller attenuation is also studied. The case in which the atom-surface potential is divided into an attractive part V/sub a/ and a repulsive part V/sub r/ is considered at length. Several techniques are presented for handling the scattering due to V/sub r/, for the case in which V/sub r/ is taken to be the hard corrugated surface potential. The theory is used to calculate the scattered intensities for the system 4 He/LiF(001). A detailed comparison with experiment is made, with polar scans, azimuthal scans, and time-of-flight measurements being considered. The theory is seen to explain the location and signature of resonant features, and to provide reasonable overall agreement with the experimental results

  11. Bifunctional Ag@Pd-Ag Nanocubes for Highly Sensitive Monitoring of Catalytic Reactions by Surface-Enhanced Raman Spectroscopy.

    Science.gov (United States)

    Li, Jumei; Liu, Jingyue; Yang, Yin; Qin, Dong

    2015-06-10

    We report a route to the facile synthesis of Ag@Pd-Ag nanocubes by cotitrating Na2PdCl4 and AgNO3 into an aqueous suspension of Ag nanocubes at room temperature in the presence of ascorbic acid and poly(vinylpyrrolidone). With an increase in the total titration volume, we observed the codeposition of Pd and Ag atoms onto the edges, corners, and side faces of the Ag nanocubes in a site-by-site fashion. By maneuvering the Pd/Ag ratio, we could optimize the SERS and catalytic activities of the Ag@Pd-Ag nanocubes for in situ SERS monitoring of the Pd-catalyzed reduction of 4-nitrothiophenol by NaBH4.

  12. Morphology dependent catalysis and surface enhanced Raman scattering (SERS) studies using Pd nanostructures in DNA, CTAB and PVA scaffolds.

    Science.gov (United States)

    Kundu, Subrata; Yi, Su-In; Ma, Lian; Chen, Yunyun; Dai, Wei; Sinyukov, Alexander M; Liang, Hong

    2017-07-25

    Palladium nanoparticles (Pd NPs) of three different morphologies viz., nanocubes with cetyltrimethylammonium bromide (CTAB), nanowires with polyvinyl alcohol (PVA) and Pd NPs with deoxyribonucleic acid (DNA) scaffolds were synthesized by UV-irradiation. Catalysis and surface enhanced Raman scattering (SERS) studies were done with the synthesized morphologically distinct Pd nanostructures for the very first time. The catalytic rate was extremely high with Pd nanowires templated with PVA and the order of the catalytic rate was Pd nanowires in PVA > Pd nanocubes in CTAB > DNA-Pd wire-like assemblies. The highest catalytic rate was observed for PVA capped Pd nanowires which is a few hundred fold higher than other metal NP catalysts. Methylene blue (MB) was used as a Raman analyte for the SERS study and the largest EF of 1.9 × 10 5 at a peak position of 1391 cm -1 was observed with Pd nanowires in the DNA scaffold as a SERS substrate. The order of the SERS EF values was DNA-Pd wire-like assemblies > Pd nanocubes in CTAB > Pd nanowires in PVA. Beyond everything, the present synthesis route is easy, faster, candid, highly reproducible and cost-effective. In the near future, the same protocol could be applied to synthesize other materials for various applications.

  13. Surface structure investigations using noncontact atomic force microscopy

    International Nuclear Information System (INIS)

    Kolodziej, J.J.; Such, B.; Goryl, M.; Krok, F.; Piatkowski, P.; Szymonski, M.

    2006-01-01

    Surfaces of several A III B V compound semiconductors (InSb, GaAs, InP, InAs) of the (0 0 1) orientation have been studied with noncontact atomic force microscopy (NC-AFM). Obtained atomically resolved patterns have been compared with structural models available in the literature. It is shown that NC-AFM is an efficient tool for imaging complex surface structures in real space. It is also demonstrated that the recent structural models of III-V compound surfaces provide a sound base for interpretation of majority of features present in recorded patterns. However, there are also many new findings revealed by the NC-AFM method that is still new experimental technique in the context of surface structure determination

  14. Performance of surface on ultrafine grained Ti-0.2Pd in simulated body fluid

    Science.gov (United States)

    Wang, Xiu-Lai; Zhou, Qing; Yang, Kai; Zou, Cheng-Hong; Wang, Lei

    2018-03-01

    Ti-0.2 wt% Pd (Ti-0.2Pd) which has high crevice corrosion resistance is highlighted for implant applications. In this work, Ti-0.2Pd alloy is subjected to equal channel angular pressing (ECAP) for grain refinement. The effect of the microstructure on the surface performance of Ti-0.2Pd in a simulated body fluid (SBF) adding bovine serum albumin is investigated. Heat-treated specimens including furnace cooled (FC) and water quenched (WQ) specimens are also prepared for comparison. The corrosion resistance is evaluated by the tests of potentiodynamic polarization and the measurement of electrochemical impedance spectroscopy (EIS). The composition and morphology of the surface after exposing to SBF 60 days were examined by X-ray photoelectronic spectroscopy (XPS), scanning electron microscope (SEM) and energy dispersive spectrometer (EDS). The results show an ultrafine grained microstructure with average grain size of 3.6 μm is obtained after ECAP. The ultrafine grained Ti-0.2Pd has higher corrosion resistance than AR(as-received), WQ and FC specimens. The quantitative analysis of the surface shows larger numbers of precipitations formed on ECAPed Ti-0.2Pd than those formed on heat-treated. The precipitation contains more oxygen, calcium and phosphorus on ECAPed specimen than those on other specimens. The Ca:P ratio is ranged from 1:0.7 to 1:4.4, no dependent on the specimen type. A larger Warburg resistance is obtained on WQ specimen indicating a denser layer formation on WQ specimen. The precipitation formed on WQ specimens is the least among three kinds of specimens. Palladium is not found on the surfaces after exposure to SBF.

  15. ATOMIC POSITIONS ON OXYGEN-COVERED CU(110) SURFACES

    NARCIS (Netherlands)

    DORENBOS, G; BREEMAN, M; BOERMA, DO

    The reconstructed Cu(110)-p(2 x 1)O and Cu(110)-c(6 x 2)O surfaces were studied using low-energy ion scattering combined with time of flight. Azimuthal scans were measured with 6 keV Ar ions for recoiling O, scattered Ar and recoiling Cu atoms. Part of the scans were analysed using a newly developed

  16. Atomic and molecular layer deposition for surface modification

    International Nuclear Information System (INIS)

    Vähä-Nissi, Mika; Sievänen, Jenni; Salo, Erkki; Heikkilä, Pirjo; Kenttä, Eija; Johansson, Leena-Sisko; Koskinen, Jorma T.; Harlin, Ali

    2014-01-01

    Atomic and molecular layer deposition (ALD and MLD, respectively) techniques are based on repeated cycles of gas–solid surface reactions. A partial monolayer of atoms or molecules is deposited to the surface during a single deposition cycle, enabling tailored film composition in principle down to molecular resolution on ideal surfaces. Typically ALD/MLD has been used for applications where uniform and pinhole free thin film is a necessity even on 3D surfaces. However, thin – even non-uniform – atomic and molecular deposited layers can also be used to tailor the surface characteristics of different non-ideal substrates. For example, print quality of inkjet printing on polymer films and penetration of water into porous nonwovens can be adjusted with low-temperature deposited metal oxide. In addition, adhesion of extrusion coated biopolymer to inorganic oxides can be improved with a hybrid layer based on lactic acid. - Graphical abstract: Print quality of a polylactide film surface modified with atomic layer deposition prior to inkjet printing (360 dpi) with an aqueous ink. Number of printed dots illustrated as a function of 0, 5, 15 and 25 deposition cycles of trimethylaluminum and water. - Highlights: • ALD/MLD can be used to adjust surface characteristics of films and fiber materials. • Hydrophobicity after few deposition cycles of Al 2 O 3 due to e.g. complex formation. • Same effect on cellulosic fabrics observed with low temperature deposited TiO 2 . • Different film growth and oxidation potential with different precursors. • Hybrid layer on inorganic layer can be used to improve adhesion of polymer melt

  17. Atomic and molecular layer deposition for surface modification

    Energy Technology Data Exchange (ETDEWEB)

    Vähä-Nissi, Mika, E-mail: mika.vaha-nissi@vtt.fi [VTT Technical Research Centre of Finland, PO Box 1000, FI‐02044 VTT (Finland); Sievänen, Jenni; Salo, Erkki; Heikkilä, Pirjo; Kenttä, Eija [VTT Technical Research Centre of Finland, PO Box 1000, FI‐02044 VTT (Finland); Johansson, Leena-Sisko, E-mail: leena-sisko.johansson@aalto.fi [Aalto University, School of Chemical Technology, Department of Forest Products Technology, PO Box 16100, FI‐00076 AALTO (Finland); Koskinen, Jorma T.; Harlin, Ali [VTT Technical Research Centre of Finland, PO Box 1000, FI‐02044 VTT (Finland)

    2014-06-01

    Atomic and molecular layer deposition (ALD and MLD, respectively) techniques are based on repeated cycles of gas–solid surface reactions. A partial monolayer of atoms or molecules is deposited to the surface during a single deposition cycle, enabling tailored film composition in principle down to molecular resolution on ideal surfaces. Typically ALD/MLD has been used for applications where uniform and pinhole free thin film is a necessity even on 3D surfaces. However, thin – even non-uniform – atomic and molecular deposited layers can also be used to tailor the surface characteristics of different non-ideal substrates. For example, print quality of inkjet printing on polymer films and penetration of water into porous nonwovens can be adjusted with low-temperature deposited metal oxide. In addition, adhesion of extrusion coated biopolymer to inorganic oxides can be improved with a hybrid layer based on lactic acid. - Graphical abstract: Print quality of a polylactide film surface modified with atomic layer deposition prior to inkjet printing (360 dpi) with an aqueous ink. Number of printed dots illustrated as a function of 0, 5, 15 and 25 deposition cycles of trimethylaluminum and water. - Highlights: • ALD/MLD can be used to adjust surface characteristics of films and fiber materials. • Hydrophobicity after few deposition cycles of Al{sub 2}O{sub 3} due to e.g. complex formation. • Same effect on cellulosic fabrics observed with low temperature deposited TiO{sub 2}. • Different film growth and oxidation potential with different precursors. • Hybrid layer on inorganic layer can be used to improve adhesion of polymer melt.

  18. H electro-insertion into Pd/Pt(1 1 1) nanofilms: an original method for isotherm measurement coupled to in situ surface X-ray diffraction structural study

    International Nuclear Information System (INIS)

    Soldo-Olivier, Y.; Sibert, E.; Previdello, B.; Lafouresse, M.C.; Maillard, F.; De Santis, M.

    2013-01-01

    In order to get a thorough comprehension of the mechanisms governing hydrogen insertion into nanometric metallic films, we have studied ultra-thin Pd/Pt(1 1 1) layers. In this paper we propose an original method allowing the measurement of hydrogen insertion electrochemical isotherms. The use of a hanging meniscus rotating disc electrode and a new calculation approach permit to remove the contributions to the insertion charge of both hydrogen evolution and hydrogen oxidation reactions. Indeed, compared to hydrogen insertion such terms become non-negligible in the case of nanometric deposits, due to their large surface/bulk atom ratio. We have measured hydrogen insertion isotherms for Pd/Pt(1 1 1) films from 14 ML down to 4 ML. Independently from the film thickness, the maximum hydrogen insertion rate (H/Pd) max is smaller than that of bulk Pd. The so-called two-phase region is still present, but contrarily to bulk Pd it is characterized by a slope. Both hydrogen solubility and the two-phase domain width diminish with the decrease of the film thickness. In the present work the behaviour of hydrogen electrochemical insertion isotherms is interpreted in the light of the Pd nanofilms structure obtained with in situ surface X-ray diffraction. The lattice constraints induced by the substrate result in a lower insertion rate in the Pd deposit close to the Pt–Pd interface. Only the outermost region of the film is relaxed and behaves like bulk Pd. This description quantitatively accounts for the experimental behaviour of (H/Pd) max as a function of the film thickness. The obtained Pd/Pt(1 1 1) films structure also corresponds to the presence of non-equivalent hydrogen insertion sites, surely contributing to the slope observed in the two-phase domain

  19. Surface Preparation of InAs (110 Using Atomic Hydrogen

    Directory of Open Access Journals (Sweden)

    T.D. Veal

    2002-06-01

    Full Text Available Atomic hydrogen cleaning has been used to produce structurally and electronically damage-free InAs(110 surfaces.  X-ray photoelectron spectroscopy (XPS was used to obtain chemical composition and chemical state information about the surface, before and after the removal of the atmospheric contamination. Low energy electron diffraction (LEED and high-resolution electron-energy-loss spectroscopy (HREELS were also used, respectively, to determine the surface reconstruction and degree of surface ordering, and to probe the adsorbed contaminant vibrational modes and the collective excitations of the clean surface. Clean, ordered and stoichiometric  InAs(110-(1×1 surfaces were obtained by exposure to thermally generated atomic hydrogen at a substrate temperature as low as 400ºC.  Semi-classical dielectric theory analysis of HREEL spectra of the phonon and plasmon excitations of the clean surface indicate that no electronic damage or dopant passivation were induced by the surface preparation method.

  20. Mechanisms of subthreshold atomic emission from solid surfaces

    International Nuclear Information System (INIS)

    Kiv, A.E.; Elango, M.A.; Britavskaya, E.P.; Zaharchenko, I.G.

    1994-01-01

    Computer simulation of the dynamics of ions and atoms on the surfaces of solids has been carried out. The Coulomb, Pauli, exchange and Van der Waals potentials have been taken into account. The semi-empirical quantum-chemical method has been used also. In the case of alkali halide surfaces it is shown that if recharge of an anion (X - → X + ) occurs in two surface layers, it may initiate the ejection of positive metal ions (M + ) and, assisted by the capture of an electron by a departing M + , of metal atoms M 0 . Besides the Coulomb repulsion the Pauli shock is shown to play an essential role in the driving of the ejection process. This mechanism of desorption has large efficiency when the excitation of a core electron occurs in case of alkali halide crystals and has a strong dependence on the crystal ionicity. We obtained the energy distribution of ejected particles for different mechanisms of electron-ion emission. (orig.)

  1. Nanoscale Structuring of Surfaces by Using Atomic Layer Deposition.

    Science.gov (United States)

    Sobel, Nicolas; Hess, Christian

    2015-12-07

    Controlled structuring of surfaces is interesting for a wide variety of areas, including microelectronic device fabrication, optical devices, bio(sensing), (electro-, photo)catalysis, batteries, solar cells, fuel cells, and sorption. A unique feature of atomic layer deposition (ALD) is the possibility to form conformal uniform coatings on arbitrarily shaped materials with controlled atomic-scale thickness. In this Minireview, we discuss the potential of ALD for the nanoscale structuring of surfaces, highlighting its versatile application to structuring both planar substrates and powder materials. Recent progress in the application of ALD to porous substrates has even made the nanoscale structuring of high-surface-area materials now feasible, thereby enabling novel applications, such as those in the fields of catalysis and alternative energy. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  2. Atomic resolution imaging of polyhedral PtPd core-shell nanoparticles by Cs-corrected STEM.

    Science.gov (United States)

    Khanal, Subarna; Casillas, Gilberto; Velazquez-Salazar, J Jesus; Ponce, Arturo; Jose-Yacaman, Miguel

    2012-11-08

    Bimetallic nanoparticles present different properties than their monometallic counterparts, opening a wide range of possibilities for different applications. PtPd nanoparticles have raised interest for their many applications in fuel cells, ethanol and methanol oxidation reactions, hydrogen storage, etc. However, the cost of Pt makes it unpractical to use in big quantities; therefore, one of the big challenges is to synthesize very small catalysts in order to maximize the efficiency in their use. In this work, we synthesized polyhedral PtPd core-shell nanoparticles under 20 nm and characterized them by Cs-corrected scanning transmission electron microscopy. This technique allowed us to probe the structure at the atomic level of these nanoparticles revealing new structural information. We determined the structure of the three main polyhedral morphologies obtained in the synthesis: octahedral, decahedral and triangular plates. Decahedral PtPd core-shell nanoparticles are novel morphologies for this system. Morphology and defects present in the nanoparticles are shown and discussed.

  3. Atomic-scale friction on stepped surfaces of ionic crystals.

    Science.gov (United States)

    Steiner, Pascal; Gnecco, Enrico; Krok, Franciszek; Budzioch, Janusz; Walczak, Lukasz; Konior, Jerzy; Szymonski, Marek; Meyer, Ernst

    2011-05-06

    We report on high-resolution friction force microscopy on a stepped NaCl(001) surface in ultrahigh vacuum. The measurements were performed on single cleavage step edges. When blunt tips are used, friction is found to increase while scanning both up and down a step edge. With atomically sharp tips, friction still increases upwards, but it decreases and even changes sign downwards. Our observations extend previous results obtained without resolving atomic features and are associated with the competition between the Schwöbel barrier and the asymmetric potential well accompanying the step edges.

  4. STIR: Improved Electrolyte Surface Exchange via Atomically Strained Surfaces

    Science.gov (United States)

    2015-09-03

    PLEASE DO NOT RETURN YOUR FORM TO THE ABOVE ADDRESS. University of Delaware 210 Hullihen Hall Newark, DE 19716 -0099 9-Jan-2015 ABSTRACT Number of Papers... Planck system modified to include reaction terms was built in COMSOL Multiphysics to describe the mass and charge fluxes related to electrons and both...include that the adsorption rate constant controls the behavior of platinum electrodes on YSZ surfaces much more than the reaction rate constant for

  5. Attractive interaction between an atom and a surface

    International Nuclear Information System (INIS)

    Manson, J.R.; Ritchie, R.H.

    1983-01-01

    Using a general self-energy formalism we examine the interaction between an atom and a surface. Considered in detail are deviations from the Van der Waals force due to recoil and finite velocity of the particle. Calculations for positronium near a metal surface show that for such systems recoil and velocity effects are significant even at very low energies. We also examine the mechanisms for energy exchange with the surface and calculations show that single quantum events do not always dominate the exchange rates. 8 references, 2 figures

  6. Collagen fiber with surface-grafted polyphenol as a novel support for Pd(0) nanoparticles: Synthesis, characterization and catalytic application

    Energy Technology Data Exchange (ETDEWEB)

    Wu Hao [Department of Biomass Chemistry and Engineering, Sichuan University, Chengdu 610065 (China); Wu Chao [National Engineering Laboratory for Clean Technology of Leather Manufacture, Sichuan University, Chengdu 610065 (China); He Qiang [Department of Biomass Chemistry and Engineering, Sichuan University, Chengdu 610065 (China); Liao Xuepin, E-mail: sibitannin@vip.163.com [National Engineering Laboratory for Clean Technology of Leather Manufacture, Sichuan University, Chengdu 610065 (China); Shi Bi, E-mail: xpliao@scu.edu.cn [Department of Biomass Chemistry and Engineering, Sichuan University, Chengdu 610065 (China); National Engineering Laboratory for Clean Technology of Leather Manufacture, Sichuan University, Chengdu 610065 (China)

    2010-06-15

    The aim of this study is to use collagen fiber (CF) as a natural polymeric support to synthesize a novel palladium (Pd) nanoparticle catalyst. To achieve a stable immobilization of Pd on CF support, epigallocatechin-3-gallate (EGCG), a typical plant polyphenol, was grafted onto CF surface, acting both as dispersing and stabilizing agent for Pd nanoparticles. Scanning electron microscopy showed that this catalyst was in ordered fibrous state with high flexibility. The presence of EGCG grafted on CF and the interaction mechanism of Pd ions with support was investigated by X-ray photoelectron spectroscopy. X-ray diffraction and transmission electron microscopy offered evidence that the well-dispersed Pd nanoparticles were generated on the outer surface of CF. By using the hydrogenation of allyl alcohol as a model reaction, the synthesized catalyst presented remarkably improved activity, selectivity and reusability as compared with the Pd catalyst supported by CF without grafting of EGCG.

  7. Fermi surface and band structure of BiPd from ARPES studies

    Science.gov (United States)

    Lohani, H.; Mishra, P.; Gupta, Anurag; Awana, V. P. S.; Sekhar, B. R.

    2017-03-01

    We present a detailed electronic structure study of the non-centrosymmetric superconductor BiPd based on our angle resolved photoemission spectroscopy (ARPES) measurements and Density Functional Theory (DFT) based calculations. We observe a high intensity distribution on the Fermi surface (FS) of this compound resulting from various electron and hole like bands which are present in the vicinity of the Fermi energy (Ef). The near Ef states are primarily composed of Bi-6p with a little admixture of Pd-4dx2-y2/zy orbitals. There are various spin-orbit split bands involved in the crossing of Ef making a complex FS. The FS mainly consists of multi sheets of three dimensions which disfavor the nesting between different sheets of the FS. Our comprehensive study elucidates that BiPd could be a s-wave multiband superconductor.

  8. Observation of the spin-polarized surface state in a noncentrosymmetric superconductor BiPd.

    Science.gov (United States)

    Neupane, Madhab; Alidoust, Nasser; Hosen, M Mofazzel; Zhu, Jian-Xin; Dimitri, Klauss; Xu, Su-Yang; Dhakal, Nagendra; Sankar, Raman; Belopolski, Ilya; Sanchez, Daniel S; Chang, Tay-Rong; Jeng, Horng-Tay; Miyamoto, Koji; Okuda, Taichi; Lin, Hsin; Bansil, Arun; Kaczorowski, Dariusz; Chou, Fangcheng; Hasan, M Zahid; Durakiewicz, Tomasz

    2016-11-07

    Recently, noncentrosymmetric superconductor BiPd has attracted considerable research interest due to the possibility of hosting topological superconductivity. Here we report a systematic high-resolution angle-resolved photoemission spectroscopy (ARPES) and spin-resolved ARPES study of the normal state electronic and spin properties of BiPd. Our experimental results show the presence of a surface state at higher-binding energy with the location of Dirac point at around 700 meV below the Fermi level. The detailed photon energy, temperature-dependent and spin-resolved ARPES measurements complemented by our first-principles calculations demonstrate the existence of the spin-polarized surface states at high-binding energy. The absence of such spin-polarized surface states near the Fermi level negates the possibility of a topological superconducting behaviour on the surface. Our direct experimental observation of spin-polarized surface states in BiPd provides critical information that will guide the future search for topological superconductivity in noncentrosymmetric materials.

  9. First principles investigation of the activity of thin film Pt, Pd and Au surface alloys for oxygen reduction

    DEFF Research Database (Denmark)

    Tripkovic, Vladimir; Hansen, Heine Anton; Rossmeisl, Jan

    2015-01-01

    driving force for surface segregation, diffusion to defects or surface self-assembling. On the basis of stability and activity analysis we conclude that the near surface alloy of Pd in Pt and some PdAu binary and PtPdAu ternary thin films with a controlled amount of Au are the best catalysts for oxygen......Further advances in fuel cell technologies are hampered by kinetic limitations associated with the sluggish cathodic oxygen reduction reaction. We have investigated a range of different formulations of binary and ternary Pt, Pd and Au thin films as electrocatalysts for oxygen reduction. The most...... active binary thin films are near-surface alloys of Pt with subsurface Pd and certain PdAu and PtAu thin films with surface and/or subsurface Au. The most active ternary thin films are with pure metal Pt or Pd skins with some degree of Au in the surface and/or subsurface layer and the near-surface alloys...

  10. The role of charge transfer in the oxidation state change of Ce atoms in the TM13-CeO2(111) systems (TM = Pd, Ag, Pt, Au): a DFT + U investigation.

    Science.gov (United States)

    Tereshchuk, Polina; Freire, Rafael L H; Ungureanu, Crina G; Seminovski, Yohanna; Kiejna, Adam; Da Silva, Juarez L F

    2015-05-28

    Despite extensive studies of transition metal (TM) clusters supported on ceria (CeO2), fundamental issues such as the role of the TM atoms in the change in the oxidation state of Ce atoms are still not well understood. In this work, we report a theoretical investigation based on static and ab initio molecular dynamics density functional theory calculations of the interaction of 13-atom TM clusters (TM = Pd, Ag, Pt, Au) with the unreduced CeO2(111) surface represented by a large surface unit cell and employing Hubbard corrections for the strong on-site Coulomb correlation in the Ce f-electrons. We found that the TM13 clusters form pyramidal-like structures on CeO2(111) in the lowest energy configurations with the following stacking sequence, TM/TM4/TM8/CeO2(111), while TM13 adopts two-dimensional structures at high energy structures. TM13 induces a change in the oxidation state of few Ce atoms (3 of 16) located in the topmost Ce layer from Ce(IV) (itinerant Ce f-states) to Ce(III) (localized Ce f-states). There is a charge flow from the TM atoms to the CeO2(111) surface, which can be explained by the electronegativity difference between the TM (Pd, Ag, Pt, Au) and O atoms, however, the charge is not uniformly distributed on the topmost O layer due to the pressure induced by the TM13 clusters on the underlying O ions, which yields a decrease in the ionic charge of the O ions located below the cluster and an increase in the remaining O ions. Due to the charge flow mainly from the TM8-layer to the topmost O-layer, the charge cannot flow from the Ce(IV) atoms to the O atoms with the same magnitude as in the clean CeO2(111) surface. Consequently, the effective cationic charge decreases mainly for the Ce atoms that have a bond with the O atoms not located below the cluster, and hence, those Ce atoms change their oxidation state from IV to III. This increases the size of the Ce(III) compared with the Ce(IV) cations, which builds-in a strain within the topmost Ce layer, and

  11. Site-selective substitutional doping with atomic precision on stepped Al (111) surface by single-atom manipulation.

    Science.gov (United States)

    Chen, Chang; Zhang, Jinhu; Dong, Guofeng; Shao, Hezhu; Ning, Bo-Yuan; Zhao, Li; Ning, Xi-Jing; Zhuang, Jun

    2014-01-01

    In fabrication of nano- and quantum devices, it is sometimes critical to position individual dopants at certain sites precisely to obtain the specific or enhanced functionalities. With first-principles simulations, we propose a method for substitutional doping of individual atom at a certain position on a stepped metal surface by single-atom manipulation. A selected atom at the step of Al (111) surface could be extracted vertically with an Al trimer-apex tip, and then the dopant atom will be positioned to this site. The details of the entire process including potential energy curves are given, which suggests the reliability of the proposed single-atom doping method.

  12. Atomic Resolution Imaging and Quantification of Chemical Functionality of Surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Schwarz, Udo D. [Yale Univ., New Haven, CT (United States). Dept. of Mechanical Engineering and Materials Science; Altman, Eric I. [Yale Univ., New Haven, CT (United States). Dept. of Chemical and Environmental Engineering

    2014-12-10

    The work carried out from 2006-2014 under DoE support was targeted at developing new approaches to the atomic-scale characterization of surfaces that include species-selective imaging and an ability to quantify chemical surface interactions with site-specific accuracy. The newly established methods were subsequently applied to gain insight into the local chemical interactions that govern the catalytic properties of model catalysts of interest to DoE. The foundation of our work was the development of three-dimensional atomic force microscopy (3DAFM), a new measurement mode that allows the mapping of the complete surface force and energy fields with picometer resolution in space (x, y, and z) and piconewton/millielectron volts in force/energy. From this experimental platform, we further expanded by adding the simultaneous recording of tunneling current (3D-AFM/STM) using chemically well-defined tips. Through comparison with simulations, we were able to achieve precise quantification and assignment of local chemical interactions to exact positions within the lattice. During the course of the project, the novel techniques were applied to surface-oxidized copper, titanium dioxide, and silicon oxide. On these materials, defect-induced changes to the chemical surface reactivity and electronic charge density were characterized with site-specific accuracy.

  13. Semiclassical perturbation theory for diffraction in heavy atom surface scattering.

    Science.gov (United States)

    Miret-Artés, Salvador; Daon, Shauli; Pollak, Eli

    2012-05-28

    The semiclassical perturbation theory formalism of Hubbard and Miller [J. Chem. Phys. 78, 1801 (1983)] for atom surface scattering is used to explore the possibility of observation of heavy atom diffractive scattering. In the limit of vanishing ℏ the semiclassical theory is shown to reduce to the classical perturbation theory. The quantum diffraction pattern is sensitive to the characteristics of the beam of incoming particles. Necessary conditions for observation of quantum diffraction are derived for the angular width of the incoming beam. An analytic expression for the angular distribution as a function of the angular and momentum variance of the incoming beam is obtained. We show both analytically and through some numerical results that increasing the angular width of the incident beam leads to decoherence of the quantum diffraction peaks and one approaches the classical limit. However, the incoherence of the beam in the parallel direction does not destroy the diffraction pattern. We consider the specific example of Ar atoms scattered from a rigid LiF(100) surface.

  14. Preparation of well-defined samples of AlPdMn quasicrystals for surface studies

    Science.gov (United States)

    Jenks, C. J.; Delaney, D. W.; Bloomer, T. E.; Chang, S.-L.; Lograsso, T. A.; Shen, Z.; Zhang, C.-M.; Thiel, P. A.

    1996-12-01

    We have developed a method for preparing single-grain, quasicrystalline AlPdMn samples for surface studies in ultrahigh vacuum. The main issues of concern are phase purity, the quality of the surface structure, and the surface, and the surface composition. Phase purity is enhanced by annealing the sample in ultra-pure Ar in a sealed quartz ampoule for several days before polishing. Polishing with colloidal silica allows secondary phases to be detected readily with an optical microscope. As a final precaution, phase purity can be checked sensitively with scanning Auger microscopy. After this stage, the sample can be cleaned in ultrahigh vacuum with ion bombardment. Annealing is required after bombardment to restore surface structure and to obtain a low-energy electron diffraction (LEED) pattern of an oriented sample. However, both ion bombardment and heating to temperatures above 870 K in vacuum, produce Pd-rich surfaces. As a final step, for the five-fold surface, we recommend heating briefly to 1050-1100 K and then annealing at 870 K for several hours. This produces both an excellent LEED pattern, and a surface composition close to that of the bulk.

  15. Investigation of magnetorheological elastomer surface properties by atomic force microscopy

    International Nuclear Information System (INIS)

    Iacobescu, G.E.; Balasoiu, M.; Bica, I.

    2012-01-01

    Magnetorheological elastomers consist of a natural or synthetic rubber matrix interspersed with micron-sized ferromagnetic particles. The magnetoelastic properties of such a composite are not merely a sum of elasticity of the polymer and stiffness and magnetic properties of the filler, but also the result of a complex synergy of several effects, relevant at different length scales and detectable by different techniques. In the present work we investigate the microstructures, the surface magnetic properties and the elastic properties of new isotropic and anisotropic magnetorheological elastomer prepared using silicone rubber and soft magnetic carbonyl iron microspheres. The measurements were performed by atomic force microscopy in the following modes: standard imaging-non-contact atomic force microscopy, magnetic force microscopy and nanoindentation. A comparative study for the samples with different particle concentrations and strength of magnetic field applied during the polymerization process is developed

  16. Atomic and electronic structure of surfaces theoretical foundations

    CERN Document Server

    Lannoo, Michel

    1991-01-01

    Surfaces and interfaces play an increasingly important role in today's solid state devices. In this book the reader is introduced, in a didactic manner, to the essential theoretical aspects of the atomic and electronic structure of surfaces and interfaces. The book does not pretend to give a complete overview of contemporary problems and methods. Instead, the authors strive to provide simple but qualitatively useful arguments that apply to a wide variety of cases. The emphasis of the book is on semiconductor surfaces and interfaces but it also includes a thorough treatment of transition metals, a general discussion of phonon dispersion curves, and examples of large computational calculations. The exercises accompanying every chapter will be of great benefit to the student.

  17. Single atom anisotropic magnetoresistance on a topological insulator surface

    KAUST Repository

    Narayan, Awadhesh

    2015-03-12

    © 2015 IOP Publishing Ltd and Deutsche Physikalische Gesellschaft. We demonstrate single atom anisotropic magnetoresistance on the surface of a topological insulator, arising from the interplay between the helical spin-momentum-locked surface electronic structure and the hybridization of the magnetic adatom states. Our first-principles quantum transport calculations based on density functional theory for Mn on Bi2Se3 elucidate the underlying mechanism. We complement our findings with a two dimensional model valid for both single adatoms and magnetic clusters, which leads to a proposed device setup for experimental realization. Our results provide an explanation for the conflicting scattering experiments on magnetic adatoms on topological insulator surfaces, and reveal the real space spin texture around the magnetic impurity.

  18. Adsorption of Cu and Pd on alpha-Al2O3(0001) surfaces with different stoichiometries

    DEFF Research Database (Denmark)

    Lodziana, Zbigniew; Nørskov, Jens Kehlet

    2001-01-01

    We report density functional theory calculations of the interaction of Cu and Pd with the (0001) surface of alpha -Al2O3. The interaction of those metals with the oxide surface varies from covalent-like for the aluminum rich surface to ionic-like for the oxygen terminated surface. Stoichiometric...

  19. Atomic force microscopy analysis of different surface treatments of Ti dental implant surfaces

    International Nuclear Information System (INIS)

    Bathomarco, R.V.; Solorzano, G.; Elias, C.N.; Prioli, R.

    2004-01-01

    The surface of commercial unalloyed titanium, used in dental implants, was analyzed by atomic force microscopy. The morphology, roughness, and surface area of the samples, submitted to mechanically-induced erosion, chemical etching and a combination of both, were compared. The results show that surface treatments strongly influence the dental implant physical and chemical properties. An analysis of the length dependence of the implant surface roughness shows that, for scan sizes larger than 50 μm, the average surface roughness is independent of the scanning length and that the surface treatments lead to average surface roughness in the range of 0.37 up to 0.48 μm. It is shown that the implant surface energy is sensitive to the titanium surface area. As the area increases there is a decrease in the surface contact angle

  20. Atomic force microscopy analysis of different surface treatments of Ti dental implant surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Bathomarco, R.V.; Solorzano, G.; Elias, C.N.; Prioli, R

    2004-06-30

    The surface of commercial unalloyed titanium, used in dental implants, was analyzed by atomic force microscopy. The morphology, roughness, and surface area of the samples, submitted to mechanically-induced erosion, chemical etching and a combination of both, were compared. The results show that surface treatments strongly influence the dental implant physical and chemical properties. An analysis of the length dependence of the implant surface roughness shows that, for scan sizes larger than 50 {mu}m, the average surface roughness is independent of the scanning length and that the surface treatments lead to average surface roughness in the range of 0.37 up to 0.48 {mu}m. It is shown that the implant surface energy is sensitive to the titanium surface area. As the area increases there is a decrease in the surface contact angle.

  1. Electro-deposition of Pd on Carbon paper and Ni foam via surface limited redox-replacement reaction for oxygen reduction reaction: Presentation

    CSIR Research Space (South Africa)

    Modibedi, M

    2013-03-01

    Full Text Available during the catalyst preparation process, Pd nanosturctures are grown directly on fuel cell gas diffusion layers and evaluated for the ORR. Pd nanostructures were synthesized via surface-limited redox replacement (SLRR) reaction employing...

  2. Atomic structure of the SbCu surface alloy: A surface X-ray diffraction study

    DEFF Research Database (Denmark)

    Meunier, I.; Gay, J.M.; Lapena, L.

    1999-01-01

    The dissolution at 400 degrees C of an antimony layer deposited at room temperature on a Cu(111) substrate leads to a surface alloy with a p(root 3x root 3)R 30 degrees x 30 degrees superstructure and a Sb composition of 1/3.We present here a structural study of this Sb-Cu compound by surface X......-ray diffraction (SXRD). The best agreement is obtained for a Cu,Sb surface layer with Sb atoms substituting 1/3 of the Cu atoms, over an essentially unperturbed Cu(111) plane. The largest relaxation is undergone by the Sb atoms which rise by 0.32+0.02 Angstrom over the mean plane of its Cu neighbours....... No substantial in-plane relaxations were observed. (C) 1999 Elsevier Science B.V. All rights reserved....

  3. Atomic O and H exposure of C-covered and oxidezed d-metal surfaces

    NARCIS (Netherlands)

    Tsarfati, T.; Tsarfati, T.; Zoethout, E.; van de Kruijs, Robbert Wilhelmus Elisabeth; Bijkerk, Frederik

    2009-01-01

    Carbon coverage, oxidation and reduction of Au, Pt, Pd, Rh, Cu, Ru, Ni and Co layers of 1.5 nm thickness on Mo have been characterized with ARPES and desorption spectroscopy upon exposure to thermal H and O radicals. We observe that only part of the carbon species is chemically eroded by atomic H

  4. Atomic O and H exposure of C-covered and oxidized d-metal surfaces

    NARCIS (Netherlands)

    T. Tsarfati,; Zoethout, E.; van de Kruijs, R. W. E.; F. Bijkerk,

    2009-01-01

    Carbon coverage, oxidation and reduction of Au, Pt, Pd, Rh, Cu, Ru, Ni and Co layers of 1.5 nm thickness on Mo have been characterized with ARPES and desorption spectroscopy upon exposure to thermal H and O radicals. We observe that only part of the carbon species is chemically eroded by atomic H

  5. Segregation at the surfaces of CuxPd1-x alloys in the presence of adsorbed S

    Energy Technology Data Exchange (ETDEWEB)

    Miller, James B.; Priyadarshini, Deepika; Gellman, Andrew J.

    2012-10-01

    The influence of adsorbed S on surface segregation in Cu{sub x}Pd{sub 1 - x} alloys (S/Cu{sub x}Pd{sub 1 - x)} was characterized over a wide range of bulk alloy compositions (x = 0.05 to 0.95) using high-throughput Composition Spread Alloy Film (CSAF) sample libraries. Top-surface and near-surface compositions of the CSAFs were measured as functions of bulk Cu composition, x, and temperature using spatially resolved low energy ion scattering spectroscopy (LEISS) and X-ray photoemission spectroscopy (XPS). Preferential segregation of Cu to the top-surface of the S/Cu{sub x}Pd{sub 1 - x} CSAF was observed at all bulk compositions, x, but the extent of Cu segregation to the S/Cu{sub x}Pd{sub 1 - x} surface was lower than the Cu segregation to the surface of a clean Cu{sub x}Pd{sub 1 - x} CSAF, clear evidence of an S-induced “segregation reversal.” The Langmuir–McLean formulation of the Gibbs isotherm was used to estimate the enthalpy and entropy of Cu segregation to the top-surface, ΔH{sub seg}(x) and ΔS{sub seg}(x), at saturation sulfur coverages. While Cu segregation to the top-surface of the clean Cu{sub x}Pd{sub 1 - x} is exothermic (ΔH{sub seg} < 0) for all bulk Cu compositions, it is endothermic (ΔH{sub seg} > 0) for S/Cu{sub x}Pd{sub 1 - x}. Segregation to the S/Cu{sub x}Pd{sub 1 - x} surface is driven by entropy. Changes in segregation patterns that occur upon adsorption of S onto Cu{sub x}Pd{sub 1 - x} appear to be related to formation of energetically favored Pd{single bond}S bonds at the surface, which counterbalance the enthalpic driving forces for Cu segregation to the clean surface.

  6. ONE-DIMENSIONAL ORDERING OF IN ATOMS IN A CU(100) SURFACE

    NARCIS (Netherlands)

    BREEMAN, M; BARKEMA, GT; BOERMA, DO

    1994-01-01

    A Monte Carlo study of the ordering of In atoms embedded in the top layer of a Cu(100) surface is presented. The interaction energies between the In and Cu atoms were derived from atom-embedding calculations, with Finnis-Sinclair potentials. It was found that the interaction between In atoms in the

  7. Influence of the atomic structure of crystal surfaces on the surface diffusion in medium temperature range

    International Nuclear Information System (INIS)

    Cousty, J.P.

    1981-12-01

    In this work, we have studied the influence of atomic structure of crystal surface on surface self-diffusion in the medium temperature range. Two ways are followed. First, we have measured, using a radiotracer method, the self-diffusion coefficient at 820 K (0.6 T melting) on copper surfaces both the structure and the cleanliness of which were stable during the experiment. We have shown that the interaction between mobile surface defects and steps can be studied through measurements of the anisotropy of surface self diffusion. Second, the behavior of an adatom and a surface vacancy is simulated via a molecular dynamics method, on several surfaces of a Lennard Jones crystal. An inventory of possible migration mechanisms of these surface defects has been drawn between 0.35 and 0.45 Tsub(m). The results obtained with both the methods point out the influence of the surface atomic structure in surface self-diffusion in the medium temperature range [fr

  8. DFT study of the structure, chemical ordering and molecular adsorption of Pd-Ir nanoalloys.

    Science.gov (United States)

    Fan, Tian-E; Demiroglu, Ilker; Hussein, Heider A; Liu, Tun-Dong; Johnston, Roy L

    2017-10-11

    The structures and surface adsorption sites of Pd-Ir nanoalloys are crucial to the understanding of their catalytic performance because they can affect the activity and selectivity of nanocatalysts. In this article, density functional theory (DFT) calculations are performed on bare Pd-Ir nanoalloys to systematically explore their stability and chemical ordering properties, before studying the adsorption of CO on the nanoalloys. First, the structural stability of 38-atom and 79-atom truncated octahedral (TO) Pd-Ir nanoalloys are investigated. Then the adsorption properties and preferred adsorption sites of CO on 38-atom Pd-Ir nanoalloys are considered. The Pd shell Ir core structure, which has the lowest energy of all the considered isomers, exhibits the highest structural stability, while the Pd core Ir shell configuration is the least stable. In addition, the adsorption strength of CO on Ir atoms is found to be greater than on Pd for Pd-Ir nanoclusters. The preferred adsorption sites of CO on pure Pd and Ir clusters are in agreement with calculations and experiments on extended Pd and Ir surfaces. In addition, d-band center and charge effects on CO adsorption strength on Pd-Ir nanoalloys are analyzed by comparison with pure clusters. The study provides a valuable theoretical insight into catalytically active Pd-Ir nanoalloys.

  9. Effects of surface and interface scattering on anomalous Hall effect in Co/Pd multilayers

    KAUST Repository

    Guo, Zaibing

    2012-09-27

    In this paper, we report the results of surface and interface scattering on anomalous Hall effect in Co/Pd multilayers with perpendicular magnetic anisotropy. The surface scattering effect has been extracted from the total anomalous Hall effect. By scaling surface scattering contribution with ρAHs∼ργss, the exponent γ has been found to decrease with the increase of surface scattering resistivity, which could account for the thickness-dependent anomalous Hall effect. Interface diffusion induced by rapid thermal annealing modifies not only the magnetization and longitudinal resistivity but also the anomalous Hall effect; a large exponent γ ∼ 5.7 has been attributed to interface scattering-dominated anomalous Hall effect.

  10. CO adsorption on the GaPd(1[combining macron]1[combining macron]1[combining macron]) surface: a comparative DFT study using different functionals.

    Science.gov (United States)

    Alarcón Villaseca, S; Levchenko, S V; Armbrüster, M

    2016-06-07

    CO adsorption on the polar (1[combining macron]1[combining macron]1[combining macron]) surface of the intermetallic compound GaPd is examined within ab initio methods using an all-electron full-potential electronic structure approach. Comparison between the PW-LDA, GGA-PBE, GGA-RPBE, GGA-revPBE, and hybrid HSE06 functionals is considered through bulk, clean surface and CO adsorption calculations. The choice of the functional is found to have a strong influence in the description of single CO adsorption on the surface model proposed in literature. As expected from the so called "CO adsorption puzzle", differences in the obtained results demonstrate that classic LDA and PBE functionals can only partially describe the complex CO adsorption bonding scenario on a surface containing transition metal elements (in this case Pd atoms), where the energies of the substrate-adsorbate electronic states are shifted, yielding important differences in the absolute values of the adsorption energies, vibrational frequencies and surface-adsorbate interaction. So far the hybrid functional HSE06 correctly retrieves all the tendencies observed experimentally as confirmed by comparing our first-principles results to experimental findings.

  11. Study on the GaAs(110) surface using emitted atom spectrometry

    International Nuclear Information System (INIS)

    Gayone, J.E.; Sanchez, E.A.; Grizzi, O.; Universidad Nacional de Cuyo, Mendoza

    1998-01-01

    The facilities implemented at Bariloche for the ion scattering spectrometry is described, and recent examples of the technique application to determine the atomic structure and the composition of metallic and semiconductor surfaces, pure and with different adsorbates. The surface analysis technique using emitted atom spectrometry is discussed. The sensitivity to the GaAs(110) surface atomic relaxation is presented, and the kinetic of hydrogen adsorption by the mentioned surface is studied

  12. Characterization of polymer surface structure and surface mechanical behaviour by sum frequency generation surface vibrational spectroscopy and atomic force microscopy

    International Nuclear Information System (INIS)

    Opdahl, Aric; Koffas, Telly S; Amitay-Sadovsky, Ella; Kim, Joonyeong; Somorjai, Gabor A

    2004-01-01

    Sum frequency generation (SFG) vibrational spectroscopy and atomic force microscopy (AFM) have been used to study polymer surface structure and surface mechanical behaviour, specifically to study the relationships between the surface properties of polymers and their bulk compositions and the environment to which the polymer is exposed. The combination of SFG surface vibrational spectroscopy and AFM has been used to study surface segregation behaviour of polyolefin blends at the polymer/air and polymer/solid interfaces. SFG surface vibrational spectroscopy and AFM experiments have also been performed to characterize the properties of polymer/liquid and polymer/polymer interfaces, focusing on hydrogel materials. A method was developed to study the surface properties of hydrogel contact lens materials at various hydration conditions. Finally, the effect of mechanical stretching on the surface composition and surface mechanical behaviour of phase-separated polyurethanes, used in biomedical implant devices, has been studied by both SFG surface vibrational spectroscopy and AFM. (topical review)

  13. Probing surfaces with single-polymer atomic force microscope experiments.

    Science.gov (United States)

    Friedsam, C; Gaub, H E; Netz, R R

    2006-03-01

    In the past 15 years atomic force microscope (AFM) based force spectroscopy has become a versatile tool to study inter- and intramolecular interactions of single polymer molecules. Irreversible coupling of polymer molecules between the tip of an AFM cantilever and the substrate allows one to study the stretching response up to the high force regime of several nN. For polymers that glide or slip laterally over the surface with negligible friction, on the other hand, the measured force profiles exhibit plateaus which allow one to extract the polymer adsorption energies. Long-term stable polymer coatings of the AFM tips allow for the possibility of repeating desorption experiments from solid supports with individual molecules many times, yielding good sampling statistics and thus reliable estimates for adsorption energies. In combination with recent advances in theoretical modeling, a detailed picture of the conformational statistics, backbone elasticity, and the adsorption characteristics of single polymer molecules is obtained.

  14. A many-body embedded atom potential for describing ejection of atoms from surfaces

    International Nuclear Information System (INIS)

    Garrison, B.J.; Walzl, K.; El-Maazawi, M.; Winograd, N.; Reimann, C.T.; Deaven, D.M.

    1989-01-01

    In this paper, we show that many-body interactions are important for describing the energy- and angle-resolved distributions of neutral Rh atoms ejected from keV-ion-bombarded Rh{111}. We compare separate classical-dynamics simulations of the sputtering process assuming either a many-body potential or a pairwise additive potential. The most dramatic difference between the many-body potential and the pair potential is the predicted kinetic energy distributions. The pair-potential kinetic energy distribution peaks at ∼ 2 eV, whereas the many-body potential predicts a broader peak at ∼ 4 eV, giving much better agreement with experiment. This difference between the model potentials is due to the predicted nature of the attractive interaction in the surface region through which all ejecting particles pass. (author)

  15. Functionalized polymer film surfaces via surface-initiated atom transfer radical polymerization

    International Nuclear Information System (INIS)

    Hu, Y.; Li, J.S.; Yang, W.T.; Xu, F.J.

    2013-01-01

    The ability to manipulate and control the surface properties of polymer films, without altering the substrate properties, is crucial to their wide-spread applications. In this work, a simple one-step method for the direct immobilization of benzyl chloride groups (as the effective atom transfer radical polymerization (ATRP) initiators) on the polymer films was developed via benzophenone-induced coupling of 4-vinylbenzyl chloride (VBC). Polyethylene (PE) and nylon films were selected as examples of polymer films to illustrate the functionalization of film surfaces via surface-initiated ATRP. Functional polymer brushes of (2-dimethylamino)ethyl methacrylate, sodium 4-styrenesulfonate, 2-hydroxyethyl methacrylate and glycidyl methacrylate, as well as their block copolymer brushes, have been prepared via surface-initiated ATRP from the VBC-coupled PE or nylon film surfaces. With the development of a simple approach to the covalent immobilization of ATRP initiators on polymer film surfaces and the inherent versatility of surface-initiated ATRP, the surface functionality of polymer films can be precisely tailored. - Highlights: ► Atom transfer radical polymerization initiators were simply immobilized. ► Different functional polymer brushes were readily prepared. ► Their block copolymer brushes were also readily prepared

  16. Fabrication of Robust and Antifouling Superhydrophobic Surfaces via Surface-Initiated Atom Transfer Radical Polymerization.

    Science.gov (United States)

    Xue, Chao-Hua; Guo, Xiao-Jing; Ma, Jian-Zhong; Jia, Shun-Tian

    2015-04-22

    Superhydrophobic surfaces were fabricated via surface-initiated atom transfer radical polymerization of fluorinated methacrylates on poly(ethylene terephthalate) (PET) fabrics. The hydrophobicity of the PET fabric was systematically tunable by controlling the polymerization time. The obtained superhydrophobic fabrics showed excellent chemical robustness even after exposure to different chemicals, such as acid, base, salt, acetone, and toluene. Importantly, the fabrics maintained superhydrophobicity after 2500 abrasion cycles, 100 laundering cycles, and long time exposure to UV irradiation. Also, the surface of the superhydrophobic fabrics showed excellent antifouling properties.

  17. Atomic-level Pd-Pt alloying and largely enhanced hydrogen-storage capacity in bimetallic nanoparticles reconstructed from core/shell structure by a process of hydrogen absorption/desorption.

    Science.gov (United States)

    Kobayashi, Hirokazu; Yamauchi, Miho; Kitagawa, Hiroshi; Kubota, Yoshiki; Kato, Kenichi; Takata, Masaki

    2010-04-28

    We have achieved the creation of a solid-solution alloy where Pd and Pt are homogeneously mixed at the atomic level, by a process of hydrogen absorption/desorption as a trigger for core (Pd)/shell (Pt) nanoparticles. The structural change from core/shell to solid solution has been confirmed by in situ powder X-ray diffraction, energy dispersive spectra, solid-state (2)H NMR measurement, and hydrogen pressure-composition isotherms. The successfully obtained Pd-Pt solid-solution nanoparticles with a Pt content of 8-21 atom % had a higher hydrogen-storage capacity than Pd nanoparticles. Moreover, the hydrogen-storage capacity of Pd-Pt solid-solution nanoparticles can be tuned by changing the composition of Pd and Pt.

  18. Surface microstructure of bitumen characterized by atomic force microscopy.

    Science.gov (United States)

    Yu, Xiaokong; Burnham, Nancy A; Tao, Mingjiang

    2015-04-01

    Bitumen, also called asphalt binder, plays important roles in many industrial applications. It is used as the primary binding agent in asphalt concrete, as a key component in damping systems such as rubber, and as an indispensable additive in paint and ink. Consisting of a large number of hydrocarbons of different sizes and polarities, together with heteroatoms and traces of metals, bitumen displays rich surface microstructures that affect its rheological properties. This paper reviews the current understanding of bitumen's surface microstructures characterized by Atomic Force Microscopy (AFM). Microstructures of bitumen develop to different forms depending on crude oil source, thermal history, and sample preparation method. While some bitumens display surface microstructures with fine domains, flake-like domains, and dendrite structuring, 'bee-structures' with wavy patterns several micrometers in diameter and tens of nanometers in height are commonly seen in other binders. Controversy exists regarding the chemical origin of the 'bee-structures', which has been related to the asphaltene fraction, the metal content, or the crystallizing waxes in bitumen. The rich chemistry of bitumen can result in complicated intermolecular associations such as coprecipitation of wax and metalloporphyrins in asphaltenes. Therefore, it is the molecular interactions among the different chemical components in bitumen, rather than a single chemical fraction, that are responsible for the evolution of bitumen's diverse microstructures, including the 'bee-structures'. Mechanisms such as curvature elasticity and surface wrinkling that explain the rippled structures observed in polymer crystals might be responsible for the formation of 'bee-structures' in bitumen. Despite the progress made on morphological characterization of bitumen using AFM, the fundamental question whether the microstructures observed on bitumen surfaces represent its bulk structure remains to be addressed. In addition

  19. Bulk and surface controlled diffusion of fission gas atoms

    Energy Technology Data Exchange (ETDEWEB)

    Andersson, Anders D. [Los Alamos National Laboratory

    2012-08-09

    in UO{sub 2{+-}x}, which compare favorably to available experiments. This is an extension of previous work [13]. In particular, it applies improved chemistry models for the UO{sub 2{+-}x} nonstoichiometry and its impact on the fission gas activation energies. The derivation of these models follows the approach that used in our recent study of uranium vacancy diffusion in UO{sub 2} [14]. Also, based on the calculated DFT data we analyze vacancy enhanced diffusion mechanisms in the intermediate temperature regime. In addition to vacancy enhanced diffusion we investigate species transport on the (111) UO{sub 2} surface. This is motivated by the formation of small voids partially filled with fission gas atoms (bubbles) in UO{sub 2} under irradiation, for which surface diffusion could be the rate-limiting transport step. Diffusion of such bubbles constitutes an alternative mechanism for mass transport in these materials.

  20. Dynamics of gas-surface interactions atomic-level understanding of scattering processes at surfaces

    CERN Document Server

    Díez Muniño, Ricardo

    2013-01-01

    This book gives a representative survey of the state of the art of research on gas-surface interactions. It provides an overview of the current understanding of gas surface dynamics and, in particular, of the reactive and non-reactive processes of atoms and small molecules at surfaces. Leading scientists in the field, both from the theoretical and the experimental sides, write in this book about their most recent advances. Surface science grew as an interdisciplinary research area over the last decades, mostly because of new experimental technologies (ultra-high vacuum, for instance), as well as because of a novel paradigm, the ‘surface science’ approach. The book describes the second transformation which is now taking place pushed by the availability of powerful quantum-mechanical theoretical methods implemented numerically. In the book, experiment and theory progress hand in hand with an unprecedented degree of accuracy and control. The book presents how modern surface science targets the atomic-level u...

  1. Interaction of Pd with steps on alpha-Al2O3(0001)

    DEFF Research Database (Denmark)

    Lodziana, Zbiegniew; Nørskov, Jens Kehlet

    2002-01-01

    Based on density functional calculations, we show that steps on the alpha-Al2O3 (0 0 0 1) surface are enriched in oxygen and that they bind Pd atoms and small clusters much stronger than the terraces. We also show that Pd can diffuse quite freely on an alumina surface and use this to explain why...

  2. He atom-surface scattering: Surface dynamics of insulators, overlayers and crystal growth

    International Nuclear Information System (INIS)

    1992-01-01

    Investigations in this laboratory have focused on the surface structure and dynamics of ionic insulators and on epitaxial growth onto alkali halide crystals. In the later the homoepitaxial growth of NaCl/NaCl(001) and the heteroepitaxial growth of KBr/NaCl(001), NaCl/KBr(001) and KBr/RbCl(001) have been studied by monitoring the specular He scattering as a function of the coverage and by measuring the angular and energy distributions of the scattered He atoms. These data provide information on the surface structure, defect densities, island sizes and surface strain during the layer-by-layer growth. The temperature dependence of these measurements also provides information on the mobilities of the admolecules. He atom scattering is unique among surface probes because the low-energy, inert atoms are sensitive only to the electronic structure of the topmost surface layer and are equally applicable to all crystalline materials. It is proposed for the next year to exploit further the variety of combinations possible with the alkali halides in order to carry out a definitive study of epitaxial growth in the ionic insulators. The work completed so far, including measurements of the Bragg diffraction and surface dispersion at various stages of growth, appears to be exceptionally rich in detail, which is particularly promising for theoretical modeling. In addition, because epitaxial growth conditions over a wide range of lattice mismatches is possible with these materials, size effects in growth processes can be explored in great depth. Further, as some of the alkali halides have the CsCl structure instead of the NaCl structure, we can investigate the effects of the heteroepitaxy with materials having different lattice preferences. Finally, by using co-deposition of different alkali halides, one can investigate the formation and stability of alloys and even alkali halide superlattices

  3. The effect of surface structure on Ag atom adsorption over CuO(111) surfaces: A first principles study

    Science.gov (United States)

    Hu, Riming; Zhou, Xiaolong; Yu, Jie

    2017-12-01

    The interactions of Ag atom with different types of CuO(111) surface, including the perfect, oxygen-vacancy and precovered oxygen surfaces, have been systematically investigated using density functional theory (DFT) calculations to examine the effect of surface structures on Ag atom adsorption. The calculated results indicate that the Cu1-Cu1 bridge site and the oxygen-vacancy site are the active centres for atomic Ag adsorption on the perfect surface and the oxygen-vacancy surface respectively, while atomic Ag preferentially adsorbs at the Op site on the precovered oxygen surface. The activity of the CuO(111) surface for atomic Ag adsorption can be improved both on the perfect and oxygen-vacancy surfaces, while the activity of the CuO(111) surface for atomic Ag adsorption will be suppressed on precovered oxygen surfaces. Furthermore, the adsorption of NO on different CuO(111) surfaces with Ag adsorption was investigated, and the calculation results show that the adsorption of NO on an Ag-loaded CuO(111) surface is greater than that on the pure CuO(111) surface.

  4. Double-segregation effect in AgxPd1-x/Ru(0001) thin film nanostructures

    Science.gov (United States)

    Marten, Tobias; Hellman, Olle; Ruban, Andrei V.; Olovsson, Weine; Kramer, Charlotte; Godowski, Jan P.; Bech, Lone; Li, Zheshen; Onsgaard, Jens; Abrikosov, Igor A.

    2008-03-01

    We study the structural properties of ultrathin AgxPd1-x films on top of a Ru(0001) substrate. Effective interatomic interactions, obtained from first-principles calculations, have been used in Monte Carlo simulations to derive the distribution of the alloy components in a four-monolayer (4-ML) Ag-Pd film. Though Ag-Pd alloys show complete solubility in the bulk, the thin film geometry leads to a pronounced segregation between Ag and Pd atoms with a strong preference of Ag atoms toward the surface and Pd atoms toward the interface. The theoretical prediction of this double-segregation effect is strongly supported by photoelectron spectroscopy experiments carried out for 4-ML thin films. We also show, in an additional experiment, that even in the case where initially 1 ML Ag is buried under 6 ML Pd, the whole Ag ML segregates to the surface.

  5. He-atom surface scattering apparatus for studies of crystalline surface dynamics. Progress report, May 1, 1985-April 30, 1986

    International Nuclear Information System (INIS)

    1986-01-01

    The primary goal of this grant is the construction of a state-of-the-art He atom-crystal surface scattering apparatus which will be capable of measuring both elastic and inelastic scattering of He atoms from crystal surfaces of metals, semiconductors and insulators. First, the apparatus will be constructed and characterized, after which a program of studies on the surface dynamics of a variety of crystal surfaces will be started. 6 refs., 2 figs

  6. SURFACE SITES AND MOBILITIES OF IN ATOMS ON A STEPPED CU(100) SURFACE STUDIED AT LOW COVERAGE

    NARCIS (Netherlands)

    BREEMAN, M; DORENBOS, G; BOERMA, DO

    The various surface sites of In atoms deposited to a coverage of 0.013 monolayer (ML) onto a stepped Cu(100) surface were determined with low-energy ion scattering (LEIS) as a function of deposition temperature. From the fractions of In atoms occupying different sites, observed in the temperature

  7. Characterization of the Surface Morphology of Bacillus Spores by Atomic Force Microscopy

    National Research Council Canada - National Science Library

    Zolock, Ruth

    2002-01-01

    The surface morphology of Bacillus spores was resolved by atomic force microscopy in order to determine if characteristic surface features could be used to distinguish between closely related species...

  8. Interactions of satellite-speed helium atoms with satellite-surfaces. 1. Spatial distributions of reflected helium atoms

    International Nuclear Information System (INIS)

    Liu, S.M.; Rodgers, W.E.; Knuth, E.L.

    1975-06-01

    Interactions of satellite-speed helium atoms with practical satellite surfaces were investigated experimentally, and spatial distributions of satellite-speed helium beams scattered from four different engineering surfaces were measured. The 7000-m/s helium beams were produced using an arc-heated supersonic molecular beam source. The test surfaces included cleaned 6061-T6 aluminum plate, anodized aluminum foil, white paint, and quartz surfaces. Both in-plane (in the plane containing the incident beam and the surface normal) and out-of-plane spatial distributions of reflected helium atoms were measured for six different incidence angles (0, 15, 30, 45, 60, and 75 deg from the surface normal). It was found that a large fraction of the incident helium atoms were scattered back in the vicinity of the incoming beam, particularly in the case of glancing incidence angles. This unexpected scattering feature results perhaps from the gross roughness of these test surfaces. This prominent backscattering could yield drag coefficients which are higher than for surfaces with either forward-lobed or diffusive (cosine) scattering patterns

  9. Atomic displacements and the electronic structure of the Mo(001) surface

    International Nuclear Information System (INIS)

    Inglesfield, J.E.

    1978-01-01

    The uniform surface contraction on Mo(001) and the phase transition observed below 300 K are due to the peak in the surface density of states at the Fermi energy. This is essentially a virtual bound 4d state on the surface atoms and contraction increases its interaction with the substrate and lowers the energy. The phase transition probably consists of a sideways displacement of the atoms which introduces new Brillouin zone boundaries broadening surface resonances at the Fermi energy. (author)

  10. Soft-landing ion deposition of isolated radioactive probe atoms on surfaces: A novel method

    NARCIS (Netherlands)

    Laurens, C.R; Rosu, M.F; Pleiter, F; Niesen, L

    1997-01-01

    We present a method to deposit a wide range of radioactive probe atoms on surfaces, without introducing lattice damage or contaminating the surface with other elements or isotopes. In this method, the probe atoms are mass separated using an isotope separator, decelerated to 5 eV, and directly

  11. Atoms

    International Nuclear Information System (INIS)

    Fuchs, Alain; Villani, Cedric; Guthleben, Denis; Leduc, Michele; Brenner, Anastasios; Pouthas, Joel; Perrin, Jean

    2014-01-01

    Completed by recent contributions on various topics (atoms and the Brownian motion, the career of Jean Perrin, the evolution of atomic physics since Jean Perrin, relationship between scientific atomism and philosophical atomism), this book is a reprint of a book published at the beginning of the twentieth century in which the author addressed the relationship between atomic theory and chemistry (molecules, atoms, the Avogadro hypothesis, molecule structures, solutes, upper limits of molecular quantities), molecular agitation (molecule velocity, molecule rotation or vibration, molecular free range), the Brownian motion and emulsions (history and general features, statistical equilibrium of emulsions), the laws of the Brownian motion (Einstein's theory, experimental control), fluctuations (the theory of Smoluchowski), light and quanta (black body, extension of quantum theory), the electricity atom, the atom genesis and destruction (transmutations, atom counting)

  12. Scalable synthesis of palladium nanoparticle catalysts by atomic layer deposition

    International Nuclear Information System (INIS)

    Liang Xinhua; Lyon, Lauren B.; Jiang Yingbing; Weimer, Alan W.

    2012-01-01

    Atomic layer deposition (ALD) was used to produce Pd/Al 2 O 3 catalysts using sequential exposures of Pd(II) hexafluoroacetylacetonate and formalin at 200 °C in a fluidized bed reactor. The ALD-prepared Pd/alumina catalysts were characterized by various methods including hydrogen chemisorption, XPS, and TEM, and compared with a commercially available 1 wt% Pd/alumina catalyst, which was also characterized. The content of Pd on alumina support and the size of Pd nanoparticles can be controlled by the number of ALD-coating cycles and the dose time of the Pd precursor. One layer of organic component from the Pd precursor remained on the Pd particle surface. The ALD 0.9 wt% Pd/alumina had greater active metal surface area and percent metal dispersion than the commercial 1 wt% Pd/alumina catalyst. The ALD and commercial catalysts were subjected to catalytic testing to determine their relative activities for glucose oxidation to gluconic acid in aqueous solution. The ALD 0.9 wt% Pd/alumina catalyst had comparable activity as compared to the commercial 1 wt% Pd catalyst. No noticeable amount of Pd leaching was observed for the ALD-prepared catalysts during the vigorously stirred reaction.

  13. Optimized Model Surfaces for Advanced Atomic Force Microscopy Studies of Surface Nanobubbles.

    Science.gov (United States)

    Song, Bo; Zhou, Yi; Schönherr, Holger

    2016-11-01

    The formation of self-assembled monolayers (SAMs) of binary mixtures of 16-mercaptohexadecanoic acid (MHDA) and 1-octadecanethiol (ODT) on ultraflat template-stripped gold (TSG) surfaces was systematically investigated to clarify the assembly behavior, composition, and degree of possible phase segregation in light of atomic force microscopy (AFM) studies of surface nanobubbles on these substrates. The data for SAMs on TSG were compared to those obtained by adsorption on rough evaporated gold, as reported in a previous study. Quartz crystal microbalance and surface plasmon resonance data acquired in situ on TSG indicate that similar to SAM formation on conventional evaporated gold substrates ODT and MHDA form monolayers and bilayers, respectively. The second layer on MHDA, whose formation is attributed to hydrogen bonding, can be easily removed by adequate rinsing with water. The favorable agreement of the grazing incidence reflection Fourier transform infrared (GIR FTIR) spectroscopy and contact angle data analyzed with the Israelachvili-Gee model suggests that the binary SAMs do not segregate laterally. This conclusion is fully validated by high-resolution friction force AFM observations down to a length scale of 8-10 nm, which is much smaller than the typical observed surface nanobubble radii. Finally, correspondingly functionalized TSG substrates are shown to be valuable supports for studying surface nanobubbles by AFM in water and for addressing the relation between surface functionality and nanobubble formation and properties.

  14. Sulfurization Study on the Ag and Ag-Pd Reflectors for GaN-Based LEDs

    Science.gov (United States)

    Chen, Y. H.; Liu, W. C.; Lin, Y. C.; Chung, C. C.; Zeng, W. J.; Chu, W. J.; Chung, T. Y.; Liu, C. Y.

    2016-01-01

    In this study, we have established a sulfurization resistance test, which is an immersion process in 0.01 M Na2S solution for 10 min. By using this process, we found that the sulfurized Ag reflector drops significantly over 52%. However, the Ag-Pd alloy reflector does not drop as much as the Ag reflector. The minimum reduction rate (around 20%) occurs at the Ag-Pd reflector with a Pd content of 3.72 at.%. It means that there is an optimal surface Pd content (around 3.72 at.%) for the reduction in reflectivity. Above, two effects of Pd alloying atoms on the sulfurization of the surface Ag atoms have been drawn, which are (1) chemical-state change effect and (2) surface microstructure effect. We found that the chemical-state change effect retards the sulfurization of the surface Ag atoms, but the surface microstructure effect (increase in Ag (111) plane) promotes the sulfurization of the surface Ag atoms. Here, we believe that these two opposite effects explain that there is an optimal Pd content on the Ag-Pd surface for the resistance of the sulfurization on the Ag surface.

  15. Atomic structure and surface defects at mineral-water interfaces probed by in situ atomic force microscopy

    NARCIS (Netherlands)

    Sîretanu, Igor; van den Ende, Henricus T.M.; Mugele, Friedrich Gunther

    2016-01-01

    Atomic scale details of surface structure play a crucial role for solid–liquid interfaces. While macroscopic characterization techniques provide averaged information about bulk and interfaces, high resolution real space imaging reveals unique insights into the role of defects that are believed to

  16. Trapping and stabilization of hydrogen atoms in intracrystalline voids. Defected calcium fluorides and Y zeolite surfaces

    International Nuclear Information System (INIS)

    Iton, L.E.; Turkevich, J.

    1978-01-01

    Using EPR spectroscopy, it has been established that H. atoms are absorbed from the gas phase when CaF 2 powder is exposed to H 2 gas in which a microwave discharge is sustained, being trapped in sites that provide unusual thermal stability. The disposition of the trapped atoms is determined by the occluded water content of the CaF 2 . For ultrapure CaF 2 , atoms are trapped in interstitial sites having A 0 = 1463 MHz; for increasing water content, two types of trapped H. atoms are discriminated, with preferential trapping in void sites (external to the regular fluorite lattice) that are associated with the H 2 O impurity. Characterization of these ''extra-lattice'' H. (and D.) atoms is presented, and their EPR parameters and behavior are discussed in detail. Failure to effect H.-D. atom exchange with D 2 gas suggests that atoms are not stabilized on the CaF 2 surface. H. atoms are trapped exclusively in ''extra-lattice'' sites when the water-containing CaF 2 is γ irradiated at 77 or 298 K indicating that the scission product atoms do not escape from the precursor void region into the regular lattice. It is concluded that the thermal stability of the ''extra-lattice'' atoms, like that of the interstitial atoms, is determined ultimately by the high activation energy for diffusion of the H. atom through the CaF 2 lattice. For comparison, results obtained from H. atoms trapped in γ-irradiated rare earth ion-exchanged Y zeolites are presented and discussed also; these ''surface'' trapped atoms do not exhibit great thermalstability. Distinctions in the H. atom formation mechanisms between the fluorides and the zeolites were deduced from the accompanying paramagnetic species formed. The intracavity electric fields in the Y zeolites have been estimated from the H. atoms hfsc contractions, and are found to be very high, about 1 V/A

  17. Van der Waals enhancement of optical atom potentials via resonant coupling to surface polaritons.

    Science.gov (United States)

    Kerckhoff, Joseph; Mabuchi, Hideo

    2009-08-17

    Contemporary experiments in cavity quantum electrodynamics (cavity QED) with gas-phase neutral atoms rely increasingly on laser cooling and optical, magneto-optical or magnetostatic trapping methods to provide atomic localization with sub-micron uncertainty. Difficult to achieve in free space, this goal is further frustrated by atom-surface interactions if the desired atomic placement approaches within several hundred nanometers of a solid surface, as can be the case in setups incorporating monolithic dielectric optical resonators such as microspheres, microtoroids, microdisks or photonic crystal defect cavities. Typically in such scenarios, the smallest atom-surface separation at which the van der Waals interaction can be neglected is taken to be the optimal localization point for associated trapping schemes, but this sort of conservative strategy generally compromises the achievable cavity QED coupling strength. Here we suggest a new approach to the design of optical dipole traps for atom confinement near surfaces that exploits strong surface interactions, rather than avoiding them, and present the results of a numerical study based on (39)K atoms and indium tin oxide (ITO). Our theoretical framework points to the possibility of utilizing nanopatterning methods to engineer novel modifications of atom-surface interactions. (c) 2009 Optical Society of America

  18. Atomic Ensemble and Electronic Effects in Ag-Rich AgPd Nanoalloy Catalysts for Oxygen Reduction in Alkaline Media

    OpenAIRE

    Slanac, Daniel A.; Hardin, William G.; Johnston, Keith P.; Stevenson, Keith J.

    2012-01-01

    The ability to design and characterize uniform, bimetallic alloy nanoparticles, where the less active metal enhances the activity of the more active metal, would be of broad interest in catalysis. Herein, we demonstrate that simultaneous reduction of Ag and Pd precursors provides uniform, Ag-rich AgPd alloy nanoparticles (~5 nm) with high activities for the oxygen reduction reaction (ORR) in alkaline media. The particles are crystalline and uniformly alloyed, as shown by X-ray diffraction and...

  19. Adsorption of oxygen atom on MoSi{sub 2} (110) surface

    Energy Technology Data Exchange (ETDEWEB)

    Sun, S.P., E-mail: sunshunping@jsut.edu.cn [School of Materials Engineering, Jiangsu University of Technology, Changzhou 213001 (China); Li, X.P.; Wang, H.J. [School of Materials Engineering, Jiangsu University of Technology, Changzhou 213001 (China); Jiang, Y., E-mail: yjiang@csu.edu.cn [School of Materials Science and Engineering, and Key Laboratory for Non-ferrous Materials of Ministry of Education, Central South University, Changsha 410083 (China); Yi, D.Q. [School of Materials Science and Engineering, and Key Laboratory for Non-ferrous Materials of Ministry of Education, Central South University, Changsha 410083 (China)

    2016-09-30

    Highlights: • The adsorption of oxygen atom on MoSi{sub 2} (110) surface was studied systematically. • The stability of MoSi{sub 2} low-index surfaces was also investigated. • The preference adsorption site of MoSi{sub 2} (110) surface for oxygen atom was H site. - Abstract: The adsorption energy, structural relaxation and electronic properties of oxygen atom on MoSi{sub 2} (110) surface have been investigated by first-principles calculations. The energetic stability of MoSi{sub 2} low-index surfaces was analyzed, and the results suggested that MoSi{sub 2} (110) surface had energetically stability. The site of oxygen atom adsorbed on MoSi{sub 2} (110) surface were discussed, and the results indicated that the preference adsorption site of MoSi{sub 2} (110) surface for oxygen atom was H site (hollow position). Our calculated work should help to understand further the interaction between oxygen atoms and MoSi{sub 2} surfaces.

  20. Transition metal atoms pathways on rutile TiO2 (110) surface: Distribution of Ti3+ states and evidence of enhanced peripheral charge accumulation

    Science.gov (United States)

    Cai, Yongqing; Bai, Zhaoqiang; Chintalapati, Sandhya; Zeng, Qingfeng; Feng, Yuan Ping

    2013-04-01

    Charge transfer between metal nanoparticles and the supported TiO2 surface is primarily important for catalytic applications as it greatly affects the catalytic activity and the thermal stability of the deposited nanoparticles on the surface. Herein, systematic spin-polarized density functional and HSE06 calculations are performed to evaluate the adsorption, diffusion, and charge state of several transition metal monomers on both stoichiometric and reduced rutile TiO2 (110) surface. Although the presence of oxygen vacancy (Ov) increases the binding of Au, Pt and Pd on the surface, it weakens the interaction thus enhancing the diffusion for Fe, Co, Ni, Ag, and Cu adatoms on the surface. For pristine reduced surface, only a small portion (around 5%) of the excess electrons occupy the topmost surface, which are mainly delocalized at the second nearest and third nearest fivefold coordinated Ti (Ti5c) atoms. Excess electrons populating at the Ti5c atoms on the basal plane can be transferred to strongly electronegative adsorbates like Au and Pt thus enabling a moderate adsorption at this site, whereas no stable adsorption is found for other less electronegative transition metal adatoms (Ag, Cu, Fe, Co, Ni, and Pd) on the reduced surface and for all the adatoms on stoichiometric surface. This result clarifies the origin of the experimental observation of the adsorption of O2 and CO molecules at Ti5c sites in connection with charge transfer. In addition, the spatial redistribution of the excess electrons around the Ov upon the adsorption of the monomers is thoroughly examined. Our finding of an accumulation of excess electrons at the Ti5c sites around the monomers explains the critical role of the perimeter interface of the deposited nanoparticles in promoting the adsorption and activation of reactants observed in experiments.

  1. Formation and structural phase transition in Co atomic chains on a Cu(775) surface

    International Nuclear Information System (INIS)

    Syromyatnikov, A. G.; Kabanov, N. S.; Saletsky, A. M.; Klavsyuk, A. L.

    2017-01-01

    The formation of Co atomic chains on a Cu(775) surface is investigated by the kinetic Monte Carlo method. It is found that the length of Co atomic chains formed as a result of self-organization during epitaxial growth is a random quantity and its mean value depends on the parameters of the experiment. The existence of two structural phases in atomic chains is detected using the density functional theory. In the first phase, the separations between an atom and its two nearest neighbors in a chain are 0.230 and 0.280 nm. In the second phase, an atomic chain has identical atomic spacings of 0.255 nm. It is shown that the temperature of the structural phase transition depends on the length of the atomic chain.

  2. Surface atomic relaxation and magnetism on hydrogen-adsorbed Fe(110) surfaces from first principles

    Energy Technology Data Exchange (ETDEWEB)

    Chohan, Urslaan K.; Jimenez-Melero, Enrique [School of Materials, The University of Manchester, Manchester M13 9PL (United Kingdom); Dalton Cumbrian Facility, The University of Manchester, Moor Row CA24 3HA (United Kingdom); Koehler, Sven P.K., E-mail: sven.koehler@manchester.ac.uk [Dalton Cumbrian Facility, The University of Manchester, Moor Row CA24 3HA (United Kingdom); School of Chemistry, The University of Manchester, Manchester M13 9PL (United Kingdom); Photon Science Institute, The University of Manchester, Manchester M13 9PL (United Kingdom)

    2016-11-30

    Highlights: • Potential energy surfaces for H diffusion on Fe(110) calculated. • Full vibrational analysis of surface modes performed. • Vibrational analysis establishes lb site as a transition state to the 3f site. • Pronounced buckling observed in the Fe surface layer. - Abstract: We have computed adsorption energies, vibrational frequencies, surface relaxation and buckling for hydrogen adsorbed on a body-centred-cubic Fe(110) surface as a function of the degree of H coverage. This adsorption system is important in a variety of technological processes such as the hydrogen embrittlement in ferritic steels, which motivated this work, and the Haber–Bosch process. We employed spin-polarised density functional theory to optimise geometries of a six-layer Fe slab, followed by frozen mode finite displacement phonon calculations to compute Fe–H vibrational frequencies. We have found that the quasi-threefold (3f) site is the most stable adsorption site, with adsorption energies of ∼3.0 eV/H for all coverages studied. The long-bridge (lb) site, which is close in energy to the 3f site, is actually a transition state leading to the stable 3f site. The calculated harmonic vibrational frequencies collectively span from 730 to 1220 cm{sup −1}, for a range of coverages. The increased first-to-second layer spacing in the presence of adsorbed hydrogen, and the pronounced buckling observed in the Fe surface layer, may facilitate the diffusion of hydrogen atoms into the bulk, and therefore impact the early stages of hydrogen embrittlement in steels.

  3. An x-ray diffraction study of interface roughness and diffusion in Ag/Pd superlattices

    NARCIS (Netherlands)

    Temst, K.; van Bael, M.J.; van Haesendonck, Ch.; Bruynseraede, Y.; de Groot, D.G.; Koeman, N.J.; Griessen, R.P.

    1999-01-01

    The influence of thermal annealing on the surface and interface roughness of epitaxial Ag/Pd superlattices has been quantitatively characterized by high-angle X-ray diffraction and atomic force microscopy. Although Ag and Pd form a continuous series of solid solutions, it is shown that thermal

  4. Improving electromechanical output of IPMC by high surface area Pd-Pt electrodes and tailored ionomer membrane thickness

    Directory of Open Access Journals (Sweden)

    Viljar Palmre

    2014-04-01

    Full Text Available In this study, we attempt to improve the electromechanical performance of ionic polymer–metal composites (IPMCs by developing high surface area Pd-Pt electrodes and tailoring the ionomer membrane thickness. With proper electroless plating techniques, a high dispersion of palladium particles is achieved deep in the ionomer membrane, thereby increasing notably the interfacial surface area of electrodes. The membrane thickness is increased using 0.5 and 1 mm thick ionomer films. For comparison, IPMCs with the same ionomer membranes, but conventional Pt electrodes, are also prepared and studied. The electromechanical, mechanoelectrical, electrochemical and mechanical properties of different IPMCs are characterized and discussed. Scanning electron microscopy-energy dispersive X-ray (SEM-EDS is used to investigate the distribution of deposited electrode metals in the cross section of Pd-Pt IPMCs. Our experiments demonstrate that IPMCs assembled with millimeter thick ionomer membranes and newly developed Pd-Pt electrodes are superior in mechanoelectrical transduction, and show significantly higher blocking force compared to conventional type of IPMCs. The blocking forces of more than 0.3 N were measured at 4V DC input, exceeding the force output of typical Nafion® 117-based Pt IPMCs more than two orders of magnitude. The newly designed Pd-Pt IPMCs can be useful in more demanding applications, e.g., in biomimetic underwater robotics, where high stress and drag forces are encountered.

  5. Relativistic Band Structure and Fermi Surface of PdTe2 by the LMTO Method

    DEFF Research Database (Denmark)

    Jan, J. P.; Skriver, Hans Lomholt

    1977-01-01

    The energy bands of the trigonal layer compound PdTe2 have been calculated, using the relativistic linear muffin-tin orbitals method. The bandstructure is separated into three distinct regions with low-lying Te 5s bands, conduction bands formed by Pd 4d and Te 5p states, and high-lying bands formed...

  6. The calculation of surface free energy based on embedded atom method for solid nickel

    International Nuclear Information System (INIS)

    Luo Wenhua; Hu Wangyu; Su Kalin; Liu Fusheng

    2013-01-01

    Highlights: ► A new solution for accurate prediction of surface free energy based on embedded atom method was proposed. ► The temperature dependent anisotropic surface energy of solid nickel was obtained. ► In isotropic environment, the approach does not change most predictions of bulk material properties. - Abstract: Accurate prediction of surface free energy of crystalline metals is a challenging task. The theory calculations based on embedded atom method potentials often underestimate surface free energy of metals. With an analytical charge density correction to the argument of the embedding energy of embedded atom method, an approach to improve the prediction for surface free energy is presented. This approach is applied to calculate the temperature dependent anisotropic surface energy of bulk nickel and surface energies of nickel nanoparticles, and the obtained results are in good agreement with available experimental data.

  7. An Analytical Model for Adsorption and Diffusion of Atoms/Ions on Graphene Surface

    Directory of Open Access Journals (Sweden)

    Yan-Zi Yu

    2015-01-01

    Full Text Available Theoretical investigations are made on adsorption and diffusion of atoms/ions on graphene surface based on an analytical continuous model. An atom/ion interacts with every carbon atom of graphene through a pairwise potential which can be approximated by the Lennard-Jones (L-J potential. Using the Fourier expansion of the interaction potential, the total interaction energy between the adsorption atom/ion and a monolayer graphene is derived. The energy-distance relationships in the normal and lateral directions for varied atoms/ions, including gold atom (Au, platinum atom (Pt, manganese ion (Mn2+, sodium ion (Na1+, and lithium-ion (Li1+, on monolayer graphene surface are analyzed. The equilibrium position and binding energy of the atoms/ions at three particular adsorption sites (hollow, bridge, and top are calculated, and the adsorption stability is discussed. The results show that H-site is the most stable adsorption site, which is in agreement with the results of other literatures. What is more, the periodic interaction energy and interaction forces of lithium-ion diffusing along specific paths on graphene surface are also obtained and analyzed. The minimum energy barrier for diffusion is calculated. The possible applications of present study include drug delivery system (DDS, atomic scale friction, rechargeable lithium-ion graphene battery, and energy storage in carbon materials.

  8. Atomic and electronic structures of novel silicon surface structures

    Energy Technology Data Exchange (ETDEWEB)

    Terry, J.H. Jr.

    1997-03-01

    The modification of silicon surfaces is presently of great interest to the semiconductor device community. Three distinct areas are the subject of inquiry: first, modification of the silicon electronic structure; second, passivation of the silicon surface; and third, functionalization of the silicon surface. It is believed that surface modification of these types will lead to useful electronic devices by pairing these modified surfaces with traditional silicon device technology. Therefore, silicon wafers with modified electronic structure (light-emitting porous silicon), passivated surfaces (H-Si(111), Cl-Si(111), Alkyl-Si(111)), and functionalized surfaces (Alkyl-Si(111)) have been studied in order to determine the fundamental properties of surface geometry and electronic structure using synchrotron radiation-based techniques.

  9. Surface structure of polymers and their model compounds observed by atomic force microscopy

    NARCIS (Netherlands)

    Stocker, W.; Bickmann, B.; Magonov, S.N.; Cantow, H.J.; Lotz, B.; Wittmann, J.C.; Moller, M.; Möller, M.

    1992-01-01

    Results of atomic force microscopy (AFM) of normal alkanes, polyethylene, isotactic polypropylene and of a diblock copolymer are presented. Various types of surfaces - naturally and epitaxially grown on different substrates - have been examined from hundreds of nanometers down to the atomic scale.

  10. Noncontact AFM Imaging of Atomic Defects on the Rutile TiO2 (110) Surface

    DEFF Research Database (Denmark)

    Lauritsen, Jeppe Vang

    2015-01-01

    The atomic force microscope (AFM) operated in the noncontact mode (nc-AFM) offers a unique tool for real space, atomic-scale characterisation of point defects and molecules on surfaces, irrespective of the substrate being electrically conducting or non-conducting. The nc-AFM has therefore in rece...

  11. Direct determination of phosphorus in different food samples by means of solid sampling electrothermal atomic absorption spectrometry using Pd+Ca chemical modifier

    Energy Technology Data Exchange (ETDEWEB)

    Coskun, Nihat [Department of Chemistry, Istanbul Technical University, Science and Letter Faculty, 34469 Maslak, Istanbul (Turkey); Akman, Sueleyman [Department of Chemistry, Istanbul Technical University, Science and Letter Faculty, 34469 Maslak, Istanbul (Turkey)]. E-mail: akmans@itu.edu.tr

    2005-03-31

    In this study, direct determination of phosphorus in different food samples (milk powder, banana, and dried banana) and in various standard reference materials (apple leaves, bovine liver, pine needles) using solid sampling electrothermal atomic absorption spectrometry was investigated. Aqueous standards were used for all determinations. 5 {mu}g Pd+5 {mu}g Ca modifier mixture was used in all experiments. Pyrolysis temperature and atomization temperature were 1100 deg. C and 2500 deg. C, respectively. High background was reduced by applying a cool-down step in the furnace program. The accuracy of solid sampling results was checked by determination of the phosphorus content after dissolving samples. There was no significant error between results found by solid sampling and solution techniques. In addition solid certified materials were investigated. There were no significant differences between the phosphorus content of CRM and results obtained. The limit of detection, based on three times the standard deviation was 0.018 {mu}g P.

  12. Surface atomic relaxation and magnetism on hydrogen-adsorbed Fe(110) surfaces from first principles

    Science.gov (United States)

    Chohan, Urslaan K.; Jimenez-Melero, Enrique; Koehler, Sven P. K.

    2016-11-01

    We have computed adsorption energies, vibrational frequencies, surface relaxation and buckling for hydrogen adsorbed on a body-centred-cubic Fe(110) surface as a function of the degree of H coverage. This adsorption system is important in a variety of technological processes such as the hydrogen embrittlement in ferritic steels, which motivated this work, and the Haber-Bosch process. We employed spin-polarised density functional theory to optimise geometries of a six-layer Fe slab, followed by frozen mode finite displacement phonon calculations to compute Fe-H vibrational frequencies. We have found that the quasi-threefold (3f) site is the most stable adsorption site, with adsorption energies of ∼3.0 eV/H for all coverages studied. The long-bridge (lb) site, which is close in energy to the 3f site, is actually a transition state leading to the stable 3f site. The calculated harmonic vibrational frequencies collectively span from 730 to 1220 cm-1, for a range of coverages. The increased first-to-second layer spacing in the presence of adsorbed hydrogen, and the pronounced buckling observed in the Fe surface layer, may facilitate the diffusion of hydrogen atoms into the bulk, and therefore impact the early stages of hydrogen embrittlement in steels.

  13. Atomic species recognition on oxide surfaces using low temperature scanning probe microscopy

    Energy Technology Data Exchange (ETDEWEB)

    Ma, Zong Min, E-mail: mzmncit@163.com [National Key Laboratory for Electronic Measurement Technology, North University of China, Taiyuan, 030051 (China); Key Laboratory of Instrumentation Science & Dynamic Measurement, North University of China, Ministry of Education, Taiyuan, 030051 (China); School of Instrument and Electronics, North University of China, Taiyuan, 030051 (China); Shi, Yun Bo; Mu, Ji Liang; Qu, Zhang; Zhang, Xiao Ming; Qin, Li [National Key Laboratory for Electronic Measurement Technology, North University of China, Taiyuan, 030051 (China); Key Laboratory of Instrumentation Science & Dynamic Measurement, North University of China, Ministry of Education, Taiyuan, 030051 (China); School of Instrument and Electronics, North University of China, Taiyuan, 030051 (China); Liu, Jun, E-mail: liuj@nuc.edu.cn [National Key Laboratory for Electronic Measurement Technology, North University of China, Taiyuan, 030051 (China); Key Laboratory of Instrumentation Science & Dynamic Measurement, North University of China, Ministry of Education, Taiyuan, 030051 (China); School of Instrument and Electronics, North University of China, Taiyuan, 030051 (China)

    2017-02-01

    Highlights: • The coexisted phase of p(2 × 1)and c(6 × 2) on Cu(110)-O surface using AFM under UHV at low temperature. • Two different c(6 × 2) phase depending on the status of the tip apex. • Electronic state of tip seriously effect the resolution and stability of the sample surface. - Abstract: In scanning probe microscopy (SPM), the chemical properties and sharpness of the tips of the cantilever greatly influence the scanning of a sample surface. Variation in the chemical properties of the sharp tip apex can induce transformation of the SPM images. In this research, we explore the relationship between the tip and the structure of a sample surface using dynamic atomic force microscopy (AFM) on a Cu(110)-O surface under ultra-high vacuum (UHV) at low temperature (78 K). We observed two different c(6 × 2) phase types in which super-Cu atoms show as a bright spot when the tip apex is of O atoms and O atoms show as a bright spot when the tip apex is of Cu atoms. We also found that the electronic state of the tip has a serious effect on the resolution and stability of the sample surface, and provide an explanation for these phenomena. This technique can be used to identify atom species on sample surfaces, and represents an important development in the SPM technique.

  14. Atomic structure of the SnO{sub 2} (110) surface

    Energy Technology Data Exchange (ETDEWEB)

    Godin, T.J.; LaFemina, J.P.

    1991-12-01

    Using a tight-binding, total-energy model, we examine atomic relaxations of the ideal stoichiometric and reduced tin oxide (11) surfaces. In both cases we find a nearly bond-length conserving rumple of the top layer, and a smaller counter-relaxation of the second layer. These calculations show no evidence of surface states in the band gap for either surface.

  15. Atomic structure of the SnO sub 2 (110) surface

    Energy Technology Data Exchange (ETDEWEB)

    Godin, T.J.; LaFemina, J.P.

    1991-12-01

    Using a tight-binding, total-energy model, we examine atomic relaxations of the ideal stoichiometric and reduced tin oxide (11) surfaces. In both cases we find a nearly bond-length conserving rumple of the top layer, and a smaller counter-relaxation of the second layer. These calculations show no evidence of surface states in the band gap for either surface.

  16. Surface-initiated Atom Transfer Radical Polymerization - a Technique to Develop Biofunctional Coatings

    DEFF Research Database (Denmark)

    Fristrup, Charlotte Juel; Jankova Atanasova, Katja; Hvilsted, Søren

    2009-01-01

    The initial formation of initiating sites for atom transfer radical polymerization (ATRP) on various polymer surfaces and numerous inorganic and metallic surfaces is elaborated. The subsequent ATRP grafting of a multitude of monomers from such surfaces to generate thin covalently linked polymer...

  17. Refined potentials for rare gas atom adsorption on rare gas and alkali-halide surfaces

    Science.gov (United States)

    Wilson, J. W.; Heinbockel, J. H.; Outlaw, R. A.

    1985-01-01

    The utilization of models of interatomic potential for physical interaction to estimate the long range attractive potential for rare gases and ions is discussed. The long range attractive force is calculated in terms of the atomic dispersion properties. A data base of atomic dispersion parameters for rare gas atoms, alkali ion, and halogen ions is applied to the study of the repulsive core; the procedure for evaluating the repulsive core of ion interactions is described. The interaction of rare gas atoms on ideal rare gas solid and alkali-halide surfaces is analyzed; zero coverage absorption potentials are derived.

  18. Calculations of Trapping and Desorption in Heavy Atom Collisions with Surfaces

    OpenAIRE

    Fan, Guoqing; Manson, J. R.

    2008-01-01

    Calculations are carried out for the scattering of heavy rare gas atoms with surfaces using a recently developed classical theory that can track particles trapped in the physisorption potential well and follow them until ultimate desorption. Comparisons are made with recent experimental data for xenon scattering from molten gallium and indium, systems for which the rare gas is heavier than the surface atoms. The good agreement with the data obtained for both time-of-flight energy-resolved spe...

  19. An important atomic process in the CVD growth of graphene: Sinking and up-floating of carbon atom on copper surface

    International Nuclear Information System (INIS)

    Li, Yingfeng; Li, Meicheng; Gu, TianSheng; Bai, Fan; Yu, Yue; Trevor, Mwenya; Yu, Yangxin

    2013-01-01

    By density functional theory (DFT) calculations, the early stages of the growth of graphene on copper (1 1 1) surface are investigated. At the very first time of graphene growth, the carbon atom sinks into subsurface. As more carbon atoms are adsorbed nearby the site, the sunken carbon atom will spontaneously form a dimer with one of the newly adsorbed carbon atoms, and the formed dimer will up-float on the top of the surface. We emphasize the role of the co-operative relaxation of the co-adsorbed carbon atoms in facilitating the sinking and up-floating of carbon atoms. In detail: when two carbon atoms are co-adsorbed, their co-operative relaxation will result in different carbon–copper interactions for the co-adsorbed carbon atoms. This difference facilitates the sinking of a single carbon atom into the subsurface. As a third carbon atom is co-adsorbed nearby, it draws the sunken carbon atom on top of the surface, forming a dimer. Co-operative relaxations of the surface involving all adsorbed carbon atoms and their copper neighbors facilitate these sinking and up-floating processes. This investigation is helpful for the deeper understanding of graphene synthesis and the choosing of optimal carbon sources or process.

  20. On-surface manipulation of atom substitution between cobalt phthalocyanine and the Cu(111) substrate

    DEFF Research Database (Denmark)

    Shen, Kongchao; Narsu, Bai; Ji, Gengwu

    2017-01-01

    (DFT). Interestingly, the scenario of atom exchange is discovered at the interface at room temperature (RT), namely the substitution of the cobalt atom in CoPc by a surface Cu adatom. Moreover, thermal annealing enhances the substitution process considerably which is demonstrated to be complete...... at about 573 K. As revealed by DFT calculations, the driving force for the observed interface transmetalation is most probably provided by the initial strong molecular-substrate interaction between Co atoms and the Cu(111) surface, the external thermodynamic energy gained from thermal sublimation...

  1. Magnetic character of holmium atom adsorbed on platinum surface

    Czech Academy of Sciences Publication Activity Database

    Shick, Alexander; Shapiro, D.S.; Kolorenč, Jindřich; Lichtenstein, A.I.

    2017-01-01

    Roč. 7, č. 1 (2017), s. 1-6, č. článku 2751. ISSN 2045-2322 R&D Projects: GA ČR GC15-05872J Grant - others:GA MŠk(CZ) LM2015042 Institutional support: RVO:68378271 Keywords : rare-earth adatoms * density-functional theory * single- atom magnets Subject RIV: BM - Solid Matter Physics ; Magnetism OBOR OECD: Condensed matter physics (including formerly solid state physics, supercond.) Impact factor: 4.259, year: 2016

  2. Characterizing the collision of potassium atoms with a siloxane coated glass surface using spectroscopic methods

    Science.gov (United States)

    Morgus, Tyler Christophe

    2001-07-01

    We have developed a series of three experiments to characterize the collisions between potassium atoms and a siloxane coated non-stick surface on a glass substrate. The first experiment looks at the aggregate effect of multiple collisions of the potassium atoms with the surface. The atoms are observed spectroscopically. The spectroscopic information allows for the calculation of the flux, average velocity, and density of the potassium atoms. These quantities are also calculated with a computer model. The parameters of the model are the probability that a potassium atom will stick to the surface during a collision, and the probabilities that the collision is specular or diffuse. The second experiment uses the photo-desorption effect to create a spatially peaked non-equilibrium density distribution. The rate of decay of this distribution is fit with a computer model whose free parameter is proportional to the probability that an atom will stick to the siloxane coated wall during a collision. The third experiment is designed to observe the results of a single collision with a siloxane coated surface. Again, the potassium atoms are observed spectroscopically, the Doppler effect providing velocity resolution. The intensity of the fluorescence is related to the velocity-density distribution. The density is then theoretically modeled using the same simple kernel, accounting for contributions to the density from the potassium source, specular collisions, and diffuse collisions.

  3. Tailoring optical metamaterials to tune the atom-surface Casimir-Polder interaction.

    Science.gov (United States)

    Chan, Eng Aik; Aljunid, Syed Abdullah; Adamo, Giorgio; Laliotis, Athanasios; Ducloy, Martial; Wilkowski, David

    2018-02-01

    Metamaterials are fascinating tools that can structure not only surface plasmons and electromagnetic waves but also electromagnetic vacuum fluctuations. The possibility of shaping the quantum vacuum is a powerful concept that ultimately allows engineering the interaction between macroscopic surfaces and quantum emitters such as atoms, molecules, or quantum dots. The long-range atom-surface interaction, known as Casimir-Polder interaction, is of fundamental importance in quantum electrodynamics but also attracts a significant interest for platforms that interface atoms with nanophotonic devices. We perform a spectroscopic selective reflection measurement of the Casimir-Polder interaction between a Cs(6P 3/2 ) atom and a nanostructured metallic planar metamaterial. We show that by engineering the near-field plasmonic resonances of the metamaterial, we can successfully tune the Casimir-Polder interaction, demonstrating both a strong enhancement and reduction with respect to its nonresonant value. We also show an enhancement of the atomic spontaneous emission rate due to its coupling with the evanescent modes of the nanostructure. Probing excited-state atoms next to nontrivial tailored surfaces is a rigorous test of quantum electrodynamics. Engineering Casimir-Polder interactions represents a significant step toward atom trapping in the extreme near field, possibly without the use of external fields.

  4. Adsorption of atomic nitrogen and oxygen on [Formula: see text] surface: a density functional theory study.

    Science.gov (United States)

    Breedon, M; Spencer, M J S; Yarovsky, I

    2009-04-08

    The adsorption of atomic nitrogen and oxygen on the ([Formula: see text]) crystal face of zinc oxide (ZnO) was studied. Binding energies, workfunction changes, vibrational frequencies, charge density differences and electron localization functions were calculated. It was elucidated that atomic oxygen binds more strongly than nitrogen, with the most stable [Formula: see text] structure exhibiting a binding energy of -2.47 eV, indicating chemisorption onto the surface. Surface reconstructions were observed for the most stable minima of both atomic species. Positive workfunction changes were calculated for both adsorbed oxygen and nitrogen if the adsorbate interacted with zinc atoms. Negative workfunction changes were calculated when the adsorbate interacted with both surface oxygen and zinc atoms. Interactions between the adsorbate and the surface zinc atoms resulted in ionic-type bonding, whereas interactions with oxygen atoms were more likely to result in the formation of covalent-type bonding. The positive workfunction changes correlate with an experimentally observed increase in resistance of ZnO conductometric sensor devices.

  5. The impact of atomization on the surface composition of spray-dried milk droplets.

    Science.gov (United States)

    Foerster, Martin; Gengenbach, Thomas; Woo, Meng Wai; Selomulya, Cordelia

    2016-04-01

    The dominant presence of fat at the surface of spray-dried milk powders has been widely reported in the literature and described as resulting in unfavourable powder properties. The mechanism(s) causing this phenomenon are yet to be clearly identified. A systematic investigation of the component distribution in atomized droplets and spray-dried particles consisting of model milk systems with different fat contents demonstrated that atomization strongly influences the final surface composition. Cryogenic flash-freezing of uniform droplets from a microfluidic jet nozzle directly after atomization helped to distinguish the influence of the atomization stage from the drying stage. It was confirmed that the overrepresentation of fat on the surface is independent of the atomization technique, including a pressure-swirl single-fluid spray nozzle and a pilot-scale rotary disk spray dryer commonly used in industry. It is proposed that during the atomization stage a disintegration mechanism along the oil-water interface of the fat globules causes the surface predominance of fat. X-ray photoelectron spectroscopic measurements detected the outermost fat layer and some adjacent protein present on both atomized droplets and spray-dried particles. Confocal laser scanning microscopy gave a qualitative insight into the protein and fat distribution throughout the cross-sections, and confirmed the presence of a fat film along the particle surface. The film remained on the surface in the subsequent drying stage, while protein accumulated underneath, driven by diffusion. The results demonstrated that atomization induces component segregation and fat-rich surfaces in spray-dried milk powders, and thus these cannot be prevented by adjusting the spray drying conditions. Copyright © 2016 Elsevier B.V. All rights reserved.

  6. Stripping scattering of fast atoms on surfaces of metal-oxide crystals and ultrathin films

    International Nuclear Information System (INIS)

    Blauth, David

    2010-01-01

    In the framework of the present dissertation the interactions of fast atoms with surfaces of bulk oxides, metals and thin films on metals were studied. The experiments were performed in the regime of grazing incidence of atoms with energies of some keV. The advantage of this scattering geometry is the high surface sensibility and thus the possibility to determine the crystallographic and electronic characteristics of the topmost surface layer. In addition to these experiments, the energy loss and the electron emission induced by scattered projectiles was investigated. The energy for electron emission and exciton excitation on Alumina/NiAl(110) and SiO 2 /Mo(112) are determined. By detection of the number of projectile induced emitted electrons as function of azimuthal angle for the rotation of the target surface, the geometrical structure of atoms forming the topmost layer of different adsorbate films on metal surfaces where determined via ion beam triangulation. (orig.)

  7. Scattering of atomic and molecular ions from single crystal surfaces of Cu, Ag and Fe

    International Nuclear Information System (INIS)

    Zoest, J.M. van.

    1986-01-01

    This thesis deals with analysis of crystal surfaces of Cu, Ag and Fe with Low Energy Ion scattering Spectroscopy (LEIS). Different atomic and molecular ions with fixed energies below 7 keV are scattered by a metal single crystal (with adsorbates). The energy and direction of the scattered particles are analysed for different selected charge states. In that way information can be obtained concerning the composition and atomic and electronic structure of the single crystal surface. Energy spectra contain information on the composition of the surface, while structural atomic information is obtained by direction measurements (photograms). In Ch.1 a description is given of the experimental equipment, in Ch.2 a characterization of the LEIS method. Ch.3 deals with the neutralization of keV-ions in surface scattering. Two different ways of data interpretation are presented. First a model is treated in which the observed directional dependence of neutralization action of the first atom layer of the surface is presented by a laterally varying thickness of the neutralizing layer. Secondly it is shown that the data can be reproduced by a more realistic, physical model based on atomic transition matrix elements. In Ch.4 the low energy hydrogen scattering is described. The study of the dissociation of H 2 + at an Ag surface r0230ted in a model based on electronic dissociation, initialized by electron capture into a repulsive (molecular) state. In Ch.5 finally the method is applied to the investigation of the surface structure of oxidized Fe. (Auth.)

  8. Nonperturbative theory of atom-surface interaction: corrections at short separations.

    Science.gov (United States)

    Bordag, M; Klimchitskaya, G L; Mostepanenko, V M

    2018-02-07

    The nonperturbative expressions for the free energy and force of interaction between a ground-state atom and a real-material surface at any temperature are presented. The transition to the Matsubara representation is performed, whereupon the comparison is made with the commonly used perturbative results based on the standard Lifshitz theory. It is shown that the Lifshitz formulas for the free energy and force of an atom-surface interaction follow from the nonperturbative ones in the lowest order of the small parameter. Numerical computations of the free energy and force for the atoms of He[Formula: see text] and Na interacting with a surface of an Au plate have been performed using the frequency-dependent dielectric permittivity of Au and highly accurate dynamic atomic polarizabilities in the framework of both the nonperturbative and perturbative theories. According to our results, the maximum deviations between the two theories are reached at the shortest atom-surface separations of about 1 nm. Simple analytic expressions for the atom-surface free energy are derived in the classical limit and for an ideal-metal plane. In the lowest order of the small parameter, they are found in agreement with the perturbative ones following from the standard Lifshitz theory. Possible applications of the obtained results in the theory of van der Waals adsorption are discussed.

  9. Surface Magnetism of Cobalt Nanoislands Controlled by Atomic Hydrogen.

    Science.gov (United States)

    Park, Jewook; Park, Changwon; Yoon, Mina; Li, An-Ping

    2017-01-11

    Controlling the spin states of the surface and interface is key to spintronic applications of magnetic materials. Here, we report the evolution of surface magnetism of Co nanoislands on Cu(111) upon hydrogen adsorption and desorption with the hope of realizing reversible control of spin-dependent tunneling. Spin-polarized scanning tunneling microscopy reveals three types of hydrogen-induced surface superstructures, 1H-(2 × 2), 2H-(2 × 2), and 6H-(3 × 3), with increasing H coverage. The prominent magnetic surface states of Co, while being preserved at low H coverage, become suppressed as the H coverage level increases, which can then be recovered by H desorption. First-principles calculations reveal the origin of the observed magnetic surface states by capturing the asymmetry between the spin-polarized surface states and identify the role of hydrogen in controlling the magnetic states. Our study offers new insights into the chemical control of magnetism in low-dimensional systems.

  10. Liquid Atomization Induced by Pulse Laser Reflection underneath Liquid Surface

    Science.gov (United States)

    Utsunomiya, Yuji; Kajiwara, Takashi; Nishiyama, Takashi; Nagayama, Kunihito; Kubota, Shiro; Nakahara, Motonao

    2009-05-01

    We observed a novel effect of pulse laser reflection at the interface between transparent materials with different refractive indices. The electric field intensity doubles when a laser beam is completely reflected from a material with a higher refractive index to a material with a lower index. This effect appreciably reduces pulse laser ablation threshold of transparent materials. We performed experiments to observe the entire ablation process for laser incidence on the water-air interface using pulse laser shadowgraphy with high-resolution film; the minimum laser fluence for laser ablation at the water-air interface was approximately 12-16 J/cm2. We confirmed that this laser ablation occurs only when the laser beam is incident on the water-air interface from water. Many slender liquid ligaments extend like a milk crown and seem to be atomized at the tip. Their detailed structures can be resolved only by pulse laser photography using high-resolution film.

  11. Davisson-Germer Prize in Atomic or Surface Physics Lecture: Exploring Flatland with Cold Atoms

    Science.gov (United States)

    Dalibard, Jean

    2012-06-01

    A two-dimensional Bose fluid is a remarkably rich many-body system, which allows one to revisit several features of quantum statistical physics. Firstly, the role of thermal fluctuations is enhanced compared to the 3D case, which destroys the ordered state associated with Bose-Einstein condensation. However interactions between particles can still cause a superfluid transition, thanks to the Berezinskii-Kosterlitz-Thouless mechanism. Secondly, a weakly interacting Bose fluid in 2D must be scale-invariant, a remarkable feature that manifests itself in the very simple form taken by the equation of state of the fluid. In this talk I will present recent experimental progress in the investigation of 2D atomic gases, which provide a nice illustration of the main features of low dimensional many-body physics.

  12. The effect of microemulsion composition on the morphology of Pd nanoparticles deposited at the surface of TiO{sub 2} and photoactivity of Pd-TiO{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Długokęcka, Marta [Faculty of Chemistry, Gdańsk University of Technology, ul. G. Narutowicza 11/12, 80-233 Gdansk (Poland); Łuczak, Justyna, E-mail: justyna.luczak@pg.gda.pl [Faculty of Chemistry, Gdańsk University of Technology, ul. G. Narutowicza 11/12, 80-233 Gdansk (Poland); Polkowska, Żaneta [Faculty of Chemistry, Gdańsk University of Technology, ul. G. Narutowicza 11/12, 80-233 Gdansk (Poland); Zaleska-Medynska, Adriana, E-mail: adriana.zaleska@ug.edu.pl [Faculty of Chemistry, Gdańsk University of Technology, ul. G. Narutowicza 11/12, 80-233 Gdansk (Poland); Faculty of Chemistry, University of Gdansk, ul. Wita Stwosza 63, 80-308 Gdansk (Poland)

    2017-05-31

    Highlights: • Pd was deposited on TiO{sub 2} surface via microemulsion route (water-to-cyclohexane system). • Reaction parameters influencing the size distribution of Pd nanoparticles was investigated. • Photocatalytic activity was maximized at average droplet size of 2.83 ± 0.18 nm. • Superoxide radical was the dominant oxidizing species in the phenol degradation. - Abstract: A series of microemulsion (ME) system, constituted by different water to surfactant molar ratios (W{sub o}) and oil to surfactant mass ratios (S), have been applied for Pd-TiO{sub 2} preparation. The effect of ME properties on the morphology of Pd nanoparticles formed at TiO{sub 2} surface and an effect of Pd size and distribution on the surface and photocatalytic properties of Pd-TiO{sub 2} were investigated. Microemulsion systems were characterized by means of viscosity, density, dynamic light scattering as well as surface tension measurements to find a correlation between the conditions of Pd nanoparticles formation, their morphology and photocatalyst features. The photocatalysts were characterized by transmission electron microscopy (TEM), X-ray diffraction analysis (XRD), UV–vis diffuse-reflectance spectroscopy (DRS), BET surface area and elemental analysis. The photocatalytic properties of Pd-modified TiO{sub 2} particles were studied in a model reaction of phenol photodegradation under Vis irradiation, as well as active species involved in the photocatalytic reaction were determined. Microemulsion composition was found to be a crucial parameter in determining the features of the TiO{sub 2}-based photocatalysts covered by metallic nanoparticles. The highest photocatalytic activity under Vis radiation was observed for the Pd-TiO{sub 2} sample (average diameter 2.4 nm) obtained using 0.1 mol% Pd in the ME system containing 1.5 wt% of water and 82.8 wt% of cyclohexane with average droplet size of 2.83 ± 0.18 nm. In this regard, synthesis of such metal-semiconductor composites

  13. Dynamics of a Rydberg hydrogen atom near a metal surface in the electron-extraction scheme

    Energy Technology Data Exchange (ETDEWEB)

    Iñarrea, Manuel [Área de Física Aplicada, Universidad de La Rioja, Logroño (Spain); Lanchares, Víctor [Departamento de Matemáticas y Computación, Universidad de La Rioja, Logroño, La Rioja (Spain); Palacián, Jesús [Departamento de Ingeniería Matemática e Informática, Universidad Pública de Navarra, Pamplona (Spain); Pascual, Ana I. [Departamento de Matemáticas y Computación, Universidad de La Rioja, Logroño, La Rioja (Spain); Salas, J. Pablo, E-mail: josepablo.salas@unirioja.es [Área de Física Aplicada, Universidad de La Rioja, Logroño (Spain); Yanguas, Patricia [Departamento de Ingeniería Matemática e Informática, Universidad Pública de Navarra, Pamplona (Spain)

    2015-01-23

    We study the classical dynamics of a Rydberg hydrogen atom near a metal surface in the presence of a constant electric field in the electron-extraction situation [1], e.g., when the field attracts the electron to the vacuum. From a dynamical point of view, this field configuration provides a dynamics richer than in the usual ion-extraction scheme, because, depending on the values of field and the atom–surface distance, the atom can be ionized only towards the metal surface, only to the vacuum or to the both sides. The evolution of the phase space structure as a function of the atom–surface distance is explored in the bound regime of the atom. In the high energy regime, the ionization mechanism is also investigated. We find that the classical results of this work are in good agreement with the results obtained in the wave-packet propagation study carried out by So et al. [1]. - Highlights: • We study a classical hydrogen atom near a metal surface plus a electric field. • We explore the phase space structure as a function of the field strength. • We find most of the electronic orbits are oriented along the field direction. • We study the ionization of the atom for several atom–surface distances. • This classical study is in good agreement with the quantum results.

  14. Towards an atomic level understanding of niobia based catalysts and catalysis by combining the science of catalysis with surface science

    Directory of Open Access Journals (Sweden)

    Martin Schmal

    2009-06-01

    Full Text Available The science of catalysis and surface science have developed, independently, key information for understanding catalytic processes. One might argue: is there anything fundamental to be discovered through the interplay between catalysis and surface science? Real catalysts of monometallic and bimetallic Co/Nb2O5 and Pd-Co/Nb2O5 catalysts showed interesting selectivity results on the Fischer-Tropsch synthesis (Noronha et al. 1996, Rosenir et al. 1993. The presence of a noble metal increased the C+5 selectivity and decreased the methane formation depending of the reduction temperature. Model catalyst of Co-Pd supported on niobia and alumina were prepared and characterized at the atomic level, thus forming the basis for a comparison with "real" support materials. Growth, morphology and structure of both pure metal and alloy particles were studied. It is possible to support the strong metal support interaction suggested by studies on real catalysts via the investigation of model systems for niobia in comparison to alumina support in which this effect does not occur. Formation of Co2+ penetration into the niobia lattice was suggested on the basis of powder studies and can be fully supported on the basis of model studies. It is shown for both real catalysts and model systems that oxidation state of Co plays a key role in controlling the reactivity in Fischer-Tropsch reactions systems and that the addition of Pd is a determining factor for the stability of the catalyst. It is demonstrated that the interaction with unsaturated hydrocarbons depends strongly on the state of oxidation.As ciências da catálise e da superfície têm desenvolvido independentemente temas básicos para o entendimento de processos catalíticos. Pode-se até questionar se há ainda algo fundamental para ser descoberto através da interface entre catálise eciência da superfície? Catalisadores mono e bimetálicos de Co/Nb2O5 e Pd-Co/ Nb2O5 apresentaram resultados interessantes de

  15. Scattering of hyperthermal argon atoms from clean and D-covered Ru surfaces

    NARCIS (Netherlands)

    Ueta, H.; Gleeson, M.A.; Kleyn, A.W.

    2011-01-01

    Hyperthermal Ar atoms were scattered from a Ru(0001) surface held at temperatures of 180, 400 and 600 K, and from a Ru(0001)-(1×1)D surface held at 114 and 180 K. The resultant angular intensity and energy distributions are complex. The in-plane angular distributions have narrow (FWHM ≤ 10°)

  16. Hydrophilization of Poly(ether ether ketone) Films by Surface-initiated Atom Transfer Radical Polymerization

    DEFF Research Database (Denmark)

    Fristrup, Charlotte Juel; Eskimergen, Rüya; Burkrinsky, J.T.

    2008-01-01

    -modified PEEK using Surface-Initiated Atom Transfer Radical Polymerization (SI ATRP). Surface reduction of PEEK to form hydroxyl groups [1, 2, 3] was .performed prior to the attachment of 2-bromoisobutyrate initiating groups. Each modification step of PEEK as well as the polymer grafting was followed...... and confirmed by ATR FTIR, water contact ang;le, and Thermal Gravimetric Analysis (TGA). The surface topography was evaluated by "Atomic Force Microscopy (AFM). X-ray Photoelectron Spectroscopy (XPS) has been used to investigate the degree of functionalization. The performed modification allowed for successful...

  17. Surface modification of polystyrene with atomic oxygen radical anions-dissolved solution

    International Nuclear Information System (INIS)

    Wang Lian; Yan Lifeng; Zhao Peitao; Torimoto, Yoshifumi; Sadakata, Masayoshi; Li Quanxin

    2008-01-01

    A novel approach to surface modification of polystyrene (PS) polymer with atomic oxygen radical anions-dissolved solution (named as O - water) has been investigated. The O - water, generated by bubbling of the O - (atomic oxygen radical anion) flux into the deionized water, was characterized by UV-absorption spectroscopy and electron paramagnetic resonance (EPR) spectroscopy. The O - water treatments caused an obvious increase of the surface hydrophilicity, surface energy, surface roughness and also caused an alteration of the surface chemical composition for PS surfaces, which were indicated by the variety of contact angle and material characterization by atomic force microscope (AFM) imaging, field emission scanning electron microscopy (FESEM), X-ray photoelectron spectroscopy (XPS), and attenuated total-reflection Fourier transform infrared (ATR-FTIR) measurements. Particularly, it was found that some hydrophilic groups such as hydroxyl (OH) and carbonyl (C=O) groups were introduced onto the polystyrene surfaces via the O - water treatment, leading to the increases of surface hydrophilicity and surface energy. The active oxygen species would react with the aromatic ring molecules on the PS surfaces and decompose the aromatic compounds to produce hydrophilic hydroxyl and carbonyl compounds. In addition, the O - water is also considered as a 'clean solution' without adding any toxic chemicals and it is easy to be handled at room temperature. Present method may suit to the surface modification of polymers and other heat-sensitive materials potentially

  18. SASP '86: Symposium on atomic and surface physics

    International Nuclear Information System (INIS)

    Howorka, F.; Lindinger, W.; Maerk, T.D.

    1986-02-01

    71 papers are presented on subject matters indicated in the section headings: 1) Ion-neutral and neutral-neutral interactions in the gas phase; 2) Laser physics and photonics; 3) Electron collisions and electronic capture; 4) Ion-surface interaction and plasma-related effects; 5) Cluster physics. 70 thereof are of INIS interested and are treated separately. (G.Q.)

  19. Palladium-atom catalyzed formic acid decomposition and the switch of reaction mechanism with temperature.

    Science.gov (United States)

    He, Nan; Li, Zhen Hua

    2016-04-21

    Formic acid decomposition (FAD) reaction has been an innovative way for hydrogen energy. Noble metal catalysts, especially palladium-containing nanoparticles, supported or unsupported, perform well in this reaction. Herein, we considered the simplest model, wherein one Pd atom is used as the FAD catalyst. With high-level theoretical calculations of CCSD(T)/CBS quality, we investigated all possible FAD pathways. The results show that FAD catalyzed by one Pd atom follows a different mechanism compared with that catalyzed by surfaces or larger clusters. At the initial stage of the reaction, FAD follows a dehydration route and is quickly poisoned by CO due to the formation of very stable PdCO. PdCO then becomes the actual catalyst for FAD at temperatures approximately below 1050 K. Beyond 1050 K, there is a switch of catalyst from PdCO to Pd atom. The results also show that dehydration is always favoured over dehydrogenation on either the Pd-atom or PdCO catalyst. On the Pd-atom catalyst, neither dehydrogenation nor dehydration follows the formate mechanism. In contrast, on the PdCO catalyst, dehydrogenation follows the formate mechanism, whereas dehydration does not. We also systematically investigated the performance of 24 density functional theory methods. We found that the performance of the double hybrid mPW2PLYP functional is the best, followed by the B3LYP, B3PW91, N12SX, M11, and B2PLYP functionals.

  20. He atom surface scattering: Surface dynamics of insulators, overlayers and crystal growth

    International Nuclear Information System (INIS)

    1992-01-01

    Investigations have focused primarily on surface structure and dynamics of ionic insulators, epitaxial growth onto alkali halide crystals and multiphoton studies. The surface dynamics of RbCl has been re-examined. We have developed a simple force constant model which provides insight into the dynamics of KBr overlayers on NaCl(001), a system with a large lattice mismatch. The KBr/NaCl(001) results are compared to Na/Cu(001) and NaCl/Ge(001). We have completed epitaxial growth experiments for KBr onto RbCl(001). Slab dynamics calculations using a shell model for this system with very small lattice mismatch are being carried out in collaboration with Professor Manson of Clemson University and with Professor Schroeder in Regensburg, Germany. Extensive experiments on multiphoton scattering of helium atoms onto NaCl and, particularly, LiF have been carried out and the theory has been developed to a rather advanced stage by Professor Manson. This work will permit the extraction of more information from time-of-flight spectra. It is shown that the theoretical model provides a very good description of the multiphoton scattering from organic films. Work has started on self-assembling organic films on gold (alkyl thiols/Au(111)). We have begun to prepare and characterize the gold crystal; one of the group members has spent two weeks at the Oak Ridge National Laboratory learning the proper Au(111) preparation techniques. One of our students has carried out neutron scattering experiments on NiO, measuring both bulk phonon and magnon dispersion curves

  1. Plant-Mediated Fabrication and Surface Enhanced Raman Property of Flower-Like Au@Pd Nanoparticles

    Directory of Open Access Journals (Sweden)

    Daohua Sun

    2014-02-01

    Full Text Available The flower-like nanostructures of an Au core and Pd petals with the average size of 47.8 nm were fabricated through the successive reduction of HAuCl4 and Na2PdCl4 at room temperature. During the synthesis, Cacumen Platycladi leaf extract served as weak reductant and capping agent. Characterization techniques such as Energy-dispersive X-ray spectroscopy, UV-Vis spectroscopy, and X-ray diffraction characterizations were employed to confirm that the as-synthesized nanoparticles have the structure of core-shell. The obtained core-shell nanoflowers exhibited good surface enhanced Raman spectroscopic activity with Rhodamine 6G.

  2. Surface modification of acetaminophen particles by atomic layer deposition.

    Science.gov (United States)

    Kääriäinen, Tommi O; Kemell, Marianna; Vehkamäki, Marko; Kääriäinen, Marja-Leena; Correia, Alexandra; Santos, Hélder A; Bimbo, Luis M; Hirvonen, Jouni; Hoppu, Pekka; George, Steven M; Cameron, David C; Ritala, Mikko; Leskelä, Markku

    2017-06-15

    Active pharmaceutical ingredients (APIs) are predominantly organic solid powders. Due to their bulk properties many APIs require processing to improve pharmaceutical formulation and manufacturing in the preparation for various drug dosage forms. Improved powder flow and protection of the APIs are often anticipated characteristics in pharmaceutical manufacturing. In this work, we have modified acetaminophen particles with atomic layer deposition (ALD) by conformal nanometer scale coatings in a one-step coating process. According to the results, ALD, utilizing common chemistries for Al 2 O 3 , TiO 2 and ZnO, is shown to be a promising coating method for solid pharmaceutical powders. Acetaminophen does not undergo degradation during the ALD coating process and maintains its stable polymorphic structure. Acetaminophen with nanometer scale ALD coatings shows slowed drug release. ALD TiO 2 coated acetaminophen particles show cytocompatibility whereas those coated with thicker ZnO coatings exhibit the most cytotoxicity among the ALD materials under study when assessed in vitro by their effect on intestinal Caco-2 cells. Copyright © 2017 Elsevier B.V. All rights reserved.

  3. Technologies for protection of the Space Station power system surfaces in atomic oxygen environment

    Science.gov (United States)

    Nahra, Henry K.; Rutledge, Sharon K.

    1988-01-01

    Technologies for protecting Space Station surfaces from degradation caused by atomic oxygen are discussed, stressing protection of the power system surfaces. The Space Station power system is described and research concerning the solar array surfaces and radiator surfaces is examined. The possibility of coating the solar array sufaces with a sputter deposited thin film of silicon oxide containing small concentrations of polytetrafluoroethylene is presented. Hexamethyldisiloxane coating for these surfaces is also considered. For the radiator surfaces, possible coatings include silver teflon thermal coating and zinc orthotitanate.

  4. Inelastic electron scattering in aggregates of transition metal atoms on metal surfaces

    Science.gov (United States)

    Goldberg, E. C.; Flores, F.

    2017-09-01

    Inelastic spin excitations, as observed with a scanning tunneling microscope for Co/Co and Fe/Fe dimers on a Cu2N/Cu(100) surface, have been analyzed theoretically in this paper. In our approach, we use an extended ionic Hamiltonian for the magnetic atom that takes into account first, the role played by the first Hund rule in the atomic states, and second, the cotunneling processes associated with the atomic excitations and the tunneling conductance. This Hamiltonian is solved using the equation of motion method that yields the appropriate Green's functions allowing us to calculate the differential conductance, the inelastic atomic excitations, and possible Kondo resonances. We also analyze an ideal dimer with spin ½ in each atom and discuss the differences and similarities this model has with the Co-Co case.

  5. Facile embedding of single vanadium atoms at the anatase TiO2(101) surface.

    Science.gov (United States)

    Koust, Stig; Arnarson, Logi; Moses, Poul G; Li, Zheshen; Beinik, Igor; Lauritsen, Jeppe V; Wendt, Stefan

    2017-04-05

    To understand the structure-reactivity relationships for mixed-metal oxide catalysts, well-defined systems are required. Mixtures of vanadia and titania (TiO 2 ) are of particular interest for application in heterogeneous catalysis, with TiO 2 often acting as the support. By utilizing high-resolution scanning tunneling microscopy, we studied the interaction of vanadium (V) with the anatase TiO 2 (101) surface in the sub-monolayer regime. At 80 K, metallic V nucleates into homogeneously distributed clusters onto the terraces with no preference for nucleation at the step edges. However, embedding of single V atoms into TiO 2 occurs following annealing at room temperature. In conjunction with X-ray photoelectron spectroscopy data and density functional theory calculations, we propose that monomeric V atoms occupy positions of regular surface Ti sites, i.e., Ti atoms are substituted by V atoms.

  6. Resonance studies of H atoms adsorbed on frozen H2 surfaces

    International Nuclear Information System (INIS)

    Crampton, S.B.

    1980-01-01

    Observations are reported of the ground state hyperfine resonance of hydrogen atoms stored in a 5 cm. diameter bottle coated with frozen molecular hydrogen. Dephasing of the hyperfine resonance while the atoms are adsorbed produces frequency shifts which vary by a factor of two over the temperature range 3.7 K to 4.6 K and radiative decay rates which vary by a factor of five over this range. The magnitudes and temperature dependences of the frequency shifts and decay rates are consistent with a non-uniform distribution of surface adsorption energies with mean about 38(8) K, in agreement with theoretical estimates for a smooth surface. Extrapolation of the 30 nanosec. mean adsorption times at 4.2 K predicts very long adsorption times for H on H 2 below 1 K. Studies of level population recovery rates provide evidence for surface electron spin exchange collisions between adsorbed atoms with collision duration long compared to the hyperfine period, suggesting that the atoms are partially mobile on the surface. The lowest rates observed for level population recovery set a lower limit of about 500 atom-surface collisions at 4.2 K without recombination

  7. Influence of Pd/Pd2 decoration on the structural, electronic and sensing properties of monolayer graphene in the presence of methane molecule: A dispersion-corrected DFT study

    Science.gov (United States)

    Nasresfahani, Sh.; Safaiee, R.; Sheikhi, M. H.

    2017-08-01

    This paper is devoted to study on the methane (CH4) adsorption ability of graphene decorated by a single palladium (Pd) atom and its dimer (Pd2), using dispersion-corrected density functional theory (DFT-D2). The adsorption energy, optimum geometry and electronic structure in terms of density of states, band structure, and charge transfer are calculated. Our results show that van der Waals interactions lead to physisorption of CH4 on the prisitine graphene with the adsorption energy of -112 meV, which is close to its experimental value. The calculations also show that hybridization of Pd and graphene electronic states strongly binds Pd atoms to graphene surface, inducing chemisorption of the adsorbate. The adsorption energies of Pd atom and its dimer have been found to be -1.43 eV and -2.27 eV, respectively. Furthermore symmetry breaking of the graphene structure, due to the Pd/Pd2-decoration, leads to opening a band gap, bringing graphene from semimetalic to semiconducting state. In the presence of methane molecule, the electronic band gap of Pd-decorated graphene is increased from 73 meV to 90 meV, while for Pd dimer it is decreased from 185 meV to 55 meV. As a result, compared to Pd-decorated graphene, Pd2-decorated graphene has a stronger interaction with the methane molecule and may provide a more sensitive signal for methane gas detection.

  8. Spatial and energy distributions of satellite-speed helium atoms reflected from satellite-type surfaces

    International Nuclear Information System (INIS)

    Liu, S.M.; Rodgers, W.E.; Knuth, E.L.

    1977-01-01

    Interactions of satellite-speed helium atoms (accelerated in an expansion from an arc-heated supersonic-molecular-beam source) with practical satellite surfaces have been investigated experimentally. The density and energy distributions of the scattered atoms were measured using a detection system developed for this study. This detection system includes (a) a target positioning mechanism, (b) a detector rotating mechanism, and (c) a mass spectrometer and/or a retarding-field energy analyzer. (Auth.)

  9. Effects of atomic oxygen irradiation on the surface properties of phenolphthalein poly(ether sulfone)

    International Nuclear Information System (INIS)

    Pei Xianqiang; Li Yan; Wang Qihua; Sun Xiaojun

    2009-01-01

    To study the effects of low earth orbit environment on the surface properties of polymers, phenolphthalein poly(ether sulfone) (PES-C) blocks were irradiated by atomic oxygen in a ground-based simulation system. The surface properties of the pristine and irradiated blocks were studied by attenuated total-reflection FTIR (FTIR-ATR), X-ray photoelectron spectroscopy (XPS), scanning electron microscope (SEM). It was found that atomic oxygen irradiation induced the destruction of PES-C molecular chains, including the scission and oxidation of PES-C molecular chains, as evidenced by FTIR and XPS results. The scission of PES-C molecular chains decreased the relative concentration of C in the surface, while the oxidation increased the relative concentration of O in the surface. The changes in surface chemical structure and composition also changed the surface morphology of the block, which shifted from smooth structure before irradiation to 'carpet-like' structure after irradiation

  10. Effects of atomic oxygen irradiation on the surface properties of phenolphthalein poly(ether sulfone)

    Energy Technology Data Exchange (ETDEWEB)

    Pei Xianqiang [State Key Laboratory of Solid Lubrication, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, No. 18, Tianshui Middle Road, Lanzhou 730000 (China); Li Yan [State Key Laboratory of Solid Lubrication, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, No. 18, Tianshui Middle Road, Lanzhou 730000 (China); Graduate school of the Chinese Academy of Sciences, Beijing 100039 (China); Wang Qihua [State Key Laboratory of Solid Lubrication, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, No. 18, Tianshui Middle Road, Lanzhou 730000 (China)], E-mail: Wangqh@lzb.ac.cn; Sun Xiaojun [State Key Laboratory of Solid Lubrication, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, No. 18, Tianshui Middle Road, Lanzhou 730000 (China)

    2009-03-15

    To study the effects of low earth orbit environment on the surface properties of polymers, phenolphthalein poly(ether sulfone) (PES-C) blocks were irradiated by atomic oxygen in a ground-based simulation system. The surface properties of the pristine and irradiated blocks were studied by attenuated total-reflection FTIR (FTIR-ATR), X-ray photoelectron spectroscopy (XPS), scanning electron microscope (SEM). It was found that atomic oxygen irradiation induced the destruction of PES-C molecular chains, including the scission and oxidation of PES-C molecular chains, as evidenced by FTIR and XPS results. The scission of PES-C molecular chains decreased the relative concentration of C in the surface, while the oxidation increased the relative concentration of O in the surface. The changes in surface chemical structure and composition also changed the surface morphology of the block, which shifted from smooth structure before irradiation to 'carpet-like' structure after irradiation.

  11. Effects of atomic oxygen irradiation on the surface properties of phenolphthalein poly(ether sulfone)

    Science.gov (United States)

    Pei, Xianqiang; Li, Yan; Wang, Qihua; Sun, Xiaojun

    2009-03-01

    To study the effects of low earth orbit environment on the surface properties of polymers, phenolphthalein poly(ether sulfone) (PES-C) blocks were irradiated by atomic oxygen in a ground-based simulation system. The surface properties of the pristine and irradiated blocks were studied by attenuated total-reflection FTIR (FTIR-ATR), X-ray photoelectron spectroscopy (XPS), scanning electron microscope (SEM). It was found that atomic oxygen irradiation induced the destruction of PES-C molecular chains, including the scission and oxidation of PES-C molecular chains, as evidenced by FTIR and XPS results. The scission of PES-C molecular chains decreased the relative concentration of C in the surface, while the oxidation increased the relative concentration of O in the surface. The changes in surface chemical structure and composition also changed the surface morphology of the block, which shifted from smooth structure before irradiation to "carpet-like" structure after irradiation.

  12. Advances in electric field and atomic surface derived properties from experimental electron densities.

    Science.gov (United States)

    Bouhmaida, Nouzha; Ghermani, Nour Eddine

    2008-07-14

    The present study is devoted to a general use of the Gauss law. This is applied to the atomic surfaces derived from the topological analysis of the electron density. The method proposed here is entirely numerical, robust and does not necessitate any specific parametrization of the atomic surfaces. We focus on two fundamental properties: the atomic charges and the electrostatic forces acting on atoms in molecules. Application is made on experimental electron densities modelized by the Hansen-Coppens model from which the electric field is derived for a heterogenic set of compounds: water molecule, NO(3) anion, bis-triazine molecule and MgO cluster. Charges and electrostatic forces are estimated by the atomic surface flux of the electric field and the Maxwell stress tensor, respectively. The charges obtained from the present method are in good agreement with those issued from the conventional volume integration. Both Feynman and Ehrenfest forces as well as the electrostatic potential at the nuclei (EPN) are here estimated from the experimental electron densities. The values found for the molecular compounds are presented and discussed in the scope of the mechanics of atomic interactions.

  13. Monte Carlo Technique Used to Model the Degradation of Internal Spacecraft Surfaces by Atomic Oxygen

    Science.gov (United States)

    Banks, Bruce A.; Miller, Sharon K.

    2004-01-01

    Atomic oxygen is one of the predominant constituents of Earth's upper atmosphere. It is created by the photodissociation of molecular oxygen (O2) into single O atoms by ultraviolet radiation. It is chemically very reactive because a single O atom readily combines with another O atom or with other atoms or molecules that can form a stable oxide. The effects of atomic oxygen on the external surfaces of spacecraft in low Earth orbit can have dire consequences for spacecraft life, and this is a well-known and much studied problem. Much less information is known about the effects of atomic oxygen on the internal surfaces of spacecraft. This degradation can occur when openings in components of the spacecraft exterior exist that allow the entry of atomic oxygen into regions that may not have direct atomic oxygen attack but rather scattered attack. Openings can exist because of spacecraft venting, microwave cavities, and apertures for Earth viewing, Sun sensors, or star trackers. The effects of atomic oxygen erosion of polymers interior to an aperture on a spacecraft were simulated at the NASA Glenn Research Center by using Monte Carlo computational techniques. A two-dimensional model was used to provide quantitative indications of the attenuation of atomic oxygen flux as a function of the distance into a parallel-walled cavity. The model allows the atomic oxygen arrival direction, the Maxwell Boltzman temperature, and the ram energy to be varied along with the interaction parameters of the degree of recombination upon impact with polymer or nonreactive surfaces, the initial reaction probability, the reaction probability dependence upon energy and angle of attack, degree of specularity of scattering of reactive and nonreactive surfaces, and the degree of thermal accommodation upon impact with reactive and non-reactive surfaces to be varied to allow the model to produce atomic oxygen erosion geometries that replicate actual experimental results from space. The degree of

  14. Grazing incidence collisions of ions and atoms with surfaces: from charge exchange to atomic diffraction; Collisions rasantes d'ions ou d'atomes sur les surfaces: de l'echange de charge a la diffraction atomique

    Energy Technology Data Exchange (ETDEWEB)

    Rousseau, P

    2006-09-15

    This thesis reports two studies about the interaction with insulating surfaces of keV ions or atoms under grazing incidence. The first part presents a study of charge exchange processes occurring during the interaction of singly charged ions with the surface of NaCl. In particular, by measuring the scattered charge fraction and the energy loss in coincidence with electron emission, the neutralization mechanism is determined for S{sup +}, C{sup +}, Xe{sup +}, H{sup +}, O{sup +}, Kr{sup +}, N{sup +}, Ar{sup +}, F{sup +}, Ne{sup +} and He{sup +}. These results show the importance of the double electron capture as neutralization process for ions having too much potential energy for resonant capture and not enough for Auger neutralization. We have also studied the ionisation of the projectile and of the surface, and the different Auger-like neutralization processes resulting in electron emission, population of conduction band or excited state. For oxygen scattering, we have measured an higher electron yield in coincidence with scattered negative ion than with scattered atom suggesting the transient formation above the surface of the oxygen doubly negative ion. The second study deals with the fast atom diffraction, a new phenomenon observed for the first time during this work. Due to the large parallel velocity, the surface appears as a corrugated wall where rows interfere. Similarly to the Thermal Atom Scattering the diffraction pattern corresponds to the surface potential and is sensitive to vibrations. We have study the H-NaCl and He-LiF atom-surface potentials in the 20 meV - 1 eV range. This new method offers interesting perspectives for surface characterisation. (author)

  15. G-6-PD level and surface nanoscopy: a novel approach in ergonomic stress management of female labours in Bengal suburbs performing manual material handling.

    Science.gov (United States)

    Ghosh, Subrata; Acharyya, Muktish; Bagchi, Anandi

    2009-12-01

    Strenous physical exercise like professional load bearing often produces oxidative stress, increasing post exercise Malondialdehyde (MDA) levels. To quantify the cellular dimension/profile of the said stress, nanoscopic observation of the erythrocyte surface was made by Atomic Forced Microscopy (AFM)/Lateral Forced Microscopy (LFM) and correspondingly the average roughness of the surface was measured. An attempt has been made to correlate the antioxidant vitamin mixture supplementation, endurance capacity, allied physiological parameters and blood glucose-6-phosphate dehydrogenase (G-6-PD) level and roughness-MDA correlation and thereby the deduced regression equation as crucial markers of performance related oxidative stress management in professional female load bearers. Three experimental groups A, B and placebo, each consisting of ten female workers (18-21 years old), were chosen. Group A was given 400 mg of vitamin E supplementation daily, while Group B was given a clinical mixture of vitamin E, vitamin C and beta-carotene daily in capsular form for a period of 28 days. The exercise- induced hike in the status of serum MDA was found to rise less significantly with vitamin supplementation. Further study showed that the supplementation was instrumental in reducing the basal MDA level. Endurance capacity, determined by bicycle ergometric method, was increased more significantly (p material handling.

  16. Observation of modified radiative properties of cold atoms in vacuum near a dielectric surface

    International Nuclear Information System (INIS)

    Ivanov, V V; Cornelussen, R A; Heuvell, H B van Linden van den; Spreeuw, R J C

    2004-01-01

    We have observed a distance-dependent absorption linewidth of cold 87 Rb atoms close to a dielectric-vacuum interface. This is the first observation of modified radiative properties in vacuum near a dielectric surface. A cloud of cold atoms was created using a magneto-optical trap (MOT) and optical molasses cooling. Evanescent waves (EW) were used to observe the behaviour of the atoms near the surface. We observed an increase of the absorption linewidth by up to 25% with respect to the free-space value. Approximately half the broadening can be explained by cavity quantum electrodynamics (CQED) as an increase of the natural linewidth and inhomogeneous broadening. The remainder we attribute to local Stark shifts near the surface. By varying the characteristic EW length we have observed a distance dependence characteristic for CQED

  17. Hydrogen atom addition to the surface of graphene nanoflakes: A density functional theory study

    International Nuclear Information System (INIS)

    Tachikawa, Hiroto

    2017-01-01

    Highlights: • The reaction pathway of the hydrogen addition to graphene surface was determined by the DFT method. • Binding energies of atomic hydrogen to graphene surface were determined. • Absorption spectrum of hydrogenated graphene was theoretically predicted. • Hyperfine coupling constant of hydrogenated graphene was theoretically predicted. - Abstract: Polycyclic aromatic hydrocarbons (PAHs) provide a 2-dimensional (2D) reaction surface in 3-dimensional (3D) interstellar space and have been utilized as a model of graphene surfaces. In the present study, the reaction of PAHs with atomic hydrogen was investigated by means of density functional theory (DFT) to systematically elucidate the binding nature of atomic hydrogen to graphene nanoflakes. PAHs with n = 4–37 were chosen, where n indicates the number of benzene rings. Activation energies of hydrogen addition to the graphene surface were calculated to be 5.2–7.0 kcal/mol at the CAM-B3LYP/6-311G(d,p) level, which is almost constant for all PAHs. The binding energies of hydrogen atom were slightly dependent on the size (n): 14.8–28.5 kcal/mol. The absorption spectra showed that a long tail is generated at the low-energy region after hydrogen addition to the graphene surface. The electronic states of hydrogenated graphenes were discussed on the basis of theoretical results.

  18. Hydrogen atom addition to the surface of graphene nanoflakes: A density functional theory study

    Energy Technology Data Exchange (ETDEWEB)

    Tachikawa, Hiroto, E-mail: hiroto@eng.hokudai.ac.jp

    2017-02-28

    Highlights: • The reaction pathway of the hydrogen addition to graphene surface was determined by the DFT method. • Binding energies of atomic hydrogen to graphene surface were determined. • Absorption spectrum of hydrogenated graphene was theoretically predicted. • Hyperfine coupling constant of hydrogenated graphene was theoretically predicted. - Abstract: Polycyclic aromatic hydrocarbons (PAHs) provide a 2-dimensional (2D) reaction surface in 3-dimensional (3D) interstellar space and have been utilized as a model of graphene surfaces. In the present study, the reaction of PAHs with atomic hydrogen was investigated by means of density functional theory (DFT) to systematically elucidate the binding nature of atomic hydrogen to graphene nanoflakes. PAHs with n = 4–37 were chosen, where n indicates the number of benzene rings. Activation energies of hydrogen addition to the graphene surface were calculated to be 5.2–7.0 kcal/mol at the CAM-B3LYP/6-311G(d,p) level, which is almost constant for all PAHs. The binding energies of hydrogen atom were slightly dependent on the size (n): 14.8–28.5 kcal/mol. The absorption spectra showed that a long tail is generated at the low-energy region after hydrogen addition to the graphene surface. The electronic states of hydrogenated graphenes were discussed on the basis of theoretical results.

  19. The kinetics of formation and transformation of silver atoms on solid surfaces subjected to ionizing irradiation

    International Nuclear Information System (INIS)

    Popovich, G.M.

    1988-01-01

    The paper discusses the results obtained in ESR-assisted studies of the kinetics of formation and transformation of silver atoms generated by γ-irradiation of silver-containing carriers. Three types of dependences have been established: (1) extreme; (2) saturation curves and (3) step-like. All the kinetic curves display, after a definite period of time, stable concentrations of adsorbed silver atoms per unit of the surface at a given temperature. Depending on the temperature of the experiment, the composition and nature of the carrier, the number of adsorbed silver ions, the irradiation dose and conditions of the experiment, a stable concentration of silver atoms at a given temperature may be equal to, higher or lower than the number of silver atoms measured immediately after γ-irradiation at a temperature of liquid nitrogen. A kinetic scheme is proposed to explain the obtained curves. The model suggests that the silver atoms adsorbed on the surface, as well as those formed after γ-irradiation, are bonded to the surface by various energies, which are related to heterogeneity of the carrier surface. (author)

  20. Supersaturation-controlled surface structure evolution of Pd@Pt core-shell nanocrystals: enhancement of the ORR activity at a sub-10 nm scale

    Science.gov (United States)

    Qi, Kun; Zheng, Weitao; Cui, Xiaoqiang

    2016-01-01

    Here, we designed and implemented a facile strategy for controlling the surface evolution of Pd@Pt core-shell nanostructures by simply adjusting the volume of OH- to control the reducing ability of ascorbic acid and finally manipulating the supersaturation in the reaction system. The surface structure of the obtained Pd@Pt bimetallic nanocrystals transformed from a Pt {111} facet-exposed island shell to a conformal Pt {100} facet-exposed shell by increasing the pH value. The as-prepared well aligned Pd@Pt core-island shell nanocubes present both significantly enhanced electrocatalytic activity and favorable long-term stability toward the oxygen reduction reaction in alkaline media.Here, we designed and implemented a facile strategy for controlling the surface evolution of Pd@Pt core-shell nanostructures by simply adjusting the volume of OH- to control the reducing ability of ascorbic acid and finally manipulating the supersaturation in the reaction system. The surface structure of the obtained Pd@Pt bimetallic nanocrystals transformed from a Pt {111} facet-exposed island shell to a conformal Pt {100} facet-exposed shell by increasing the pH value. The as-prepared well aligned Pd@Pt core-island shell nanocubes present both significantly enhanced electrocatalytic activity and favorable long-term stability toward the oxygen reduction reaction in alkaline media. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr07940c

  1. Pd/MWCNTs catalytic activity in the formic acid electrooxidation dependent on catalyst surface treatment

    Czech Academy of Sciences Publication Activity Database

    Mazurkiewicz, M.; Malolepszy, A.; Mikolajczuk, A.; Stobinski, L.; Borodzinski, A.; Lesiak, B.; Zemek, Josef; Jiříček, Petr

    2011-01-01

    Roč. 248, č. 11 (2011), s. 2516-2519 ISSN 0370-1972 Institutional research plan: CEZ:AV0Z10100521 Keywords : electrooxidation reaction * Pd/MWCNT * TEM * XPS * XRD Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 1.316, year: 2011

  2. Single OR molecule and OR atomic circuit logic gates interconnected on a Si(100)H surface

    International Nuclear Information System (INIS)

    Ample, F; Joachim, C; Duchemin, I; Hliwa, M

    2011-01-01

    Electron transport calculations were carried out for three terminal OR logic gates constructed either with a single molecule or with a surface dangling bond circuit interconnected on a Si(100)H surface. The corresponding multi-electrode multi-channel scattering matrix (where the central three terminal junction OR gate is the scattering center) was calculated, taking into account the electronic structure of the supporting Si(100)H surface, the metallic interconnection nano-pads, the surface atomic wires and the molecule. Well interconnected, an optimized OR molecule can only run at a maximum of 10 nA output current intensity for a 0.5 V bias voltage. For the same voltage and with no molecule in the circuit, the output current of an OR surface atomic scale circuit can reach 4 μA.

  3. Interaction of slow and highly charged ions with surfaces: formation of hollow atoms

    Energy Technology Data Exchange (ETDEWEB)

    Stolterfoht, N.; Grether, M.; Spieler, A.; Niemann, D. [Hahn-Meitner Institut, Berlin (Germany). Bereich Festkoerperphysik; Arnau, A.

    1997-03-01

    The method of Auger spectroscopy was used to study the interaction of highly charged ions with Al and C surfaces. The formation of hollow Ne atoms in the first surface layers was evaluated by means of a Density Functional theory including non-linear screening effects. The time-dependent filling of the hollow atom was determined from a cascade model yielding information about the structure of the K-Auger spectra. Variation of total intensities of the L- and K-Auger peaks were interpreted by the cascade model in terms of attenuation effects on the electrons in the solid. (author)

  4. SASP. Contributions to the 13. Symposium on atomic and surface physics and related topics

    International Nuclear Information System (INIS)

    Scheier, P.; Maerk, T.

    2002-01-01

    The XIII symposium on Atomic and Surface Physics and related Topics (SASP) is devoted to cover the research of interactions between ions, electrons, photons, atoms, molecules and clusters and their interaction with surfaces. This year there was a special session dedicated to proton transfer reaction mass spectrometry covering its applications in different fields and a mini symposium on the radiation action on bio-molecules such as uracil. The contributions included in the proceeding correspond to invited lectures and poster sessions, consisting of short and extended abstracts as well as short articles. (nevyjel)

  5. Resonant coherent ionization in grazing ion/atom-surface collisions at high velocities

    International Nuclear Information System (INIS)

    Garcia de Abajo, F.J.; Pitarke, J.M.

    1994-01-01

    The resonant coherent interaction of a fast ion/atom with an oriented crystal surface under grazing incidence conditions is shown to contribute significantly to ionize the probe for high enough velocities and motion along a random direction. The dependence of this process on both the distance to the surface and the velocity of the projectile is studied in detail. We focus on the case of hydrogen moving with a velocity above 2 a.u. Comparison with other mechanisms of charge transfer, such as capture from inner shells of the target atoms, permits us to draw some conclusions about the charge state of the outgoing projectiles. (orig.)

  6. Atomic Oxygen Treatment for Non-Contact Removal of Organic Protective Coatings from Painting Surfaces

    Science.gov (United States)

    Rutledge, Sharon K.; Banks, Bruce A.; Cales, Michael

    1994-01-01

    Current techniques for removal of varnish (lacquer) and other organic protective coatings from paintings involve contact with the surface. This contact can remove pigment, or alter the shape and location of paint on the canvas surface. A thermal energy atomic oxygen plasma, developed to simulate the space environment in low Earth orbit, easily removes these organic materials. Uniform removal of organic protective coatings from the surfaces of paintings is accomplished through chemical reaction. Atomic oxygen will not react with oxides so that most paint pigments will not be affected by the reaction. For paintings containing organic pigments, the exposure can be carefully timed so that the removal stops just short of the pigment. Color samples of Alizarin Crimson, Sap Green, and Zinc White coated with Damar lacquer were exposed to atomic oxygen. The lacquer was easily removed from all of the samples. Additionally, no noticeable change in appearance was observed after the lacquer was reapplied. The same observations were made on a painted canvas test sample obtained from the Cleveland Museum of Art. Scanning electron microscope photographs showed a slight microscopic texturing of the vehicle after exposure. However, there was no removal or disturbance of the paint pigment on the surface. It appears that noncontact cleaning using atomic oxygen may provide a viable alternative to other cleaning techniques. It is especially attractive in cases where the organic protective surface cannot be acceptably or safely removed by conventional techniques.

  7. Site-specific growth of Au-Pd alloy horns on Au nanorods: A platform for highly sensitive monitoring of catalytic reactions by surface enhancement raman spectroscopy

    KAUST Repository

    Huang, Jianfeng

    2013-06-12

    Surface-enhanced Raman scattering (SERS) is a highly sensitive probe for molecular detection. The aim of this study was to develop an efficient platform for investigating the kinetics of catalytic reactions with SERS. To achieve this, we synthesized a novel Au-Pd bimetallic nanostructure (HIF-AuNR@AuPd) through site-specific epitaxial growth of Au-Pd alloy horns as catalytic sites at the ends of Au nanorods. Using high-resolution electron microscopy and tomography, we successfully reconstructed the complex three-dimensional morphology of HIF-AuNR@AuPd and identified that the horns are bound with high-index {11l} (0.25 < l < 0.43) facets. With an electron beam probe, we visualized the distribution of surface plasmon over the HIF-AuNR@AuPd nanorods, finding that strong longitudinal surface plasmon resonance concentrated at the rod ends. This unique crystal morphology led to the coupling of high catalytic activity with a strong SERS effect at the rod ends, making HIF-AuNR@AuPd an excellent bifunctional platform for in situ monitoring of surface catalytic reactions. Using the hydrogenation of 4-nitrothiophenol as a model reaction, we demonstrated that its first-order reaction kinetics could be accurately determined from this platform. Moreover, we clearly identified the superior catalytic activity of the rod ends relative to that of the rod bodies, owing to the different SERS activities at the two positions. In comparison with other reported Au-Pd bimetallic nanostructures, HIF-AuNR@AuPd offered both higher catalytic activity and greater detection sensitivity. © 2013 American Chemical Society.

  8. Temperature dependent dual hydrogen sensor response of Pd nanoparticle decorated Al doped ZnO surfaces

    Science.gov (United States)

    Gupta, D.; Dutta, D.; Kumar, M.; Barman, P. B.; Som, T.; Hazra, S. K.

    2015-10-01

    Sputter deposited Al doped ZnO (AZO) thin films exhibit a dual hydrogen sensing response in the temperature range 40 °C-150 °C after surface modifications with palladium nanoparticles. The unmodified AZO films showed no response in hydrogen in the temperature range 40 °C-150 °C. The operational temperature windows on the low and high temperature sides have been estimated by isolating the semiconductor-to-metal transition temperature zone of the sensor device. The gas response pattern was modeled by considering various adsorption isotherms, which revealed the dominance of heterogeneous adsorption characteristics. The Arrhenius adsorption barrier showed dual variation with change in hydrogen gas concentration on either side of the semiconductor-to-metal transition. A detailed analysis of the hydrogen gas response pattern by considering the changes in nano palladium due to hydrogen adsorption, and semiconductor-to-metal transition of nanocrystalline Al doped ZnO layer due to temperature, along with material characterization studies by glancing incidence X-ray diffraction, atomic force microscopy, and transmission electron microscopy, are presented.

  9. Atomic Level Cleaning of Poly Methyl Methacrylate Residues from the Graphene Surface Using Radiolized Water at High Temperatures (Postprint)

    Science.gov (United States)

    2017-09-05

    AFRL-RX-WP-JA-2017-0321 ATOMIC LEVEL CLEANING OF POLY-METHYL- METHACRYLATE RESIDUES FROM THE GRAPHENE SURFACE USING RADIOLIZED WATER AT...COVERED (From - To) 9 March 2017 Interim 8 September 2014 – 9 February 2017 4. TITLE AND SUBTITLE ATOMIC LEVEL CLEANING OF POLY-METHYL- METHACRYLATE...graphene surfaces and can only provide atomically clean graphene surfaces in areas as large as ˜10-4 µm2. Here, we transfer CVD-grown graphene using

  10. Surface structures from low energy electron diffraction: Atoms, small molecules and an ordered ice film on metal surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Materer, Nicholas F. [Univ. of California, Berkeley, CA (United States)

    1995-09-01

    We investigated the surface bonding of various adsorbates (0, S, C2H3 and NO) along with the resulting relaxation of the Pt(111) surface using low energy electron diffiraction (LEED). LEED experiments have been performed on these ordered overlayers along with theoretical structural analysis using automated tensor LEED (ATLEED). The resulting surface structures of these ordered overlayers exhibit similar adsorbate-induced relaxations. In all cases the adsorbate occupies the fcc hollow site and induces an approximately 0.1 A buckling of the metal surface. The three metal atoms directly bonded to the adsorbate are ``pulled`` out of the surface and the metal atom that is not bound to the adsorbate is `pushed`` inward. In order to understand the reliability of such details, we have carried out a comprehensive study of various non-structural parameters used in a LEED computation. We also studied the adsorption of water on the Pt(lll) surface. We ordered an ultra thin ice film on this surface. The film`s surface is found to be the (0001) face of hexagonal ice. This surface is apparently terminated by a full-bilayer, in which the uppermost water molecules have large vibrational amplitudes even at temperatures as low as 90 K. We examined two other metal surfaces besides Pt(111): Ni(111) and Fe(lll). On Ni(111), we have studied the surface under a high coverage of NO. On both Ni(111) and Pt(111) NO molecules occupy the hollow sites and the N-0 bond distances are practically identical. The challenging sample preparation of an Fe(111) surface has been investigated and a successful procedure has been obtained. The small interlayer spacing found on Fe(111) required special treatment in the LEED calculations. A new ATLEED program has been developed to handle this surface.

  11. Evaluation of the roughness of the surface of porcelain systems with the atomic force microscope

    International Nuclear Information System (INIS)

    Chavarria Rodriguez, Bernal

    2013-01-01

    The surface of a dental ceramic was evaluated and compared with an atomic force microscope after being treated with different systems of polishing. 14 identical ceramic Lava® Zirconia discs were used to test the different polishing systems. 3 polishing systems from different matrix houses were used to polish dental porcelain. The samples were evaluated quantitatively with an atomic force microscope in order to study the real effectiveness of each system, on the roughness average (Ra) and the maximum peak to valley roughness (Ry) of the ceramic surfaces. A considerable reduction of the surface roughness was obtained by applying different polishing systems on the surface of dental ceramics. Very reliable values of Ra and Ry were obtained by making measurements on the structure reproduced by the atomic force microscope. The advanced ceramics of zirconium oxide presented the best physical characteristics and low levels of surface roughness. A smoother surface was achieved with the application of polishing systems, thus demonstrating the reduction of the surface roughness of a dental ceramic [es

  12. Magnetic frustration, short-range correlations and the role of the paramagnetic Fermi surface of PdCrO2

    Science.gov (United States)

    Billington, David; Ernsting, David; Millichamp, Thomas E.; Lester, Christopher; Dugdale, Stephen B.; Kersh, David; Duffy, Jonathan A.; Giblin, Sean R.; Taylor, Jonathan W.; Manuel, Pascal; Khalyavin, Dmitry D.; Takatsu, Hiroshi

    2015-01-01

    Frustrated interactions exist throughout nature, with examples ranging from protein folding through to frustrated magnetic interactions. Whilst magnetic frustration is observed in numerous electrically insulating systems, in metals it is a rare phenomenon. The interplay of itinerant conduction electrons mediating interactions between localised magnetic moments with strong spin-orbit coupling is likely fundamental to these systems. Therefore, knowledge of the precise shape and topology of the Fermi surface is important in any explanation of the magnetic behaviour. PdCrO2, a frustrated metallic magnet, offers the opportunity to examine the relationship between magnetic frustration, short-range magnetic order and Fermi surface topology. By mapping the short-range order in reciprocal space and experimentally determining the electronic structure, we have identified the dual role played by the Cr electrons in which the itinerant ones on the nested paramagnetic Fermi surface mediate the frustrated magnetic interactions between local moments. PMID:26206589

  13. Ultrafast terahertz control of extreme tunnel currents through single atoms on a silicon surface

    DEFF Research Database (Denmark)

    Jelic, Vedran; Iwaszczuk, Krzysztof; Nguyen, Peter H.

    2017-01-01

    Ultrafast control of current on the atomic scale is essential for future innovations in nanoelectronics. Extremely localized transient electric fields on the nanoscale can be achieved by coupling picosecond duration terahertz pulses to metallic nanostructures. Here, we demonstrate terahertz...... scanning tunnelling microscopy (THz-STM) in ultrahigh vacuum as a new platform for exploring ultrafast non-equilibrium tunnelling dynamics with atomic precision. Extreme terahertz-pulse-driven tunnel currents up to 10(7) times larger than steady-state currents in conventional STM are used to image...... individual atoms on a silicon surface with 0.3nm spatial resolution. At terahertz frequencies, the metallic-like Si(111)-(7 x 7) surface is unable to screen the electric field from the bulk, resulting in a terahertz tunnel conductance that is fundamentally different than that of the steady state. Ultrafast...

  14. Surface morphology study on CdZnTe crystals by atomic force microscopy

    Energy Technology Data Exchange (ETDEWEB)

    Azoulay, M.; George, M.A.; Burger, A.; Collins, W.E.; Silberman, E. [Fisk Univ., Nashville, TN (United States)

    1993-03-01

    The study of the crystal surface morphology of CdZnTe is important for the understanding of the fundamentals of crystal growth in order to improve the crystal quality which is essential in applications such as substrates for epitaxy or performance of devices, i.e., room temperature nuclear spectrometers. We present a first atomic force microscopy study on CdZnTe. Cleaved (110) surfaces were imaged in the ambient and an atomic layer step structure was revealed. The effects of thermal annealing on the atomic steps together with Te precipitation along these steps are discussed in terms of deformation due to stress relief and the diffusion of tellurium precipitates. 12 refs., 3 figs.

  15. Improvement and protection of niobium surface superconductivity by atomic layer deposition and heat treatment

    Energy Technology Data Exchange (ETDEWEB)

    Proslier, T.; /IIT, Chicago /Argonne; Zasadzinski, J.; /IIT, Chicago; Moore, J.; Pellin, M.; Elam, J.; /Argonne; Cooley, L.; /Fermilab; Antoine, C.; /Saclay

    2008-11-01

    A method to treat the surface of Nb is described, which potentially can improve the performance of superconducting rf cavities. We present tunneling and x-ray photoemission spectroscopy measurements at the surface of cavity-grade niobium samples coated with a 3 nm alumina overlayer deposited by atomic layer deposition. The coated samples baked in ultrahigh vacuum at low temperature degraded superconducting surface. However, at temperatures above 450 C, the tunneling conductance curves show significant improvements in the superconducting density of states compared with untreated surfaces.

  16. Track sensitivity and the surface roughness measurements of CR-39 with atomic force microscope

    CERN Document Server

    Yasuda, N; Amemiya, K; Takahashi, H; Kyan, A; Ogura, K

    1999-01-01

    Atomic Force Microscope (AFM) has been applied to evaluate the surface roughness and the track sensitivity of CR-39 track detector. We experimentally confirmed the inverse correlation between the track sensitivity and the roughness of the detector surface after etching. The surface of CR-39 (CR-39 doped with antioxidant (HARZLAS (TD-1)) and copolymer of CR-39/NIPAAm (TNF-1)) with high sensitivity becomes rough by the etching, while the pure CR-39 (BARYOTRAK) with low sensitivity keeps its original surface clarity even for the long etching.

  17. Behaviour of oxygen atoms near the surface of nanostructured Nb2O5

    International Nuclear Information System (INIS)

    Cvelbar, U; Mozetic, M

    2007-01-01

    Recombination of neutral oxygen atoms on oxidized niobium foil was studied. Three sets of samples have been prepared: a set of niobium foils with a film of polycrystalline niobium oxide with a thickness of 40 nm, another one with a film thickness of about 2 μm and a set of foils covered with dense bundles of single-crystal Nb 2 O 3 nanowires. All the samples were prepared by oxidation of a pure niobium foil. The samples with a thin oxide film were prepared by exposure of as-received foils to a flux of O-atoms, the samples with a thick polycrystalline niobium oxide were prepared by baking the foils in air at a temperature of 800 deg. C, while the samples covered with nanowires were prepared by oxidation in a highly reactive oxygen plasma. The samples were exposed to neutral oxygen atoms from a remote oxygen plasma source. Depending on discharge parameters, the O-atom density in the postglow chamber, as measured with a catalytic probe, was between 5 x 10 20 and 8 x 10 21 m -3 . The O-atom density in the chamber without the samples was found rather independent of the probe position. The presence of the samples caused a decrease in the O-atom density. Depending on the distance from the samples, the O-atom density was decreased up to 5 times. The O-atom density also depended on the surface morphology of the samples. The strongest decrease in the O-atom density was observed with the samples covered with dense bundles of nanowires. The results clearly showed that niobium oxide nanowires exhibit excellent catalytic behaviour for neutral radicals and can be used as catalysts of exhaust radicals found in many applications

  18. First principles predictions of electron tunneling rates between atoms and crystalline surfaces

    Science.gov (United States)

    Neidfeldt, Keith

    Charge transfer is a critical process that controls many important reactions such as photosynthesis, corrosion, and catalysis. We developed a quantitative method for calculating charge transfer rates using periodic density functional theory (DFT). This approach allows us to model from first principles the interaction between an adsorbate and arbitrary material surfaces. By deconvoluting the projected density of states of the ionization level of the atom, we can determine its width, which is proportional to the charge transfer rate. These rates can be used to predict important properties such as adsorbate excited state lifetimes and neutralization fractions for scattered ions. By comparing neutralization fractions for Li scattering off of Al(001) to experimental data, we validated our first principles method of predicting charge transfer rates. While our results are consistent with the classic Langmuir-Gurney (LG) model of adsorption for nearly-free-electron-like metal surfaces, we find several important deviations caused by the actual electronic structure of more complicated material surfaces. For example, we find that the d-band of transition metal surfaces mediates an intra-atomic hybridization of the Li ionization level. Secondly, we find that surface-projected band gaps (e.g., in Cu(111)) enhance the lifetimes of alkali atoms above surfaces containing such band gaps. In addition, our method allows us to also study atoms interacting with non-metallic surfaces where the LG model does not apply. For example, we find that alkali charge transfer rates are controlled by dangling bonds on covalently-bonded surfaces (e.g., Si(001)-(2xl)) instead of by the traditional image potential.

  19. On surface-initiated atom transfer radical polymerization using diazonium chemistry to introduce the initiator layer

    DEFF Research Database (Denmark)

    Iruthayaraj, Joseph; Chernyy, Sergey; Lillethorup, Mie

    2011-01-01

    This work features the controllability of surface-initiated atom transfer radical polymerization (SI-ATRP) of methyl methacrylate, initiated by a multilayered 2-bromoisobutyryl moiety formed via diazonium chemistry. The thickness as a function of polymerization time has been studied by varying...

  20. Protein repellent hydrophilic grafts prepared by surface-initiated atom transfer radical polymerization from polypropylene

    DEFF Research Database (Denmark)

    Fristrup, Charlotte Juel; Jankova Atanasova, Katja; Eskimergen, Rüya

    2012-01-01

    Grafting of poly(ethylene glycol)methacrylate (PEGMA) and N,N-dimethylacrylamide (DMAAm) from UV-initiator modified polypropylene (PP) was performed by Surface-Initiated Atom Transfer Radical Polymerization (SI-ATRP). The modification and hydrophilization of the PP substrates were confirmed...

  1. Polymer coating comprising 2-methoxyethyl acrylate units synthesized by surface-initiated atom transfer radical polymerization

    DEFF Research Database (Denmark)

    2011-01-01

    Source: US2012184029A The present invention relates to preparation of a polymer coating comprising or consisting of polymer chains comprising or consisting of units of 2-methoxyethyl acrylate synthesized by Surface-Initiated Atom Transfer Radical Polymerization (SI ATRP) such as ARGET SI ATRP...... or AGET SI ATRP and uses of said polymer coating....

  2. Atomic interactions at the (100) diamond surface and the impact of surface and interface changes on the electronic transport properties

    Science.gov (United States)

    Deferme, Wim

    Centuries and centuries already, diamond is a material that speaks to ones imagination. Till the 18th century it was only mined in India, after it was also found in Brazil and South-Africa. But along the fascinating properties of diamond, it is also a very interesting material for industry. After the discovery at the end of the 18th century that diamond consists of carbon, it took until the 50's of the previous century before research groups from Russia, Japan and the USA were able to reproduce the growth process of diamond. In 1989 it was discovered that the surface of intrinsic, insulation diamond can be made conductive by hydrogenating the surface. It was clear that not only hydrogen at the surface but also the so called "adsorbates" were responsible for this conductivity. It was still not completely clear what was the influence of other species (like oxygen) on the mechanism of surface conductivity and therefore in this thesis the influence of oxygen on the electronic transport properties of atomically flat diamond are researched. Besides the growth of atomically flat diamond with the use of CVD (chemical vapour deposition) en the study of the grown surfaces with characterising techniques such as AFM (atomic force microscopy) and STM (scanning tunnelling microscopy), the study of the surface treatment with plasma techniques is the main topic of this thesis. The influence of oxygen on the surface conductivity is studied and with the ToF (Time-of-Flight) technique the transport properties of the freestanding diamond are examined. With a short laserflash, electrons and holes are created at the diamond/aluminium interface and due to an electric field (up to 500V) the charge carriers are translated to the back contact. In this way the influence of the surface and the changes at the aluminum contacts is studied leading to very interesting results.

  3. Electrodeposition of Pd based binary catalysts on Carbon paper via surface limited redox-replacement reaction for oxygen reduction reaction

    CSIR Research Space (South Africa)

    Modibedi, RM

    2014-05-01

    Full Text Available attention as it is more abundant and also cheaper than Pt. In this presentation, Electrochemical Atomic Layer Deposition (ECALD) was used in the preparation of binary ORR catalysts. The binary nanoclusters were synthesised via surface-limited redox-replacement...

  4. Preservation of atomically clean silicon surfaces in air by contact bonding

    DEFF Research Database (Denmark)

    Grey, Francois; Ljungberg, Karin

    1997-01-01

    When two hydrogen-passivated silicon surfaces are placed in contact under cleanroom conditions, a weak bond is formed. Cleaving this bond under ultrahigh vacuum (UHV) conditions, and observing the surfaces with low energy electron diffraction and scanning tunneling microscopy, we find that the or......When two hydrogen-passivated silicon surfaces are placed in contact under cleanroom conditions, a weak bond is formed. Cleaving this bond under ultrahigh vacuum (UHV) conditions, and observing the surfaces with low energy electron diffraction and scanning tunneling microscopy, we find...... that the ordered atomic structure of the surfaces is protected from oxidation, even after the bonded samples have been in air for weeks. Further, we show that silicon surfaces that have been cleaned and hydrogen-passivated in UHV can be contacted in UHV in a similarly hermetic fashion, protecting the surface...

  5. Atomic force microscopy characterization of the surface wettability of natural fibres

    International Nuclear Information System (INIS)

    Pietak, Alexis; Korte, Sandra; Tan, Emelyn; Downard, Alison; Staiger, Mark P.

    2007-01-01

    Natural fibres represent a readily available source of ecologically friendly and inexpensive reinforcement in composites with degradable thermoplastics, however chemical treatments of fibres are required to prepare feasible composites. It is desirable to characterize the surface wettability of fibres after chemical treatment as the polarity of cellulose-based fibres influences compatibility with a polymer matrix. Assessment of the surface wettability of natural fibres using conventional methods presents a challenge as the surfaces are morphologically and chemically heterogeneous, rough, and can be strongly wicking. In this work it is shown that under atmospheric conditions the adhesion force between an atomic force microscopy (AFM) tip and the fibre surface can estimate the water contact angle and surface wettability of the fibre. AFM adhesion force measurements are suitable for the more difficult surfaces of natural fibres and in addition allow for correlations between microstructural features and surface wettability characteristics

  6. Engineering the Eigenstates of Coupled Spin-1 /2 Atoms on a Surface

    Science.gov (United States)

    Yang, Kai; Bae, Yujeong; Paul, William; Natterer, Fabian D.; Willke, Philip; Lado, Jose L.; Ferrón, Alejandro; Choi, Taeyoung; Fernández-Rossier, Joaquín; Heinrich, Andreas J.; Lutz, Christopher P.

    2017-12-01

    Quantum spin networks having engineered geometries and interactions are eagerly pursued for quantum simulation and access to emergent quantum phenomena such as spin liquids. Spin-1 /2 centers are particularly desirable, because they readily manifest coherent quantum fluctuations. Here we introduce a controllable spin-1 /2 architecture consisting of titanium atoms on a magnesium oxide surface. We tailor the spin interactions by atomic-precision positioning using a scanning tunneling microscope (STM) and subsequently perform electron spin resonance on individual atoms to drive transitions into and out of quantum eigenstates of the coupled-spin system. Interactions between the atoms are mapped over a range of distances extending from highly anisotropic dipole coupling to strong exchange coupling. The local magnetic field of the magnetic STM tip serves to precisely tune the superposition states of a pair of spins. The precise control of the spin-spin interactions and ability to probe the states of the coupled-spin network by addressing individual spins will enable the exploration of quantum many-body systems based on networks of spin-1 /2 atoms on surfaces.

  7. Quantitative measurements of ground state atomic oxygen in atmospheric pressure surface micro-discharge array

    Science.gov (United States)

    Li, D.; Kong, M. G.; Britun, N.; Snyders, R.; Leys, C.; Nikiforov, A.

    2017-06-01

    The generation of atomic oxygen in an array of surface micro-discharge, working in atmospheric pressure He/O2 or Ar/O2 mixtures, is investigated. The absolute atomic oxygen density and its temporal and spatial dynamics are studied by means of two-photon absorption laser-induced fluorescence. A high density of atomic oxygen is detected in the He/O2 mixture with up to 10% O2 content in the feed gas, whereas the atomic oxygen concentration in the Ar/O2 mixture stays below the detection limit of 1013 cm-3. The measured O density near the electrode under the optimal conditions in He/1.75% O2 gas is 4.26  ×  1015 cm-3. The existence of the ground state O (2p 4 3 P) species has been proven in the discharge at a distance up to 12 mm away from the electrodes. Dissociative reactions of the singlet O2 with O3 and deep vacuum ultraviolet radiation, including the radiation of excimer \\text{He}2\\ast , are proposed to be responsible for O (2p 4 3 P) production in the far afterglow. A capability of the surface micro-discharge array delivering atomic oxygen to long distances over a large area is considered very interesting for various biomedical applications.

  8. Engineering the Eigenstates of Coupled Spin-1/2 Atoms on a Surface.

    Science.gov (United States)

    Yang, Kai; Bae, Yujeong; Paul, William; Natterer, Fabian D; Willke, Philip; Lado, Jose L; Ferrón, Alejandro; Choi, Taeyoung; Fernández-Rossier, Joaquín; Heinrich, Andreas J; Lutz, Christopher P

    2017-12-01

    Quantum spin networks having engineered geometries and interactions are eagerly pursued for quantum simulation and access to emergent quantum phenomena such as spin liquids. Spin-1/2 centers are particularly desirable, because they readily manifest coherent quantum fluctuations. Here we introduce a controllable spin-1/2 architecture consisting of titanium atoms on a magnesium oxide surface. We tailor the spin interactions by atomic-precision positioning using a scanning tunneling microscope (STM) and subsequently perform electron spin resonance on individual atoms to drive transitions into and out of quantum eigenstates of the coupled-spin system. Interactions between the atoms are mapped over a range of distances extending from highly anisotropic dipole coupling to strong exchange coupling. The local magnetic field of the magnetic STM tip serves to precisely tune the superposition states of a pair of spins. The precise control of the spin-spin interactions and ability to probe the states of the coupled-spin network by addressing individual spins will enable the exploration of quantum many-body systems based on networks of spin-1/2 atoms on surfaces.

  9. First-principles study of small palladium clusters on NiAl(1 1 0) alloy surface

    Science.gov (United States)

    Wu, Ping; Cao, Gengyu; Tang, Fuling; Huang, Min

    2013-09-01

    Theoretical calculations focused on the geometry, stability, electronic and magnetic properties of small palladium clusters Pdn (n=1-5) adsorbed on the NiAl(1 1 0) alloy surface were carried out within the framework of density functional theory (DFT). In agreement with the experimental observations, both Ni-bridge and Al-bridge sites are preferential for the adsorption of single palladium atom, with an adsorption energy difference of 0.04 eV. Among the possible structures considered for Pdn (n=1-5) clusters adsorbed on NiAl(1 1 0) surface, Pd atoms tend to form one-dimensional (1D) chain structure at low coverage (from Pd1 to Pd3) and two-dimensional (2D) structures are more stable than three-dimensional (3D) structures for Pd4 and Pd5. Furthermore, metal-substrate bonding prevails over metal-metal bonding for Pd cluster adsorbed on NiAl(1 1 0) surface. The density of states for Pd atoms of Pd/NiAl(1 1 0) system are strongly affected by their chemical environment. The magnetic feature emerged upon the adsorption of Pd clusters on NiAl(1 1 0) surface was due to the charge transfer between Pd atoms and the substrate. These findings may shade light on the understanding of the growth of Pd metal clusters on alloy surface and the construction of nanoscale devices.

  10. Spin-split Surface States and Superconductivity at Twin Boundaries of Non-centrosymmetric BiPd

    Science.gov (United States)

    Yim, Chi Ming; Trainer, Christopher; Maldonado, Ana; Peets, Darren C.; Wahl, Peter

    In non-magnetic bulk materials lacking a center of inversion symmetry, spin-orbit interactions can lift the spin degeneracy, resulting in Rashba metals whose Fermi surfaces exhibit an intricate spin texture. Combined with superconductivity, this can lead to an admixture of both singlet and triplet components of the superconducting pairing. Using scanning tunneling spectroscopy we study the surface electronic structure in the superconducting state of BiPd, which has previously been reported to exhibit a Dirac-like surface state with a non-trivial spin texture. Topographic images reveal domains of [0 1 0] and [010] terminations corresponding to opposing faces of the crystal structure, separated by twin boundaries. From differential conductance spectra obtained on the two terminations we can characterize the surface electronic structure of the two non-equivalent surfaces. The signature of the surface state within domains of the two terminations are located at 0.4 eV above the Fermi level with only small differences. Intriguingly, we find an additional bound state localized at the twin boundary, the precise energy of which depends on the orientation of the twin boundary. Superconductivity between the two surface terminations and at the twin boundaries is discussed.

  11. Magnetic Interaction between Surface-Engineered Rare-Earth Atomic Spins

    Directory of Open Access Journals (Sweden)

    Chiung-Yuan Lin

    2012-06-01

    Full Text Available We report the ab-initio study of rare-earth adatoms (Gd on an insulating surface. This surface is of interest because of previous studies by scanning tunneling microscopy showing spin excitations of transition-metal adatoms. The present work is the first study of rare-earth spin-coupled adatoms, as well as the geometry effect of spin coupling and the underlying mechanism of ferromagnetic coupling. The exchange coupling between Gd atoms on the surface is calculated to be antiferromagnetic in a linear geometry and ferromagnetic in a diagonal geometry. We also find that the Gd dimers in these two geometries are similar to the nearest-neighbor and the next-nearest-neighbor Gd atoms in GdN bulk. We analyze how much direct exchange, superexchange, and Ruderman-Kittel-Kasuya-Yosida interactions contribute to the exchange coupling for both geometries by additional first-principles calculations of related model systems.

  12. Formation of nanostructures on HOPG surface in presence of surfactant atom during low energy ion irradiation

    Energy Technology Data Exchange (ETDEWEB)

    Ranjan, M., E-mail: ranjanm@ipr.res.in; Joshi, P.; Mukherjee, S.

    2016-07-15

    Low energy ions beam often develop periodic patterns on surfaces under normal or off-normal incidence. Formation of such periodic patterns depends on the substrate material, the ion beam parameters, and the processing conditions. Processing conditions introduce unwanted contaminant atoms, which also play strong role in pattern formation by changing the effective sputtering yield of the material. In this work we have analysed the effect of Cu, Fe and Al impurities introduced during low energy Ar{sup +} ion irradiation on HOPG substrate. It is observed that by changing the species of foreign atoms the surface topography changes drastically. The observed surface topography is co-related with the modified sputtering yield of HOPG. Presence of Cu and Fe amplify the effective sputtering yield of HOPG, so that the required threshold for the pattern formation is achieved with the given fluence, whereas Al does not lead to any significant change in the effective yield and hence no pattern formation occurs.

  13. Apparatus and method for atmospheric pressure reactive atom plasma processing for shaping of damage free surfaces

    Science.gov (United States)

    Carr,; Jeffrey, W [Livermore, CA

    2009-03-31

    Fabrication apparatus and methods are disclosed for shaping and finishing difficult materials with no subsurface damage. The apparatus and methods use an atmospheric pressure mixed gas plasma discharge as a sub-aperture polisher of, for example, fused silica and single crystal silicon, silicon carbide and other materials. In one example, workpiece material is removed at the atomic level through reaction with fluorine atoms. In this example, these reactive species are produced by a noble gas plasma from trace constituent fluorocarbons or other fluorine containing gases added to the host argon matrix. The products of the reaction are gas phase compounds that flow from the surface of the workpiece, exposing fresh material to the etchant without condensation and redeposition on the newly created surface. The discharge provides a stable and predictable distribution of reactive species permitting the generation of a predetermined surface by translating the plasma across the workpiece along a calculated path.

  14. Reversal of atomic contrast in scanning probe microscopy on (111) metal surfaces

    Czech Academy of Sciences Publication Activity Database

    Ondráček, Martin; González, C.; Jelínek, Pavel

    2012-01-01

    Roč. 24, 08 (2012), 084003/1-084003/7 ISSN 0953-8984 R&D Projects: GA ČR(CZ) GPP204/11/P578; GA ČR GAP204/10/0952; GA ČR GA202/09/0545; GA MŠk(CZ) ME10076 Grant - others:AVČR(CZ) M100100904 Institutional research plan: CEZ:AV0Z10100521 Keywords : atomic force microscopy * metallic surfaces * atomic contrast * scanning tunneling microscopy Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 2.355, year: 2012 http://iopscience.iop.org/0953-8984/24/8/084003

  15. Exploring a potential energy surface by machine learning for characterizing atomic transport

    Science.gov (United States)

    Kanamori, Kenta; Toyoura, Kazuaki; Honda, Junya; Hattori, Kazuki; Seko, Atsuto; Karasuyama, Masayuki; Shitara, Kazuki; Shiga, Motoki; Kuwabara, Akihide; Takeuchi, Ichiro

    2018-03-01

    We propose a machine-learning method for evaluating the potential barrier governing atomic transport based on the preferential selection of dominant points for atomic transport. The proposed method generates numerous random samples of the entire potential energy surface (PES) from a probabilistic Gaussian process model of the PES, which enables defining the likelihood of the dominant points. The robustness and efficiency of the method are demonstrated on a dozen model cases for proton diffusion in oxides, in comparison with a conventional nudge elastic band method.

  16. Investigation of graphite composite anodes surfaces by atomic force microscopy and related techniques

    Energy Technology Data Exchange (ETDEWEB)

    Hirasawa, Karen Akemi; Nishioka, Keiko; Sato, Tomohiro; Yamaguchi, Shoji; Mori, Shoichiro [Mitsubishi Chemical Corp., Tsukuba Research Center, Ibaraki (Japan)

    1997-11-01

    The surface of a synthetic graphite (KS-44) and polyvinylidene difluoride binder (PVDF) anode for lithium-ion secondary batteries is imaged using atomic force microscopy (AFM) and several related scanning probe microscope (SPM) instruments including: dynamic force microscopy (DFM), friction force microscopy (FFM), laterally-modulated friction force microscopy (LM-FFM), visco-elasticity atomic force microscopy (VE-AFM), and AFM/simultaneous current measurement mode (SCM). DFM is found to be an exceptional mode for topographic imaging while FFM results in the clearest contrast distinction between PVDF binder and KS-44 graphite regions. (orig.)

  17. Effective adsorption/electrocatalytic degradation of perchlorate using Pd/Pt supported on N-doped activated carbon fiber cathode

    International Nuclear Information System (INIS)

    Yao, Fubing; Zhong, Yu; Yang, Qi; Wang, Dongbo; Chen, Fei; Zhao, Jianwei; Xie, Ting; Jiang, Chen; An, Hongxue; Zeng, Guangming; Li, Xiaoming

    2017-01-01

    Highlights: • Pd/Pt-NACF served as an adsorption/electrocatalysis electrode to reduce perchlorate. • The possible mechanisms involved in the reaction process were explained. • The reusability and stability of Pd/Pt-NACF bifunctional material was evaluated. - Abstract: In this work, Pd/Pt supported on N-doped activated carbon fiber (Pd/Pt-NACF) was employed as the electrode for electrocatalytic degradation of perchlorate through adsorption/electroreduction process. Perchlorate in solution was firstly adsorbed on Pd/Pt-NACF and then reduced to non-toxic chloride by the catalytic function of Pd/Pt at a constant current (20 mA). Compared with Pd/Pt-ACF, the adsorption capacity and electrocatalytic degradation efficiency of Pd/Pt-NACF for perchlorate increased 161% and 28%, respectively. Obviously, positively charged N-functional groups on NACF surface enhanced the adsorption capacity of Pd/Pt-NACF, and the dissociation of hydrogen to atomic H* by the Pd/Pt nanostructures on the cathode might drastically promote the electrocatalytic reduction of perchlorate. The role of atomic H* in the electroreduction process was identified by tertiary butanol inhibition test. Meanwhile, the perchlorate degradation performance was not substantially lower after three successive adsorption/electrocatalytic degradation experiments, demonstrating the electrochemical reusability and stability of the as-prepared electrode. These results showed that Pd/Pt-NACF was effective for electrocatalytic degradation of perchlorate and had great potential in perchlorate removal from water.

  18. Stripping scattering of fast atoms on surfaces of metal-oxide crystals and ultrathin films; Streifende Streuung schneller Atome an Oberflaechen von Metalloxid-Kristallen und ultraduennen Filmen

    Energy Technology Data Exchange (ETDEWEB)

    Blauth, David

    2010-03-11

    In the framework of the present dissertation the interactions of fast atoms with surfaces of bulk oxides, metals and thin films on metals were studied. The experiments were performed in the regime of grazing incidence of atoms with energies of some keV. The advantage of this scattering geometry is the high surface sensibility and thus the possibility to determine the crystallographic and electronic characteristics of the topmost surface layer. In addition to these experiments, the energy loss and the electron emission induced by scattered projectiles was investigated. The energy for electron emission and exciton excitation on Alumina/NiAl(110) and SiO{sub 2}/Mo(112) are determined. By detection of the number of projectile induced emitted electrons as function of azimuthal angle for the rotation of the target surface, the geometrical structure of atoms forming the topmost layer of different adsorbate films on metal surfaces where determined via ion beam triangulation. (orig.)

  19. Molecular dynamics study of the interactions of incident N or Ti atoms with the TiN(001) surface

    Energy Technology Data Exchange (ETDEWEB)

    Xu, Zhenhai [National Key Laboratory for Precision Hot Processing of Metals & School of Materials Science and Engineering, Harbin Institute of Technology, Harbin 150001 (China); School of Mechatronics Engineering, Harbin Institute of Technology, Harbin 150001 (China); Centre for Precision Manufacturing, Department of Design, Manufacture and Engineering Management, The University of Strathclyde, Glasgow G1 1XJ (United Kingdom); Zeng, Quanren [Centre for Precision Manufacturing, Department of Design, Manufacture and Engineering Management, The University of Strathclyde, Glasgow G1 1XJ (United Kingdom); Yuan, Lin [National Key Laboratory for Precision Hot Processing of Metals & School of Materials Science and Engineering, Harbin Institute of Technology, Harbin 150001 (China); Qin, Yi [Centre for Precision Manufacturing, Department of Design, Manufacture and Engineering Management, The University of Strathclyde, Glasgow G1 1XJ (United Kingdom); Chen, Mingjun [School of Mechatronics Engineering, Harbin Institute of Technology, Harbin 150001 (China); Shan, Debin, E-mail: d.b.shan@gmail.com [National Key Laboratory for Precision Hot Processing of Metals & School of Materials Science and Engineering, Harbin Institute of Technology, Harbin 150001 (China)

    2016-01-01

    Graphical abstract: - Highlights: • Interactions of incident N or Ti atoms with TiN(001) surface are studied by CMD. • The impact position of incident N on the surface determines the interaction modes. • Adsorption could occur due to the atomic exchange process. • Resputtering and reflection may simultaneously occur. • The initial sticking coefficient of N on TiN(001) is much smaller than that of Ti. - Abstract: The interaction processes between incident N or Ti atoms and the TiN(001) surface are simulated by classical molecular dynamics based on the second nearest-neighbor modified embedded-atom method potentials. The simulations are carried out for substrate temperatures between 300 and 700 K and kinetic energies of the incident atoms within the range of 0.5–10 eV. When N atoms impact against the surface, adsorption, resputtering and reflection of particles are observed; several unique atomic mechanisms are identified to account for these interactions, in which the adsorption could occur due to the atomic exchange process while the resputtering and reflection may simultaneously occur. The impact position of incident N atoms on the surface plays an important role in determining the interaction modes. Their occurrence probabilities are dependent on the kinetic energy of incident N atoms but independent on the substrate temperature. When Ti atoms are the incident particles, adsorption is the predominant interaction mode between particles and the surface. This results in the much smaller initial sticking coefficient of N atoms on the TiN(001) surface compared with that of Ti atoms. Stoichiometric TiN is promoted by N/Ti flux ratios larger than one.

  20. Atomic-Scale Visualization of Quantum Interference on a Weyl Semimetal Surface by Scanning Tunneling Microscopy.

    Science.gov (United States)

    Zheng, Hao; Xu, Su-Yang; Bian, Guang; Guo, Cheng; Chang, Guoqing; Sanchez, Daniel S; Belopolski, Ilya; Lee, Chi-Cheng; Huang, Shin-Ming; Zhang, Xiao; Sankar, Raman; Alidoust, Nasser; Chang, Tay-Rong; Wu, Fan; Neupert, Titus; Chou, Fangcheng; Jeng, Horng-Tay; Yao, Nan; Bansil, Arun; Jia, Shuang; Lin, Hsin; Hasan, M Zahid

    2016-01-26

    Weyl semimetals may open a new era in condensed matter physics, materials science, and nanotechnology after graphene and topological insulators. We report the first atomic scale view of the surface states of a Weyl semimetal (NbP) using scanning tunneling microscopy/spectroscopy. We observe coherent quantum interference patterns that arise from the scattering of quasiparticles near point defects on the surface. The measurements reveal the surface electronic structure both below and above the chemical potential in both real and reciprocal spaces. Moreover, the interference maps uncover the scattering processes of NbP's exotic surface states. Through comparison between experimental data and theoretical calculations, we further discover that the orbital and/or spin texture of the surface bands may suppress certain scattering channels on NbP. These results provide a comprehensive understanding of electronic properties on Weyl semimetal surfaces.

  1. Mapping Hydrophobicity on the Protein Molecular Surface at Atom-Level Resolution

    Science.gov (United States)

    Nicolau Jr., Dan V.; Paszek, Ewa; Fulga, Florin; Nicolau, Dan V.

    2014-01-01

    A precise representation of the spatial distribution of hydrophobicity, hydrophilicity and charges on the molecular surface of proteins is critical for the understanding of the interaction with small molecules and larger systems. The representation of hydrophobicity is rarely done at atom-level, as this property is generally assigned to residues. A new methodology for the derivation of atomic hydrophobicity from any amino acid-based hydrophobicity scale was used to derive 8 sets of atomic hydrophobicities, one of which was used to generate the molecular surfaces for 35 proteins with convex structures, 5 of which, i.e., lysozyme, ribonuclease, hemoglobin, albumin and IgG, have been analyzed in more detail. Sets of the molecular surfaces of the model proteins have been constructed using spherical probes with increasingly large radii, from 1.4 to 20 Å, followed by the quantification of (i) the surface hydrophobicity; (ii) their respective molecular surface areas, i.e., total, hydrophilic and hydrophobic area; and (iii) their relative densities, i.e., divided by the total molecular area; or specific densities, i.e., divided by property-specific area. Compared with the amino acid-based formalism, the atom-level description reveals molecular surfaces which (i) present an approximately two times more hydrophilic areas; with (ii) less extended, but between 2 to 5 times more intense hydrophilic patches; and (iii) 3 to 20 times more extended hydrophobic areas. The hydrophobic areas are also approximately 2 times more hydrophobicity-intense. This, more pronounced “leopard skin”-like, design of the protein molecular surface has been confirmed by comparing the results for a restricted set of homologous proteins, i.e., hemoglobins diverging by only one residue (Trp37). These results suggest that the representation of hydrophobicity on the protein molecular surfaces at atom-level resolution, coupled with the probing of the molecular surface at different geometric resolutions

  2. Electron mobility on the surface of liquid Helium: influence of surface level atoms and depopulation of lowest subbands

    International Nuclear Information System (INIS)

    Grigoriev, P. D.; Dyugaev, A. M.; Lebedeva, E. V.

    2008-01-01

    The temperature dependence of electron mobility is examined. We calculate the contribution to the electron scattering rate from the surface level atoms (SLAs), proposed in [10]. This contribution is substantial at low temperatures T < 0.5, when the He vapor concentration is exponentially small. We also study the effect of depopulation of the lowest energy subband, which leads to an increase in the electron mobility at high temperature. The results explain certain long-standing discrepancies between the existing theory and experiment on electron mobility on the surface of liquid helium

  3. Methane combustion reactivity during the metal→metallic oxide transformation of Pd-Pt catalysts: Effect of oxygen pressure

    Science.gov (United States)

    Qi, Wenjie; Ran, Jingyu; Zhang, Zhien; Niu, Juntian; Zhang, Peng; Fu, Lijuan; Hu, Bo; Li, Qilai

    2018-03-01

    Density functional theory combined with kinetic models were used to probe different kinetics consequences by which methane activation on different oxygen chemical potential surfaces as oxygen pressure increased. The metallic oxide → metal transformation temperature of Pd-Pt catalysts increased with the increase of the Pd content or/and O2 pressure. The methane conversion rate on Pt catalyst increased and then decreased to a constant value when increasing the O2 pressure, and Pd catalyst showed a poor activity performance in the case of low O2 pressure. Moreover, its activity increased as the oxygen chemical potential for O2 pressure increased in the range of 2.5-10 KPa. For metal clusters, the Csbnd H bond and Odbnd O bond activation steps occurred predominantly on *-* site pairs. The methane conversion rate was determined by O2 pressure because the adsorbed O atoms were rapidly consumed by other adsorbed species in this kinetic regime. As the O2 pressure increased, the metallic active sites for methane activation were decreased and there was no longer lack of adsorbed O atoms, resulting in the decrease of the methane conversion rate. Furthermore, when the metallic surfaces were completely covered by adsorbed oxygen atoms at higher oxygen chemical potentials, Pt catalyst showed a poor activity due to a high Csbnd H bond activation barrier on O*sbnd O*. In the case of high O2 pressure, Pd atoms preferred to segregate to the active surface of Pd-Pt catalysts, leading to the formation of PdO surfaces. The increase of Pd segregation promoted a subsequent increase in active sites and methane conversion rate. The PdO was much more active than metallic and O* saturated surfaces for methane activation, inferred from the theory and experimental study. Pd-rich bimetallic catalyst (75% molar Pd) showed a dual high methane combustion activity on O2-poor and O2-rich conditions.

  4. Magnetic Dichroism of Potassium Atoms on the Surface of Helium Nanodroplets

    International Nuclear Information System (INIS)

    Nagl, Johann; Auboeck, Gerald; Callegari, Carlo; Ernst, Wolfgang E.

    2007-01-01

    The population ratio of Zeeman sublevels of atoms on the surface of superfluid helium droplets (T=0.37 K) has been measured. Laser induced fluorescence spectra of K atoms are measured in the presence of a moderately strong magnetic field (2.9 kG). The relative difference between the two states of circular polarization of the exciting laser is used to determine the electron spin polarization of the ensemble. Equal fluorescence levels indicate that the two spin sublevels of the ground-state K atom are equipopulated, within 1%. Thermalization to 0.37 K would give a population ratio of 0.35. We deduce that the rate of spin relaxation induced by the droplet must be 2 triplet dimer we find instead full thermalization of the spin

  5. Atomic configuration of hydrogenated and clean tantalum(111) surfaces: Bond relaxation, energy entrapment and electron polarization

    Science.gov (United States)

    Bo, Maolin; Li, Lei; Guo, Yongling; Yao, Chuang; Peng, Cheng; Sun, Chang Q.

    2018-01-01

    By studying the tantalum (Ta)(111) surface with X-ray photoemission spectroscopy and density functional theory, we determined binding energy values for the clean Ta(111) (+3.068 eV) and hydrogenated Ta(111) (+3.421 eV) surfaces with an isolated atom level of 18.977 eV. Using the bond-band barrier and zone-selective electron spectroscopy correlation, we investigated the mechanism of hydrogenation adsorption on the Ta(111) surface. We found the local densities of states of the first layer of Ta atoms in the reconstructed structure, which formed on the adsorbent hydrogen of the surface chemical bond contracts and dipole polarization. Moreover, we showed that on the Ta(111) surface, the hydrogen-induced surface core level shifts are dominated by quantum entrapment and are proportional to the calculated hybridized orbitals of the valence band. The latter is therefore correlated to the local surface chemical reactivity and is useful for other adsorbate systems on transition metals.

  6. DNA adsorption and desorption on mica surface studied by atomic force microscopy

    International Nuclear Information System (INIS)

    Sun Lanlan; Zhao Dongxu; Zhang Yue; Xu Fugang; Li Zhuang

    2011-01-01

    The adsorption of DNA molecules on mica surface and the following desorption of DNA molecules at ethanol-mica interface were studied using atomic force microscopy. By changing DNA concentration, different morphologies on mica surface have been observed. A very uniform and orderly monolayer of DNA molecules was constructed on the mica surface with a DNA concentration of 30 ng/μL. When the samples were immersed into ethanol for about 15 min, various desorption degree of DNA from mica (0-99%) was achieved. It was found that with the increase of DNA concentration, the desorption degree of DNA from the mica at ethanol-mica interface decreased. And when the uniform and orderly DNA monolayers were formed on the mica surface, almost no DNA molecule desorbed from the mica surface in this process. The results indicated that the uniform and orderly DNA monolayer is one of the most stable DNA structures formed on the mica surface. In addition, we have studied the structure change of DNA molecules after desorbed from the mica surface with atomic force microscopy, and found that the desorption might be ascribed to the ethanol-induced DNA condensation.

  7. Electrical and Surface Properties of InAs/InSb Nanowires Cleaned by Atomic Hydrogen.

    Science.gov (United States)

    Webb, James L; Knutsson, Johan; Hjort, Martin; Gorji Ghalamestani, Sepideh; Dick, Kimberly A; Timm, Rainer; Mikkelsen, Anders

    2015-08-12

    We present a study of InAs/InSb heterostructured nanowires by X-ray photoemission spectroscopy (XPS), scanning tunneling microscopy (STM), and in-vacuum electrical measurements. Starting with pristine nanowires covered only by the native oxide formed through exposure to ambient air, we investigate the effect of atomic hydrogen cleaning on the surface chemistry and electrical performance. We find that clean and unreconstructed nanowire surfaces can be obtained simultaneously for both InSb and InAs by heating to 380 ± 20 °C under an H2 pressure 2 × 10(-6) mbar. Through electrical measurement of individual nanowires, we observe an increase in conductivity of 2 orders of magnitude by atomic hydrogen cleaning, which we relate through theoretical simulation to the contact-nanowire junction and nanowire surface Fermi level pinning. Our study demonstrates the significant potential of atomic hydrogen cleaning regarding device fabrication when high quality contacts or complete control of the surface structure is required. As hydrogen cleaning has recently been shown to work for many different types of III-V nanowires, our findings should be applicable far beyond the present materials system.

  8. Optically excited structural transition in atomic wires on surfaces at the quantum limit

    Science.gov (United States)

    Frigge, T.; Hafke, B.; Witte, T.; Krenzer, B.; Streubühr, C.; Samad Syed, A.; Mikšić Trontl, V.; Avigo, I.; Zhou, P.; Ligges, M.; von der Linde, D.; Bovensiepen, U.; Horn-von Hoegen, M.; Wippermann, S.; Lücke, A.; Sanna, S.; Gerstmann, U.; Schmidt, W. G.

    2017-03-01

    Transient control over the atomic potential-energy landscapes of solids could lead to new states of matter and to quantum control of nuclear motion on the timescale of lattice vibrations. Recently developed ultrafast time-resolved diffraction techniques combine ultrafast temporal manipulation with atomic-scale spatial resolution and femtosecond temporal resolution. These advances have enabled investigations of photo-induced structural changes in bulk solids that often occur on timescales as short as a few hundred femtoseconds. In contrast, experiments at surfaces and on single atomic layers such as graphene report timescales of structural changes that are orders of magnitude longer. This raises the question of whether the structural response of low-dimensional materials to femtosecond laser excitation is, in general, limited. Here we show that a photo-induced transition from the low- to high-symmetry state of a charge density wave in atomic indium (In) wires supported by a silicon (Si) surface takes place within 350 femtoseconds. The optical excitation breaks and creates In-In bonds, leading to the non-thermal excitation of soft phonon modes, and drives the structural transition in the limit of critically damped nuclear motion through coupling of these soft phonon modes to a manifold of surface and interface phonons that arise from the symmetry breaking at the silicon surface. This finding demonstrates that carefully tuned electronic excitations can create non-equilibrium potential energy surfaces that drive structural dynamics at interfaces in the quantum limit (that is, in a regime in which the nuclear motion is directed and deterministic). This technique could potentially be used to tune the dynamic response of a solid to optical excitation, and has widespread potential application, for example in ultrafast detectors.

  9. Study of the Adsorption of Atoms and Molecules on Silicon Surfaces Crystallographics and Electronic Structure

    CERN Document Server

    Bengio, S

    2003-01-01

    This thesis work has been concerned with adsorption properties of silicon surfaces.The atomic and electronic structure of molecules and atoms adsorbed on Si has been investigated by means of photoemission experiments combined with synchrotron radiation.The quantitative atomic structure determination was held applying the photoelectron diffraction technique.This technique is sensible to the local structure of a reference atomic specie and has elemental and chemical-state specificity.This approach has been applied to three quite different systems with different degrees of complexity, Sb/Si(111) sq root 3x sq root 3R30 sup 0 , H sub 2 O/Si(100)2x1 and NH sub 3 /Si(111)7x7.Our results show that Sb which forms a ( sq root 3 sq root 3)R30 sup 0 phase produces a bulklike-terminated Si(111)1x1 substrate free of stacking faults.Regarding the atomic structure of its interface, this study strongly favours the T4-site milkstool model over the H3 one.An important aspect regarding the H sub 2 O/Si(100)(2x1) system was esta...

  10. The surface reactivity of acrylonitrile with oxygen atoms on an analogue of interstellar dust grains.

    Science.gov (United States)

    Kimber, Helen J.; Toscano, Jutta; Price, Stephen D.

    2018-03-01

    Experiments designed to reveal the low temperature reactivity on the surfaces of interstellar dust grains are used to probe the heterogeneous reaction between oxygen atoms and acrylonitrile (C2H3CN, H2C = CH-CN). The reaction is studied at a series of fixed surface temperatures between 14 K and 100 K. After dosing the reactants onto the surface, temperature programmed desorption, coupled with time-of-flight mass spectrometry, reveals the formation of a product with the molecular formula C3H3NO. This product results from the addition of a single oxygen atom to the acrylonitrile reactant. The oxygen atom attack appears to occur exclusively at the C = C double bond, rather than involving the cyano (-CN) group. The absence of reactivity at the cyano site hints that full saturation of organic molecules on dust grains may not always occur in the interstellar medium. Modelling the experimental data provides a reaction probability of 0.007 ± 0.003 for a Langmuir-Hinshelwood style (diffusive) reaction mechanism. Desorption energies for acrylonitrile, oxygen atoms and molecular oxygen, from the multilayer mixed ice their deposition forms, are also extracted from the kinetic model and are 22.7 ± 1.0 kJ mol-1 (2730 ± 120 K), 14.2 ± 1.0 kJ mol-1 (1710 ± 120 K) and 8.5 ± 0.8 kJ mol-1 (1020 ± 100 K) respectively. The kinetic parameters we extract from our experiments indicate that the reaction between atomic oxygen and acrylonitrile could occur on interstellar dust grains on an astrophysical time scale.

  11. Preparation of gallium nitride surfaces for atomic layer deposition of aluminum oxide.

    Science.gov (United States)

    Kerr, A J; Chagarov, E; Gu, S; Kaufman-Osborn, T; Madisetti, S; Wu, J; Asbeck, P M; Oktyabrsky, S; Kummel, A C

    2014-09-14

    A combined wet and dry cleaning process for GaN(0001) has been investigated with XPS and DFT-MD modeling to determine the molecular-level mechanisms for cleaning and the subsequent nucleation of gate oxide atomic layer deposition (ALD). In situ XPS studies show that for the wet sulfur treatment on GaN(0001), sulfur desorbs at room temperature in vacuum prior to gate oxide deposition. Angle resolved depth profiling XPS post-ALD deposition shows that the a-Al2O3 gate oxide bonds directly to the GaN substrate leaving both the gallium surface atoms and the oxide interfacial atoms with XPS chemical shifts consistent with bulk-like charge. These results are in agreement with DFT calculations that predict the oxide/GaN(0001) interface will have bulk-like charges and a low density of band gap states. This passivation is consistent with the oxide restoring the surface gallium atoms to tetrahedral bonding by eliminating the gallium empty dangling bonds on bulk terminated GaN(0001).

  12. Phonon-mediated decay of an atom in a surface-induced potential

    International Nuclear Information System (INIS)

    Kien, Fam Le; Hakuta, K.; Dutta Gupta, S.

    2007-01-01

    We study phonon-mediated transitions between translational levels of an atom in a surface-induced potential. We present a general master equation governing the dynamics of the translational states of the atom. In the framework of the Debye model, we derive compact expressions for the rates for both upward and downward transitions. Numerical calculations for the transition rates are performed for a deep silica-induced potential allowing for a large number of bound levels as well as free states of a cesium atom. The total absorption rate is shown to be determined mainly by the bound-to-bound transitions for deep bound levels and by bound-to-free transitions for shallow bound levels. Moreover, the phonon emission and absorption processes can be orders of magnitude larger for deep bound levels as compared to the shallow bound ones. We also study various types of transitions from free states. We show that, for thermal atomic cesium with a temperature in the range from 100 μK to 400 μK in the vicinity of a silica surface with a temperature of 300 K, the adsorption (free-to-bound decay) rate is about two times larger than the heating (free-to-free upward decay) rate, while the cooling (free-to-free downward decay) rate is negligible

  13. Atomic resolution on the (111 )B surface of mercury cadmium telluride by scanning tunneling microscopy

    Science.gov (United States)

    Zha, Fang-Xing; Hong, Feng; Pan, Bi-Cai; Wang, Yin; Shao, Jun; Shen, Xue-Chu

    2018-01-01

    The real-space atomic surface structure of mercury cadmium telluride was successfully achieved on the (111 )B surface of H g0.78C d0.22Te by ultrahigh-vacuum scanning tunneling microscopy (STM). The work casts light on the reconstructions of the (111 )B surface unraveling a (2 ×2 ) surface reconstruction induced by adatom adsorption of Cd. The other (2 ×2 ) surface reconstruction is clarified to be induced by the single Te vacancy, which is more stable than the reconstruction of multivacancies in contrast to the prevailing view. The simulated STM images are in good agreement with the experiments. We also observed an in situ morphology transition from the (1 ×1 ) structure to those (2 ×2 ) reconstructions, implying the stability of the reconstructions.

  14. Optical spectroscopy study of c(4 x 2) Ge (001)-surfaces, covered with atomic Au wires

    Energy Technology Data Exchange (ETDEWEB)

    Bass, Utz; Meyer, Sebastian; Schaefer, Joerg; Geurts, Jean [Universitaet Wuerzburg, Physikalisches Institut, Am Hubland, 97074 Wuerzburg (Germany); Speiser, Eugen; Esser, Norbert [ISAS, Albert-Einstein-Strasse 9, 12489 Berlin (Germany)

    2011-07-01

    Novel quasi-1D systems like e.g. atomic gold chains on a c(4x2) reconstructed Ge(001)-surfaces enable the investigation of 1D-effects like the possible occurrence of the Luttinger- to Fermi liquid transition. As there is a crucial interplay of the lattice vibrations and the electrical and structural properties on such sensitive systems, phonon dynamics are in the focus of this work. The phonons were addressed by Raman spectroscopy and reveal a clear change from the Ge-oxide layer to the final surface with Au-nano wires. Thermally deoxidizing the Ge-surface under UHV leads to a distinct low-frequency vibration around 65cm-1. Its frequency range and its persistence after Gold deposition in the submonolayer range indicate that this signal is surface related. Additionally, the surface-induced anisotropy of the optical reflectance was complementary investigated by Reflectance-Anisotropy-Spectroscopy (RAS) and IR-ellipsometry.

  15. Surface recombination of oxygen atoms in O2 plasma at increased pressure: II. Vibrational temperature and surface production of ozone

    Science.gov (United States)

    Lopaev, D. V.; Malykhin, E. M.; Zyryanov, S. M.

    2011-01-01

    Ozone production in an oxygen glow discharge in a quartz tube was studied in the pressure range of 10-50 Torr. The O3 density distribution along the tube diameter was measured by UV absorption spectroscopy, and ozone vibrational temperature TV was found comparing the calculated ab initio absorption spectra with the experimental ones. It has been shown that the O3 production mainly occurs on a tube surface whereas ozone is lost in the tube centre where in contrast the electron and oxygen atom densities are maximal. Two models were used to analyse the obtained results. The first one is a kinetic 1D model for the processes occurring near the tube walls with the participation of the main particles: O(3P), O2, O2(1Δg) and O3 molecules in different vibrational states. The agreement of O3 and O(3P) density profiles and TV calculated in the model with observed ones was reached by varying the single model parameter—ozone production probability (\\gamma_{O_{3}}) on the quartz tube surface on the assumption that O3 production occurs mainly in the surface recombination of physisorbed O(3P) and O2. The phenomenological model of the surface processes with the participation of oxygen atoms and molecules including singlet oxygen molecules was also considered to analyse \\gamma_{O_{3}} data obtained in the kinetic model. A good agreement between the experimental data and the data of both models—the kinetic 1D model and the phenomenological surface model—was obtained in the full range of the studied conditions that allowed consideration of the ozone surface production mechanism in more detail. The important role of singlet oxygen in ozone surface production was shown. The O3 surface production rate directly depends on the density of physisorbed oxygen atoms and molecules and can be high with increasing pressure and energy inputted into plasma while simultaneously keeping the surface temperature low enough. Using the special discharge cell design, such an approach opens up the

  16. Surface recombination of oxygen atoms in O2 plasma at increased pressure: II. Vibrational temperature and surface production of ozone

    International Nuclear Information System (INIS)

    Lopaev, D V; Malykhin, E M; Zyryanov, S M

    2011-01-01

    Ozone production in an oxygen glow discharge in a quartz tube was studied in the pressure range of 10-50 Torr. The O 3 density distribution along the tube diameter was measured by UV absorption spectroscopy, and ozone vibrational temperature T V was found comparing the calculated ab initio absorption spectra with the experimental ones. It has been shown that the O 3 production mainly occurs on a tube surface whereas ozone is lost in the tube centre where in contrast the electron and oxygen atom densities are maximal. Two models were used to analyse the obtained results. The first one is a kinetic 1D model for the processes occurring near the tube walls with the participation of the main particles: O( 3 P), O 2 , O 2 ( 1 Δ g ) and O 3 molecules in different vibrational states. The agreement of O 3 and O( 3 P) density profiles and T V calculated in the model with observed ones was reached by varying the single model parameter-ozone production probability (γ O 3 ) on the quartz tube surface on the assumption that O 3 production occurs mainly in the surface recombination of physisorbed O( 3 P) and O 2 . The phenomenological model of the surface processes with the participation of oxygen atoms and molecules including singlet oxygen molecules was also considered to analyse γ O 3 data obtained in the kinetic model. A good agreement between the experimental data and the data of both models-the kinetic 1D model and the phenomenological surface model-was obtained in the full range of the studied conditions that allowed consideration of the ozone surface production mechanism in more detail. The important role of singlet oxygen in ozone surface production was shown. The O 3 surface production rate directly depends on the density of physisorbed oxygen atoms and molecules and can be high with increasing pressure and energy inputted into plasma while simultaneously keeping the surface temperature low enough. Using the special discharge cell design, such an approach opens up

  17. Structural optimization of Ag-Pd clusters based on different potential parameterizations

    Science.gov (United States)

    Wu, Xia; Wu, Yiping; Kai, Xiaoming; Wu, Genhua; Chen, Youcun

    2011-11-01

    The putative stable structures of bimetallic Ag-Pd clusters are investigated. Gupta potential is applied to describe the interatomic interactions in Ag-Pd clusters. Experimental-fitted parameters and density-functional-theory (DFT)-fitted parameters are used to determine the lowest energy structures. Global optimization of Ag mPd n ( m + n = 15) and Ag 3mPd 38-3m ( m = 1-12) clusters is performed using adaptive immune optimization algorithm (AIOA). The growth rules of Ag-Pd clusters for both sets of parameterizations are studied, and the differences of structures and excess energies are compared. With the order parameters adopted to show the atomic distribution in the clusters, it is shown that for both parameterized clusters silver atoms have strong tendencies towards segregating at the surface of the structures. However, for both potentials, the atomic distribution of Ag and Pd atoms in Ag-Pd clusters is different because of the geometrical and symmetrical difference.

  18. Ground state potential energy surfaces around selected atoms from resonant inelastic x-ray scattering.

    Science.gov (United States)

    Schreck, Simon; Pietzsch, Annette; Kennedy, Brian; Såthe, Conny; Miedema, Piter S; Techert, Simone; Strocov, Vladimir N; Schmitt, Thorsten; Hennies, Franz; Rubensson, Jan-Erik; Föhlisch, Alexander

    2016-01-29

    Thermally driven chemistry as well as materials' functionality are determined by the potential energy surface of a systems electronic ground state. This makes the potential energy surface a central and powerful concept in physics, chemistry and materials science. However, direct experimental access to the potential energy surface locally around atomic centers and to its long-range structure are lacking. Here we demonstrate how sub-natural linewidth resonant inelastic soft x-ray scattering at vibrational resolution is utilized to determine ground state potential energy surfaces locally and detect long-range changes of the potentials that are driven by local modifications. We show how the general concept is applicable not only to small isolated molecules such as O2 but also to strongly interacting systems such as the hydrogen bond network in liquid water. The weak perturbation to the potential energy surface through hydrogen bonding is observed as a trend towards softening of the ground state potential around the coordinating atom. The instrumental developments in high resolution resonant inelastic soft x-ray scattering are currently accelerating and will enable broad application of the presented approach. With this multidimensional potential energy surfaces that characterize collective phenomena such as (bio)molecular function or high-temperature superconductivity will become accessible in near future.

  19. Local atomic structure of Pd and Ag in the SiC containment layer of TRISO fuel particles fissioned to 20% burn-up

    Science.gov (United States)

    Seibert, Rachel L.; Terrani, Kurt A.; Velázquez, Daniel; Hunn, John D.; Baldwin, Charles A.; Montgomery, Fred C.; Terry, Jeff

    2018-03-01

    The structure and speciation of fission products within the SiC barrier layer of tristructural-isotropic (TRISO) fuel particles irradiated to 19.6% fissions per initial metal atom (FIMA) burnup in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) was investigated. As-irradiated fuel particles, as well as those subjected to simulated accident scenarios, were examined. The TRISO particles were characterized using synchrotron X-ray absorption fine-structure spectroscopy (XAFS) at the Materials Research Collaborative Access Team (MRCAT) beamline at the Advanced Photon Source. The TRISO particles were produced at Oak Ridge National Laboratory under the Advanced Gas Reactor Fuel Development and Qualification Program and sent to the ATR for irradiation. XAFS measurements on the palladium and silver K-edges were collected using the MRCAT undulator beamline. Analysis of the Pd edge indicated the formation of palladium silicides of the form PdxSi (2 ≤ x ≤ 3). In contrast, Ag was found to be metallic within the SiC shell safety tested to 1700 °C. To the best of our knowledge, this is the first result demonstrating metallic bonding of silver from fissioned samples. Knowledge of these reaction pathways will allow for better simulations of radionuclide transport in the various coating layers of TRISO fuels for next generation nuclear reactors. They may also suggest different ways to modify TRISO particles to improve their fuel performance and to mitigate potential fission product release under both normal operation and accident conditions.

  20. Topography and Mechanical Property Mapping of International Simple Glass Surfaces with Atomic Force Microscopy

    Energy Technology Data Exchange (ETDEWEB)

    Pierce, Eric M [ORNL

    2014-01-01

    Quantitative Nanomechanical Peak Force (PF-QNM) TappingModeTM atomic force microscopy measurements are presented for the first time on polished glass surfaces. The PF-QNM technique allows for topography and mechanical property information to be measured simultaneously at each pixel. Results for the international simple glass which represents a simplified version of SON68 glass suggests an average Young s modulus of 78.8 15.1 GPa is within the experimental error of the modulus measured for SON68 glass (83.6 2 GPa) with conventional approaches. Application of the PF-QNM technique will be extended to in situ glass corrosion experiments with the goal of gaining atomic-scale insights into altered layer development by exploiting the mechanical property differences that exist between silica gel (e.g., altered layer) and pristine glass surface.

  1. Surface sticking probabilities for sputtered atoms of Nb-93 and Rh-103

    Science.gov (United States)

    Weller, M. R.; Tombrello, T. A.

    1979-01-01

    The capture coefficient probabilities for sputtered atoms of Nb-93 and Rh-103 incident on Al2O3 surfaces were measured using the backscattering of MeV heavy ions. In the circumstance where the collecting surface is thickly covered, the sticking probabilities integrated over the energy distribution of sputtered atoms are 0.97 plus or minus 0.01 for Nb-93 and 0.95 plus or minus 0.01 for Rh-103 respectively. In the limit of negligible areal coverage of the collector, the accuracy is less; in this case the sticking probabilities are 0.97 + 0.03 or -0.08 and 0.95 + 0.05 or -0.08.

  2. Second order classical perturbation theory for atom surface scattering: analysis of asymmetry in the angular distribution.

    Science.gov (United States)

    Zhou, Yun; Pollak, Eli; Miret-Artés, Salvador

    2014-01-14

    A second order classical perturbation theory is developed and applied to elastic atom corrugated surface scattering. The resulting theory accounts for experimentally observed asymmetry in the final angular distributions. These include qualitative features, such as reduction of the asymmetry in the intensity of the rainbow peaks with increased incidence energy as well as the asymmetry in the location of the rainbow peaks with respect to the specular scattering angle. The theory is especially applicable to "soft" corrugated potentials. Expressions for the angular distribution are derived for the exponential repulsive and Morse potential models. The theory is implemented numerically to a simplified model of the scattering of an Ar atom from a LiF(100) surface.

  3. XPS study of Pd/Co multilayers: identification of Pd and Co interface bonding states by pattern recognition methods

    Science.gov (United States)

    Lesiak, B.; Zemek, J.; de Haan, P.; Jozwik, A.

    1996-02-01

    Artificially structured magnetic superlattices consisting of ultrathin Pd/Co multilayers with varying thickness exhibit strong perpendicular magnetic anisotropy. This particular property in such systemsis strongly correlated with the structure of the interface and its local environment. In the present work, the interface of Pd/Co in two multilayer system was sampled applying X-ray photoelectron spectroscopy (XPS) and sophisticated pattern recognition methods for spectrum processing, i.e. the k-nearest neighbour rule (kNN) and a clusterization algorithm. For the first time, the fuzzy kNN approach has been applied for investigating surface effects. The above methods consider the lineshape of photoelectron spectra recorded for a set of reference samples, evaluate the criteria for the optimum separation of groups, and identity the unknown samples. Photoelectron Pd 3d and Co 2p spectra were recorded from metallic Pd, Co and CoPd solid solutions with varying concentrations of constituents, and from Pd/Co magnetic multilayers. The applied methods were able to identify the alloying of Pd and Co atoms at the Pd/Co interface of the multilayer systems with different concentrations of component involved. The results obtained indicate that both interfaces have finite thickness, which may influence the magnetic properties of the investigated systems.

  4. Study of the Adsorption of Atoms and Molecules on Silicon Surfaces: Crystallographics and Electronic Structure

    International Nuclear Information System (INIS)

    Bengio, Silvina

    2003-01-01

    This thesis work has been concerned with adsorption properties of silicon surfaces.The atomic and electronic structure of molecules and atoms adsorbed on Si has been investigated by means of photoemission experiments combined with synchrotron radiation.The quantitative atomic structure determination was held applying the photoelectron diffraction technique.This technique is sensible to the local structure of a reference atomic specie and has elemental and chemical-state specificity.This approach has been applied to three quite different systems with different degrees of complexity, Sb/Si(111) √3x √3R30 0 , H 2 O/Si(100)2x1 and NH 3 /Si(111)7x7.Our results show that Sb which forms a ( √3√3)R30 0 phase produces a bulklike-terminated Si(111)1x1 substrate free of stacking faults.Regarding the atomic structure of its interface, this study strongly favours the T4-site milkstool model over the H3 one.An important aspect regarding the H 2 O/Si(100)(2x1) system was establishing the limits of precision with which one can determine not only the location of the adsorbed hydroxyl (OH) species, but also the extent to which this adsorption modifes the asymmetric dimers of the clean surface to which it is bonded.On the Si(111)(7x7) surface the problem is particularly complex because there are several different potentially active sites for NH3 adsorption and fragmentation.The application of the PhD method, however, has shown that the majority of the N atoms are on so-called 'rest atom' sites when deposited at RT.This is consistent with the N in the NH2 chemical state.This investigation represents the first quantitative structural study of any molecular adsorbate on the complex Si(111)(7x7) surface.This atomic structures determination shows the PhD is a powerful tool for the atomic structure determination.The molecular systems interacting with the active sites of the substrate fragments producing a short-range order surface.This long-range disorder is produced by the

  5. Charge transfer and formation of reduced Ce3+ upon adsorption of metal atoms at the ceria (110) surface

    International Nuclear Information System (INIS)

    Nolan, Michael

    2012-01-01

    The modification of cerium dioxide with nanoscale metal clusters is intensely researched for catalysis applications, with gold, silver, and copper having been particularly well studied. The interaction of the metal cluster with ceria is driven principally by a localised interaction between a small number of metal atoms (as small as one) and the surface and understanding the fundamentals of the interaction of metal atoms with ceria surfaces is therefore of great interest. Much attention has been focused on the interaction of metals with the (111) surface of ceria, since this is the most stable surface and can be grown as films, which are probed experimentally. However, nanostructures exposing other surfaces such as (110) show high activity for reactions including CO oxidation and require further study; these nanostructures could be modified by deposition of metal atoms or small clusters, but there is no information to date on the atomic level details of metal-ceria interactions involving the (110) surface. This paper presents the results of density functional theory (DFT) corrected for on-site Coulomb interactions (DFT+U) calculations of the adsorption of a number of different metal atoms at an extended ceria (110) surface; the metals are Au, Ag, Cu, Al, Ga, In, La, Ce, V, Cr, and Fe. Upon adsorption all metals are oxidised, transferring electron(s) to the surface, resulting in localised surface distortions. The precise details depend on the identity of the metal atom. Au, Ag, Cu each transfer one electron to the surface, reducing one Ce ion to Ce 3+ , while of the trivalent metals, Al and La are fully oxidised, but Ga and In are only partially oxidised. Ce and the transition metals are also partially oxidised, with the number of reduced Ce ions possible in this surface no more than three per adsorbed metal atom. The predicted oxidation states of the adsorbed metal atoms should be testable in experiments on ceria nanostructures modified with metal atoms.

  6. Charge transfer and formation of reduced Ce3+ upon adsorption of metal atoms at the ceria (110) surface

    Science.gov (United States)

    Nolan, Michael

    2012-04-01

    The modification of cerium dioxide with nanoscale metal clusters is intensely researched for catalysis applications, with gold, silver, and copper having been particularly well studied. The interaction of the metal cluster with ceria is driven principally by a localised interaction between a small number of metal atoms (as small as one) and the surface and understanding the fundamentals of the interaction of metal atoms with ceria surfaces is therefore of great interest. Much attention has been focused on the interaction of metals with the (111) surface of ceria, since this is the most stable surface and can be grown as films, which are probed experimentally. However, nanostructures exposing other surfaces such as (110) show high activity for reactions including CO oxidation and require further study; these nanostructures could be modified by deposition of metal atoms or small clusters, but there is no information to date on the atomic level details of metal-ceria interactions involving the (110) surface. This paper presents the results of density functional theory (DFT) corrected for on-site Coulomb interactions (DFT+U) calculations of the adsorption of a number of different metal atoms at an extended ceria (110) surface; the metals are Au, Ag, Cu, Al, Ga, In, La, Ce, V, Cr, and Fe. Upon adsorption all metals are oxidised, transferring electron(s) to the surface, resulting in localised surface distortions. The precise details depend on the identity of the metal atom. Au, Ag, Cu each transfer one electron to the surface, reducing one Ce ion to Ce3+, while of the trivalent metals, Al and La are fully oxidised, but Ga and In are only partially oxidised. Ce and the transition metals are also partially oxidised, with the number of reduced Ce ions possible in this surface no more than three per adsorbed metal atom. The predicted oxidation states of the adsorbed metal atoms should be testable in experiments on ceria nanostructures modified with metal atoms.

  7. Lateral and vertical manipulations of single atoms on the Ag(1 1 1) surface with the copper single-atom and trimer-apex tips

    International Nuclear Information System (INIS)

    Xie Yiqun; Yang Tianxing; Ye Xiang; Huang Lei

    2011-01-01

    We study the lateral and vertical manipulations of single Ag and Cu atoms on the Ag(1 1 1) surface with the Cu single-atom and trimer-apex tips using molecular statics simulations. The reliability of the lateral manipulation with the Cu single-atom tip is investigated, and compared with that for the Ag tips. We find that overall the manipulation reliability (MR) increases with the decreasing tip height, and in a wide tip-height range the MR is better than those for both the Ag single-atom and trimer-apex tips. This is due to the stronger attractive force of the Cu tip and its better stability against the interactions with the Ag surface. With the Cu trimer-apex tip, the single Ag and Cu adatoms can be picked up from the flat Ag(1 1 1) surface, and moreover a reversible vertical manipulation of single Ag atoms on the stepped Ag(1 1 1) surface is possible, suggesting a method to modify two-dimensional Ag nanostructures on the Ag(1 1 1) surface with the Cu trimer-apex tip.

  8. Energy spectra and charge states of light atoms scattered by solid surface

    International Nuclear Information System (INIS)

    Parilis, E.S.; Verleger, V.K.

    1980-01-01

    The theories of backscattering and charge state formation of light atoms (H, D, and He) for the energy range 1 keV 0 0 and theta. The dependence of epsilonsub(max) on theta determines the mean effective range for the scattering at the angle theta. The appearance of surface peaks in the energy spectra of neutrals below energy E 0 + , Hsup(*), and H - . (orig.)

  9. Surface passivation of GaAs nanowires by the atomic layer deposition of AlN

    Energy Technology Data Exchange (ETDEWEB)

    Shtrom, I. V., E-mail: igorstrohm@mail.ru; Bouravleuv, A. D. [Russian Academy of Sciences, Ioffe Physical–Technical Institute (Russian Federation); Samsonenko, Yu. B.; Khrebtov, A. I. [Russian Academy of Sciences, St. Petersburg National Research Academic University—Nanotechnology Research and Education Center (Russian Federation); Soshnikov, I. P. [Russian Academy of Sciences, Ioffe Physical–Technical Institute (Russian Federation); Reznik, R. R.; Cirlin, G. E., E-mail: cirlin@beam.ioffe.ru [Russian Academy of Sciences, St. Petersburg National Research Academic University—Nanotechnology Research and Education Center (Russian Federation); Dhaka, V.; Perros, A.; Lipsanen, H. [Aalto University (Finland)

    2016-12-15

    It is shown that the atomic layer deposition of thin AlN layers can be used to passivate the surface states of GaAs nanowires synthesized by molecular-beam epitaxy. Studies of the optical properties of samples by low-temperature photoluminescence measurements shows that the photoluminescence-signal intensity can be increased by a factor of up to five by passivating the nanowires with a 25-Å-thick AlN layer.

  10. Surface Modification of Nanoporous 1,2-Polybutadiene by Atom Transfer Radical Polymerization or Click Chemistry

    DEFF Research Database (Denmark)

    Guo, Fengxiao; Jankova Atanasova, Katja; Schulte, Lars

    2010-01-01

    Surface-initiated atom transfer radical polymerization (ATRP) and click chemistry were used to obtain functional nanoporous polymers based oil nanoporous 1,2-polybutadiene (PB) with gyroid morphology. The ATRP monolith initiator was prepared by immobilizing bromoester initiators onto the pore walls...... ATRP-grafting of hydrophilic polyacrylates and click of MPEG, the originally hydrophobic samples transformed into hydrophilic nanoporous materials. The successful modification was confirmed by infrared spectroscopy, contact angle measurements and measurements of spontaneous water uptake, while...

  11. Adsorption/desorption kinetics of Na atoms on reconstructed Si (111)-7 x 7 surface

    International Nuclear Information System (INIS)

    Chauhan, Amit Kumar Singh; Govind; Shivaprasad, S.M.

    2010-01-01

    Self-assembled nanostructures on a periodic template are fundamentally and technologically important as they put forward the possibility to fabricate and pattern micro/nano-electronics for sensors, ultra high-density memories and nanocatalysts. Alkali-metal (AM) nanostructure grown on a semiconductor surface has received considerable attention because of their simple hydrogen like electronic structure. However, little efforts have been made to understand the fundamental aspects of the growth mechanism of self-assembled nanostructures of AM on semiconductor surfaces. In this paper, we report organized investigation of kinetically controlled room-temperature (RT) adsorption/desorption of sodium (Na) metal atoms on clean reconstructed Si (111)-7 x 7 surface, by X-ray photoelectron spectroscopy (XPS). The RT uptake curve shows a layer-by-layer growth (Frank-vander Merve growth) mode of Na on Si (111)-7 x 7 surfaces and a shift is observed in the binding energy position of Na (1s) spectra. The thermal stability of the Na/Si (111) system was inspected by annealing the system to higher substrate temperatures. Within a temperature range from RT to 350 o C, the temperature induced mobility to the excess Na atoms sitting on top of the bilayer, allowing to arrange themselves. Na atoms desorbed over a wide temperature range of 370 o C, before depleting the Si (111) surface at temperature 720 o C. The acquired valence-band (VB) spectra during Na growth revealed the development of new electronic-states near the Fermi level and desorption leads the termination of these. For Na adsorption up to 2 monolayers, decrease in work function (-1.35 eV) was observed, whereas work function of the system monotonically increases with Na desorption from the Si surface as observed by other studies also. This kinetic and thermodynamic study of Na adsorbed Si (111)-7 x 7 system can be utilized in fabrication of sensors used in night vision devices.

  12. Defects in oxide surfaces studied by atomic force and scanning tunneling microscopy

    Directory of Open Access Journals (Sweden)

    Thomas König

    2011-01-01

    Full Text Available Surfaces of thin oxide films were investigated by means of a dual mode NC-AFM/STM. Apart from imaging the surface termination by NC-AFM with atomic resolution, point defects in magnesium oxide on Ag(001 and line defects in aluminum oxide on NiAl(110, respectively, were thoroughly studied. The contact potential was determined by Kelvin probe force microscopy (KPFM and the electronic structure by scanning tunneling spectroscopy (STS. On magnesium oxide, different color centers, i.e., F0, F+, F2+ and divacancies, have different effects on the contact potential. These differences enabled classification and unambiguous differentiation by KPFM. True atomic resolution shows the topography at line defects in aluminum oxide. At these domain boundaries, STS and KPFM verify F2+-like centers, which have been predicted by density functional theory calculations. Thus, by determining the contact potential and the electronic structure with a spatial resolution in the nanometer range, NC-AFM and STM can be successfully applied on thin oxide films beyond imaging the topography of the surface atoms.

  13. Interactions between nitrogen molecules and barium atoms on Ru (0001) surface

    International Nuclear Information System (INIS)

    Zhao Xinxin; Mi Yiming; Xu Hongxia; Wang Lili; Ren Li; Tao Xiangming; Tan Mingqiu

    2011-01-01

    We had performed first principles calculations on interactions between nitrogen molecules and barium atoms on Ru (0001) surface using density function theory methods. It was shown that effects of barium atoms weakened the bond strength of nitrogen molecules. The bond length of nitrogen molecule increases from 0.113 nm on Ru (001)-N 2 to 0.120 nm on Ru (001)-N 2 /Ba surface. While stretch vibrational frequency of nitrogen molecule decreased from 2222 cm -1 and charge transfer toward nitrogen molecule increased from 0.3 e to 1.1 e. Charge was mainly translated from 6 s orbitals of barium atoms to 4 d orbitals of substrate, which enhanced the hybridization between 4 d and 2 π orbitals and increased the dipole moment of 5 σ and d π orbitals of nitrogen molecule. The molecular dipole moment of nitrogen molecule was increased by -0.136 e Anstrom. It was suggested that barium had some characters to be an electronic promoter on the process of activating nitrogen molecules on Ru (0001) surface. (authors)

  14. Quantitative characterization of the atomic-scale structure of oxyhydroxides in rusts formed on steel surfaces

    International Nuclear Information System (INIS)

    Saito, M.; Suzuki, S.; Kimura, M.; Suzuki, T.; Kihira, H.; Waseda, Y.

    2005-01-01

    Quantitative X-ray structural analysis coupled with anomalous X-ray scattering has been used for characterizing the atomic-scale structure of rust formed on steel surfaces. Samples were prepared from rust layers formed on the surfaces of two commercial steels. X-ray scattered intensity profiles of the two samples showed that the rusts consisted mainly of two types of ferric oxyhydroxide, α-FeOOH and γ-FeOOH. The amounts of these rust components and the realistic atomic arrangements in the components were estimated by fitting both the ordinary and the environmental interference functions with a model structure calculated using the reverse Monte Carlo simulation technique. The two rust components were found to be the network structure formed by FeO 6 octahedral units, the network structure itself deviating from the ideal case. The present results also suggest that the structural analysis method using anomalous X-ray scattering and the reverse Monte Carlo technique is very successful in determining the atomic-scale structure of rusts formed on the steel surfaces

  15. Interaction of scandium and titanium atoms with a carbon surface containing five- and seven-membered rings

    International Nuclear Information System (INIS)

    Krasnov, P. O.; Eliseeva, N. S.; Kuzubov, A. A.

    2012-01-01

    The use of carbon nanotubes coated by atoms of transition metals to store molecular hydrogen is associated with the problem of the aggregation of these atoms, which leads to the formation of metal clusters. The quantum-chemical simulation of cluster models of the carbon surface of a graphene type with scandium and titanium atoms has been performed. It has been shown that the presence of five- and seven-membered rings, in addition to six-membered rings, in these structures makes it possible to strongly suppress the processes of the migration of metal atoms over the surface, preventing their clustering.

  16. Spectral studies on sulfur poisoning of Pd/Mg{sub 6}Ni by NEXAFS and XPS

    Energy Technology Data Exchange (ETDEWEB)

    Yagi, S., E-mail: s-yagi@nucl.nagoya-u.ac.jp [Department of Quantum Engineering, School of Engineering, Nagoya University, Furo-cho, Chikusa-ku, Nagoya 464-8603 (Japan); Synchrotron Radiation Center, Hiroshima University, Kagamiyama, Higashi-Hiroshima 739-0046 (Japan); Nambu, M.; Tsukada, C.; Ogawa, S. [Department of Quantum Engineering, School of Engineering, Nagoya University, Furo-cho, Chikusa-ku, Nagoya 464-8603 (Japan); Kutluk, G.; Namatame, H.; Taniguchi, M. [Synchrotron Radiation Center, Hiroshima University, Kagamiyama, Higashi-Hiroshima 739-0046 (Japan)

    2013-02-15

    We have studied on the hydrogen storage materials based on Mg–Ni alloy and fabricated the sample constructed with the Pd thin layer (TL) on Mg{sub 6}Ni alloy substrate. The adsorption behavior of the dimethyl disulfide (DMS) molecules on the sample has been measured to reveal the sulfur poisoning of the Pd TL/Mg{sub 6}Ni by means of XPS and Sulfur K-edge NEXAFS techniques. The chemisorbed DMS, methanethiolate (MT) and atomic S have been observed on the surface. Especially, it is clear that some atomic S has been oxidized by air and detected the adsorbate of the SO{sub 3}{sup 2−} and SO{sub 4}{sup 2−} species. During exposure to the atmosphere, most of the adsorbed DMS and MT adsorbates desorb from the Pd TL surface. We thus conclude the Pd TL might be able to prevent the hydrogen storage materials from the sulfur poisoning.

  17. Spectral studies on sulfur poisoning of Pd/Mg6Ni by NEXAFS and XPS

    International Nuclear Information System (INIS)

    Yagi, S.; Nambu, M.; Tsukada, C.; Ogawa, S.; Kutluk, G.; Namatame, H.; Taniguchi, M.

    2013-01-01

    We have studied on the hydrogen storage materials based on Mg–Ni alloy and fabricated the sample constructed with the Pd thin layer (TL) on Mg 6 Ni alloy substrate. The adsorption behavior of the dimethyl disulfide (DMS) molecules on the sample has been measured to reveal the sulfur poisoning of the Pd TL/Mg 6 Ni by means of XPS and Sulfur K-edge NEXAFS techniques. The chemisorbed DMS, methanethiolate (MT) and atomic S have been observed on the surface. Especially, it is clear that some atomic S has been oxidized by air and detected the adsorbate of the SO 3 2− and SO 4 2− species. During exposure to the atmosphere, most of the adsorbed DMS and MT adsorbates desorb from the Pd TL surface. We thus conclude the Pd TL might be able to prevent the hydrogen storage materials from the sulfur poisoning.

  18. Low-energy 4He+ scattering from deuterium adsorbed on stepped Pd(331)

    International Nuclear Information System (INIS)

    Ellis, W.P.; Bastasz, R.

    1996-01-01

    We have taken angle-resolved data for the scattering of low-energy ( 4 He + from deuterium adsorbed on a stepped Pd(331) surface. The impact geometry was up the staircase, that is, the 4 He + beam was perpendicular to and directly incident onto the unshadowed Pd ledge atoms. A strong quasi-elastic scattering signal of 4 He + from D ( 4 He + /D) was observed at a forward scattering angle of θ = 25 degrees and an incidence angle of α = 76 degrees from the (331) normal. The results agree with shadow cone calculations of scattering first from Pd ledge atoms followed by a second event, 4 He + /D. The resultant adsorption geometry shows D to reside in the quasi- threefold ledge site on the surface directly above the bulk fcc octahedral void. These results are consistent with the previous 4 He + scattering study of the geometrically related Pd(110)- D(ads) system

  19. Surface tension effect on the mechanical properties of nanomaterials measured by atomic force microscopy

    Science.gov (United States)

    Cuenot, Stéphane; Frétigny, Christian; Demoustier-Champagne, Sophie; Nysten, Bernard

    2004-04-01

    The effect of reduced size on the elastic properties measured on silver and lead nanowires and on polypyrrole nanotubes with an outer diameter ranging between 30 and 250 nm is presented and discussed. Resonant-contact atomic force microscopy (AFM) is used to measure their apparent elastic modulus. The measured modulus of the nanomaterials with smaller diameters is significantly higher than that of the larger ones. The latter is comparable to the macroscopic modulus of the materials. The increase of the apparent elastic modulus for the smaller diameters is attributed to surface tension effects. The surface tension of the probed material may be experimentally determined from these AFM measurements.

  20. Theoretical Models for Surface Forces and Adhesion and Their Measurement Using Atomic Force Microscopy

    Science.gov (United States)

    Leite, Fabio L.; Bueno, Carolina C.; Da Róz, Alessandra L.; Ziemath, Ervino C.; Oliveira, Osvaldo N.

    2012-01-01

    The increasing importance of studies on soft matter and their impact on new technologies, including those associated with nanotechnology, has brought intermolecular and surface forces to the forefront of physics and materials science, for these are the prevailing forces in micro and nanosystems. With experimental methods such as the atomic force spectroscopy (AFS), it is now possible to measure these forces accurately, in addition to providing information on local material properties such as elasticity, hardness and adhesion. This review provides the theoretical and experimental background of AFS, adhesion forces, intermolecular interactions and surface forces in air, vacuum and in solution. PMID:23202925

  1. Theoretical models for surface forces and adhesion and their measurement using atomic force microscopy.

    Science.gov (United States)

    Leite, Fabio L; Bueno, Carolina C; Da Róz, Alessandra L; Ziemath, Ervino C; Oliveira, Osvaldo N

    2012-10-08

    The increasing importance of studies on soft matter and their impact on new technologies, including those associated with nanotechnology, has brought intermolecular and surface forces to the forefront of physics and materials science, for these are the prevailing forces in micro and nanosystems. With experimental methods such as the atomic force spectroscopy (AFS), it is now possible to measure these forces accurately, in addition to providing information on local material properties such as elasticity, hardness and adhesion. This review provides the theoretical and experimental background of afs, adhesion forces, intermolecular interactions and surface forces in air, vacuum and in solution.

  2. Characterization of surface electrochemical reactions used in electrochemical atomic layer epitaxy and digital etching

    Science.gov (United States)

    Sorenson, Thomas Allen

    Surface analytical techniques have been used to characterize electrochemical reactions to be used in semiconductor processing technologies. Studies have been performed using UHV-EC methodology to determine conditions for the surface limited dissolution of CdTe(100). Electrochemical conditions were identified which resulted in the reduction of the top layer of tellurium atoms, leaving behind a cadmium enriched surface. Attempts to find an electrochemical potential for the oxidative dissolution of the cadmium surface were complicated by the simultaneous oxidation of the compound CdTe. In situ scanning tunneling microscopy has also been used to characterize the formation of tellurium atomic layers formed on Au(111) and Au(100) by underpotential deposition. On Au(100), the following sequence of surface structures was observed prior to bulk electrodeposition: a p(2x2), a (2x✓10), a (2x4), and a (✓2x✓5). The transitions between these structures was observed by STM and mechanisms for the phase transitions are presented. The results are correlated to UHV-EC studies of tellurium UPD on Au(100). On Au(111), the following sequence of structures was observeḑ: a (✓3 x✓3), a (✓7x✓13), and a (3x3). The (✓3x✓3) was shown to exist with a network of domain walls, forming long range triangular and diamond shaped superstructures. Conversion of the (✓3x✓3) to higher coverage structure resulted in roughening of the underlying Au surface and a mechanism is hypothesized to explain this transition. The STM results are also correlated to low energy electron diffraction (LEED) results obtained by UHV-EC studies. The surface structures formed by reductive UPD of the chalcogenide elements and Se on both Au(100) and Au(111) are compared. Both elements initially resulted in structures consisting of isolated atoms separated by distances close to the reported van der Waals diameter. Higher coverage structures resulted in interatomic chalcogenide bonding and the structures

  3. Preparation of TiO₂ supported Au–Pd and Cu–Pd by the combined ...

    Indian Academy of Sciences (India)

    TiO₂ supported Au–Pd and Cu–Pd catalysts were prepared by strong electrostatic adsorption (SEA) of Pd followed by electroless deposition (ED) of a second metal with incremental surface coverages of Au or Cu. High dispersion of small Pd particles on the Pd/TiO2 prepared by SEA led to the high amount of second metal ...

  4. Preparation of supported Au–Pd and Cu–Pd by the combined strong ...

    Indian Academy of Sciences (India)

    BOONTIDA PONGTHAWORNSAKUN

    2017-10-25

    Oct 25, 2017 ... Abstract. TiO2 supported Au–Pd and Cu–Pd catalysts were prepared by strong electrostatic adsorption (SEA) of Pd followed by electroless deposition (ED) of a second metal with incremental surface coverages of Au or. Cu. High dispersion of small Pd particles on the Pd/TiO2 prepared by SEA led to the ...

  5. Measurement of the surface susceptibility and the surface conductivity of atomically thin by spectroscopic ellipsometry

    KAUST Repository

    Jayaswal, Gaurav

    2017-10-01

    We show how to correctly extract from the ellipsometric data the surface susceptibility and the surface conductivity that describe the optical properties of monolayer $\\ m MoS_2$. Theoretically, these parameters stem from modelling a single-layer two-dimensional crystal as a surface current, a truly two-dimensional model. Currently experimental practice is to consider this model equivalent to a homogeneous slab with an effective thickness given by the interlayer spacing of the exfoliating bulk material. We prove that the error in the evaluation of the surface susceptibility of monolayer $\\ m MoS_2$, owing to the use of the slab model, is at least 10% or greater, a significant discrepancy in the determination of the optical properties of this material.

  6. DFT study of hydrogen production from formic acid decomposition on Pd-Au alloy nanoclusters

    Science.gov (United States)

    Liu, D.; Gao, Z. Y.; Wang, X. C.; Zeng, J.; Li, Y. M.

    2017-12-01

    Recently, it has been reported that the hydrogen production rate of formic acid decomposition can be significantly increased using Pd-Au binary alloy nano-catalysts [Wang et al. J. Mater. Chem. A 1 (2013) 12721-12725]. To explain the reaction mechanism of this alloy catalysis method, formic acid decomposition reactions on pure Pd and Pd-Au alloy nanoclusters are studied via density functional theory simulations. The simulation results indicate that the addition of inert element Au would not influence formic acid decomposition on Pd surface sites of Pd-Au alloy nanoclusters. On the other hand, the existence of Au surface sites brings relative weak hydrogen atom adsorption. On Pd-Au alloy nanoclusters, the dissociated hydrogen atoms from formic acid are easier to combine as hydrogen molecules than that on pure Pd clusters. Via the synergetic effect between Pd and Au, both formic acid decomposition and hydrogen production are events with large probability, which eventually results in high hydrogen production rate.

  7. Angular distribution of sputtered atoms from Al-Sn alloy and surface topography

    International Nuclear Information System (INIS)

    Wang Zhenxia; Pan Jisheng; Zhang Jiping; Tao Zhenlan

    1992-01-01

    If an alloy is sputtered the angular distribution of the sputtered atoms can be different for each component. At high ion energies in the range of linear cascade theory, different energy distributions for components of different mass in the solid are predicted. Upon leaving the surface, i.e. overcoming the surface binding energy, these differences should show up in different angular distributions. Differences in the angular distribution are of much practical interest, for example, in thin-film deposition by sputtering and surface analysis by secondary-ion mass spectroscopy and Auger electron spectroscopy. Recently our experimental work has shown that for Fe-W alloy the surface microtopography becomes dominant and determines the shape of the angular distribution of the component. However, with the few experimental results available so far it is too early to draw any general conclusions for the angular distribution of the sputtered constituents. Thus, the aim of this work was to study further the influence of the surface topography on the shape of the angular distribution of sputtered atoms from an Al-Sn alloy. (Author)

  8. Atomic force microscopy of surface topography of nitrogen plasma treated steel

    CERN Document Server

    Mahboubi, F

    2002-01-01

    Nitriding of steels, using plasma environments has been practiced for many years. A lot of efforts have been put on developing new methods, such as plasma immersion ion implantation (Pl sup 3) and radio frequency (RF) plasma nitriding, for mass transfer of nitrogen into the surface of the work piece. This article presents the results obtained from an in depth investigation of the surface morphology of the treated samples, carried out using an atomic force microscope. Samples from a microalloyed steel, were treated by both methods for 5 hours at different temperatures ranging from 350 to 550 sup d eg sup C in 75% N sub 2 -25% H sub 2 atmosphere. It has been found that the surface of the samples treated by PI sup 3 technique, although having more favorable properties, were rougher than the surfaces treated by RF plasma nitriding.

  9. Method for atmospheric pressure reactive atom plasma processing for surface modification

    Science.gov (United States)

    Carr, Jeffrey W [Livermore, CA

    2009-09-22

    Reactive atom plasma processing can be used to shape, polish, planarize and clean the surfaces of difficult materials with minimal subsurface damage. The apparatus and methods use a plasma torch, such as a conventional ICP torch. The workpiece and plasma torch are moved with respect to each other, whether by translating and/or rotating the workpiece, the plasma, or both. The plasma discharge from the torch can be used to shape, planarize, polish, and/or clean the surface of the workpiece, as well as to thin the workpiece. The processing may cause minimal or no damage to the workpiece underneath the surface, and may involve removing material from the surface of the workpiece.

  10. Charge transfer driven surface segregation of gold atoms in 13-atom Au-Ag nanoalloys and its relevance to their structural, optical and electronic properties

    International Nuclear Information System (INIS)

    Chen Fuyi; Johnston, Roy L.

    2008-01-01

    The structural, optical and electronic properties of 13-atom Ag-Au nanoalloys are determined by a combination of global optimization using semi-empirical potentials and density functional theory calculations. A family of Au surface-segregated structures are found for core-shell Ag n Au 13-n (n = 1, 2, 3, 5, 7, 8, 9, 12) and hollow Ag n Au 13-n (n = 4, 6, 10, 11) clusters, whose stability is enhanced by directional charge transfer. The atomic ordering in core-shell structures is related to the electric dipole moment and odd-numbered surface Au-atom clusters have high moments. Their ferroelectric and ferromagnetic properties provide a potential approach for tailoring their surface plasmonic modes

  11. Thermal cyclic test for Sn-4Ag-0.5Cu solders on high P Ni/Au and Ni/Pd/Au surface finishes

    Directory of Open Access Journals (Sweden)

    M.A. Azmah Hanim

    2015-12-01

    Full Text Available In electronic packaging, the reliability of the interconnection changes with the surface finish and the type of solders being used. Thermal cycling is one method of reliability assessment. In thermal cycling experiments, the strain state is simplified by soldering together regular shaped pieces of materials with different coefficients of thermal expansion and exposing the joint to repeated fluctuations of temperature within a certain range. Thus, this study focuses on the intermetallic evolution of Sn-4Ag-0.5Cu on Ni/Au and Ni/Pd/Au surface finishes with thermal cycling up to 1000 cycles with the range of temperature varying from 10 to 80 °C. Sandwich samples were prepared by placing solder balls of Sn-4Ag-0.5Cu between two substrates of two different surface finishes: Ni/Au and Ni/Pd/Au. Optical microscope and FESEM (Field emission scanning electron microscope were used to analyze the samples. From the study, it was observed that the intermetallic changes from (Cu, Ni6Sn5 to (Ni, Cu3Sn4 after 1000 thermal cycles for Ni/Au. These changes promote the formation of cracks at the solder joint because of the different mechanical properties between Ni-Sn based intermetallic and Cu-Sn intermetallics. However, for the Ni/Pd/Au surface finishes, no cracks formed after thermal cycling up to 1000 cycles. This shows that the reliability of the solder joint is higher for Ni/Pd/Au surface finishes in this experiment. Based on these results, it can be concluded that the reliability of the Ni/Pd/Au surface finishes with Sn-4Ag-0.5Cu solders is higher within the given condition of this research.

  12. Alternative splice variants of the human PD-1 gene

    DEFF Research Database (Denmark)

    Nielsen, Christian; Ohm-Laursen, Line; Barington, Torben

    2005-01-01

    PD-1 is an immunoregulatory receptor expressed on the surface of activated T cells, B cells, and monocytes. We describe four alternatively spliced PD-1 mRNA transcripts (PD-1Deltaex2, PD-1Deltaex3, PD-1Deltaex2,3, and PD-1Deltaex2,3,4) in addition to the full length isoform. PD-1Deltaex2 and PD-1...

  13. High rates of catalytic hydrogen combustion with air over Ti ₀. ₉₇Pd ...

    Indian Academy of Sciences (India)

    The surface morphology of coated catalystwas unchanged by long time exposure to hydrogencombustion reaction; i.e., H ₂ +O ₂ recombination reaction which indicated the stability of coating on monolith. Ti ₀. ₉₇Pd ₀. ₀3O ₂− δ showed high rates of H ₂ + O ₂ recombination compared to 2 atom% Pd(metal)/γ -Al ₂O ...

  14. Adsorption behavior of Fe atoms on a naphthalocyanine monolayer on Ag(111) surface

    Energy Technology Data Exchange (ETDEWEB)

    Yan, Linghao; Wu, Rongting; Bao, Deliang; Ren, Junhai; Zhang, Yanfang; Zhang, Haigang; Huang, Li; Wang, Yeliang; Du, Shixuan; Huan, Qing; Gao, Hong-Jun

    2015-05-29

    Adsorption behavior of Fe atoms on a metal-free naphthalocyanine (H2Nc) monolayer on Ag(111) surface at room temperature has been investigated using scanning tunneling microscopy combined with density functional theory (DFT) based calculations. We found that the Fe atoms adsorbed at the centers of H2Nc molecules and formed Fe-H2Nc complexes at low coverage. DFT calculations show that the configuration of Fe at the center of a molecule is the most stable site, in good agreement with the experimental observations. After an Fe-H2Nc complex monolayer was formed, the extra Fe atoms self-assembled to Fe clusters of uniform size and adsorbed dispersively at the interstitial positions of Fe-H2Nc complex monolayer. Furthermore, the H2Nc monolayer grown on Ag(111) could be a good template to grow dispersed magnetic metal atoms and clusters at room temperature for further investigation of their magnetism-related properties.

  15. Comparison of kinetic models for atom recombination on high-temperature reusable surface insulation

    Science.gov (United States)

    Willey, Ronald J.

    1993-01-01

    Five kinetic models are compared for their ability to predict recombination coefficients for oxygen and nitrogen atoms over high-temperature reusable surface insulation (HRSI). Four of the models are derived using Rideal-Eley or Langmuir-Hinshelwood catalytic mechanisms to describe the reaction sequence. The fifth model is an empirical expression that offers certain features unattainable through mechanistic description. The results showed that a four-parameter model, with temperature as the only variable, works best with data currently available. The model describes recombination coefficients for oxygen and nitrogen atoms for temperatures from 300 to 1800 K. Kinetic models, with atom concentrations, demonstrate the influence of atom concentration on recombination coefficients. These models can be used for the prediction of heating rates due to catalytic recombination during re-entry or aerobraking maneuvers. The work further demonstrates a requirement for more recombination experiments in the temperature ranges of 300-1000 K, and 1500-1850 K, with deliberate concentration variation to verify model requirements.

  16. Self-diffusion dynamic behavior of atomic clusters on Re(0 0 0 1) surface

    Energy Technology Data Exchange (ETDEWEB)

    Liu Fusheng [Department of Applied Physics, Hunan University, Changsha 410082 (China); Hu Wangyu, E-mail: wangyuhu2001cn@yahoo.com.cn [Department of Applied Physics, Hunan University, Changsha 410082 (China); Deng Huiqiu; Luo Wenhua; Xiao Shifang [Department of Applied Physics, Hunan University, Changsha 410082 (China); Yang Jianyu [Department of Maths and Physics, Hunan Institute of Engineering, Xiangtan 411104 (China)

    2009-08-15

    Using molecular dynamics simulations and a modified analytic embedded atom potential, the self-diffusion dynamics of rhenium atomic clusters up to seven atoms on Re(0 0 0 1) surface have been studied in the temperature ranges from 600 K to 1900 K. The simulation time varies from 20 ns to 200 ns according to the cluster sizes and the temperature. The heptamer and trimer are more stable comparing to other neighboring non-compact clusters. The diffusion coefficients of clusters are derived from the mean square displacement of cluster's mass-center, and diffusion prefactors D{sub 0} and activation energies E{sub a} are derived from the Arrhenius relation. It is found that the Arrhenius relation of the adatom can be divided into two parts at different temperature range. The activation energy of clusters increases with the increasing of the atom number in clusters. The prefactor of the heptamer is 2-3 orders of magnitude higher than a usual prefactor because of a large number of nonequivalent diffusion processes. The trimer and heptamer are the nuclei at different temperature range according to the nucleation theory.

  17. Optimization of Pd-B/γ-Al2O3 catalyst preparation for palm oil hydrogenation by response surface methodology (RSM)

    OpenAIRE

    Alshaibani, A. M.; Yaakob, Z.; Alsobaai, A. M.; Sahri, M.

    2014-01-01

    Response surface methodology was used to design and evaluate the experimental variables for Pd-B/γ-Al2O3 catalyst preparation. The catalyst was prepared by impregnation and chemical reduction. Thirteen different samples of the catalyst were prepared at different KOH concentrations and annealed at various temperatures, before applying them in palm oil hydrogenation. Hydrogenation was performed on a 0.12% Pd-B/γ-Al2O3 catalyst at a temperature of 393 K, hydrogen pressure of 500 kPa and agitatio...

  18. Optimization of Pd-B/γ-Al2O3 catalyst preparation for palm oil hydrogenation by response surface methodology (RSM)

    OpenAIRE

    Alshaibani,A. M.; Yaakob,Z.; Alsobaai,A. M.; Sahri,M.

    2014-01-01

    Response surface methodology was used to design and evaluate the experimental variables for Pd-B/γ-Al2O3 catalyst preparation. The catalyst was prepared by impregnation and chemical reduction. Thirteen different samples of the catalyst were prepared at different KOH concentrations and annealed at various temperatures, before applying them in palm oil hydrogenation. Hydrogenation was performed on a 0.12% Pd-B/γ-Al2O3 catalyst at a temperature of 393 K, hydrogen pressure of 500 kPa an...

  19. Metal nanostructures with complex surface morphology: The case of supported lumpy Pd and Pt nanoparticles produced by laser processing of metal films

    Science.gov (United States)

    Ruffino, F.; Maugeri, P.; Cacciato, G.; Zimbone, M.; Grimaldi, M. G.

    2016-09-01

    In this work we report on the formation of lumpy Pd and Pt nanoparticles on fluorine-doped tin oxide/glass (FTO/glass) substrate by a laser-based approach. In general, complex-surface morphology metal nanoparticles can be used in several technological applications exploiting the peculiarities of their physical properties as modulated by nanoscale morphology. For example plasmonic metal nanoparticles presenting a lumpy morphology (i.e. larger particles coated on the surface by smaller particles) can be used in plasmonic solar cell devices providing broadband scattering enhancement over the smooth nanoparticles leading, so, to the increase of the device efficiency. However, the use of plasmonic lumpy nanoparticles remains largely unexplored due to the lack of simply, versatile, low-cost and high-throughput methods for the controllable production of such nanostructures. Starting from these considerations, we report on the observation that nanoscale-thick Pd and Pt films (17.6 and 27.9 nm, 12.1 and 19.5 nm, respectively) deposited on FTO/glass surface irradiated by nanosecond pulsed laser at fluences E in the 0.5-1.5 J/cm2 range, produce Pd and Pt lumpy nanoparticles on the FTO surface. In addition, using scanning electron microscopy analyses, we report on the observation that starting from each metal film of fixed thickness h, the fraction F of lumpy nanoparticles increases with the laser fluence E and saturates at the higher fluences. For each fixed fluence, F was found higher starting from the Pt films (at each starting film thickness h) with respect to the Pd films. For each fixed metal and fluence, F was found to be higher decreasing the starting thickness of the deposited film. To explain the formation of the lumpy Pd and Pt nanoparticles and the behavior of F as a function of E and h both for Pd and Pt, the thermodynamic behavior of the Pd and Pt films and nanoparticles due to the interaction with the nanosecond laser is discussed. In particular, the

  20. Size Effects on Surface Elastic Waves in a Semi-Infinite Medium with Atomic Defect Generation

    Directory of Open Access Journals (Sweden)

    F. Mirzade

    2013-01-01

    Full Text Available The paper investigates small-scale effects on the Rayleigh-type surface wave propagation in an isotopic elastic half-space upon laser irradiation. Based on Eringen’s theory of nonlocal continuum mechanics, the basic equations of wave motion and laser-induced atomic defect dynamics are derived. Dispersion equation that governs the Rayleigh surface waves in the considered medium is derived and analyzed. Explicit expressions for phase velocity and attenuation (amplification coefficients which characterize surface waves are obtained. It is shown that if the generation rate is above the critical value, due to concentration-elastic instability, nanometer sized ordered concentration-strain structures on the surface or volume of solids arise. The spatial scale of these structures is proportional to the characteristic length of defect-atom interaction and increases with the increase of the temperature of the medium. The critical value of the pump parameter is directly proportional to recombination rate and inversely proportional to deformational potentials of defects.

  1. Method for controlling a coolant liquid surface of cooling system instruments in an atomic power plant

    International Nuclear Information System (INIS)

    Monta, Kazuo.

    1974-01-01

    Object: To prevent coolant inventory within a cooling system loop in an atomic power plant from being varied depending on loads thereby relieving restriction of varied speed of coolant flow rate to lowering of a liquid surface due to short in coolant. Structure: Instruments such as a superheater, an evaporator, and the like, which constitute a cooling system loop in an atomic power plant, have a plurality of free liquid surface of coolant. Portions whose liquid surface is controlled and portions whose liquid surface is varied are adjusted in cross-sectional area so that the sum total of variation in coolant inventory in an instrument such as a superheater provided with an annulus portion in the center thereof and an inner cylindrical portion and a down-comer in the side thereof comes equal to that of variation in coolant inventory in an instrument such as an evaporator similar to the superheater. which is provided with an overflow pipe in its inner cylindrical portion or down-comer, thereby minimizing variation in coolant inventory of the entire coolant due to loads thus minimizing variation in varied speed of the coolant. (Kamimura, M.)

  2. Mechanistic insights on ethanol dehydrogenation on Pd-Au model catalysts: a combined experimental and DFT study.

    Science.gov (United States)

    Evans, E J; Li, H; Yu, Wen-Yueh; Mullen, G M; Henkelman, G; Mullins, C Buddie

    2017-11-22

    In this study, we have combined ultra-high vacuum (UHV) experiments and density functional theory (DFT) calculations to investigate ethanol (EtOH) dehydrogenation on Pd-Au model catalysts. Using EtOH reactive molecular beam scattering (RMBS), EtOH temperature-programmed desorption (TPD), and DFT calculations, we show how different Pd ensemble sizes on Au(111) can affect the mechanism for EtOH dehydrogenation and H 2 production. The Au(111) surface with an initial coverage of 2 monolayers of Pd (2 ML Pd-Au) had the highest H 2 yield. However, the 1 ML Pd-Au catalyst showed the highest selectivity and stability, yielding appreciable amounts of only H 2 and acetaldehyde. Arrhenius plots of H 2 production confirm that the mechanisms for EtOH dehydrogenation differed between 1 and 2 ML Pd-Au, supporting the perceived difference in selectivity between the two surfaces. DFT calculations support this difference in mechanism, showing a dependence of the initial dehydrogenation selectivity of EtOH on the size of Pd ensemble. DFT binding energies and EtOH TPD confirm that EtOH has increasing surface affinity with increasing Pd ensemble size and Pd coverage, indicating that surfaces with more Pd are more likely to induce an EtOH reaction instead of desorb. Our theoretical results show that the synergistic influence of atomic ensemble and electronic effects on Pd/Au(111) can lead to different H 2 association energies and EtOH dehydrogenation capacities at different Pd ensembles. These results provide mechanistic insights into ethanol's dehydrogenation interactions with different sites on the Pd-Au surface and can potentially aid in bimetallic catalyst design for applications such as fuel cells.

  3. Atomic structure of the adsorption of transition metals on silicon surfaces

    International Nuclear Information System (INIS)

    Cocoletzi, G.H.; Takeuchi, N.

    2007-01-01

    Full text: Solid state devices are useful for their high sensitivity in a small volume. Applications of such devices as dose materials include semi-conducting dose-rate, and dose-reading measuring devices. Transition metals (TM) have electronic and atomic properties similar to those of rare earth elements when they are adsorbed on silicon surfaces. The interfaces of transition metals silicides with Si (111) have very small lattice mismatches, sharp interfaces, and low Schottky barrier, making them ideal in electronic devices, such as infrared detectors and rectifying contacts. In this work we shall describe our first principles total energy calculations to investigate structural properties of bulk ScSi and YSi, the two dimensional arrangement of ScSi 2 and YSi 2 on the Si(111) surface, and the growth of a few layers of ScSi 1.7 and YSi 1.7 on the Si(111) surface. Our calculated bulk structural parameters are in excellent agreement with experimental values. It will be shown that one monolayer of a TM on Si( l l 1) yields a two dimensional phase with (lxl) periodicity consisting of a layer of TM atoms on T4 sites and a Si bilayer on top. This double layer of Si atoms is very close to ideal Si(111)-(1x1) surface, but rotated 180 with respect to the rest of the crystal. More layers of TM silicide epitaxially grown on Si(l 11) result in a hexagonal structure similar to bulk ScSi2 and YSi2: graphite-like Si planes (with vacancies) intercalated with TM planes, and forming a (√3x√3) arrangement with a ScSi 1.7 and YSi 1.7 stoichiometry. The top Si layer does not contain vacancies and it does not present a graphite-like structure, but forms a bilayer arrangement as in bulk Si. (Author)

  4. Atomic structure of the adsorption of transition metals on silicon surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Cocoletzi, G.H. [IF-BUAP, 72000 Puebla (Mexico); Takeuchi, N. [CCMC-UNAM, Ensenada, BCN (Mexico)

    2007-07-01

    Full text: Solid state devices are useful for their high sensitivity in a small volume. Applications of such devices as dose materials include semi-conducting dose-rate, and dose-reading measuring devices. Transition metals (TM) have electronic and atomic properties similar to those of rare earth elements when they are adsorbed on silicon surfaces. The interfaces of transition metals silicides with Si (111) have very small lattice mismatches, sharp interfaces, and low Schottky barrier, making them ideal in electronic devices, such as infrared detectors and rectifying contacts. In this work we shall describe our first principles total energy calculations to investigate structural properties of bulk ScSi and YSi, the two dimensional arrangement of ScSi{sub 2} and YSi{sub 2} on the Si(111) surface, and the growth of a few layers of ScSi{sub 1.7} and YSi{sub 1.7} on the Si(111) surface. Our calculated bulk structural parameters are in excellent agreement with experimental values. It will be shown that one monolayer of a TM on Si( l l 1) yields a two dimensional phase with (lxl) periodicity consisting of a layer of TM atoms on T4 sites and a Si bilayer on top. This double layer of Si atoms is very close to ideal Si(111)-(1x1) surface, but rotated 180 with respect to the rest of the crystal. More layers of TM silicide epitaxially grown on Si(l 11) result in a hexagonal structure similar to bulk ScSi2 and YSi2: graphite-like Si planes (with vacancies) intercalated with TM planes, and forming a ({radical}3x{radical}3) arrangement with a ScSi{sub 1.7} and YSi{sub 1.7} stoichiometry. The top Si layer does not contain vacancies and it does not present a graphite-like structure, but forms a bilayer arrangement as in bulk Si. (Author)

  5. Self-cleaning and surface chemical reactions during hafnium dioxide atomic layer deposition on indium arsenide.

    Science.gov (United States)

    Timm, Rainer; Head, Ashley R; Yngman, Sofie; Knutsson, Johan V; Hjort, Martin; McKibbin, Sarah R; Troian, Andrea; Persson, Olof; Urpelainen, Samuli; Knudsen, Jan; Schnadt, Joachim; Mikkelsen, Anders

    2018-04-12

    Atomic layer deposition (ALD) enables the ultrathin high-quality oxide layers that are central to all modern metal-oxide-semiconductor circuits. Crucial to achieving superior device performance are the chemical reactions during the first deposition cycle, which could ultimately result in atomic-scale perfection of the semiconductor-oxide interface. Here, we directly observe the chemical reactions at the surface during the first cycle of hafnium dioxide deposition on indium arsenide under realistic synthesis conditions using photoelectron spectroscopy. We find that the widely used ligand exchange model of the ALD process for the removal of native oxide on the semiconductor and the simultaneous formation of the first hafnium dioxide layer must be significantly revised. Our study provides substantial evidence that the efficiency of the self-cleaning process and the quality of the resulting semiconductor-oxide interface can be controlled by the molecular adsorption process of the ALD precursors, rather than the subsequent oxide formation.

  6. Atomic Structure of a Spinel-like Transition Al2O3 (100) Surface

    DEFF Research Database (Denmark)

    Jensen, Thomas Nørregaard; Meinander, Kristoffer; Helveg, Stig

    2014-01-01

    We study a crystalline epitaxial alumina thin film with the characteristics of a spinel-type transition Al2O3(100) surface by using atom-resolved noncontact atomic force microscopy and density functional theory. It is shown that the films are terminated by an Al-O layer rich in Al vacancies...

  7. Structural, atomic Hirschfeld surface, magnetic and magnetocaloric properties of SmNi{sub 5} compound

    Energy Technology Data Exchange (ETDEWEB)

    Nouri, K., E-mail: nouri@icmpe.cnrs.fr [C.M.T.R, I.C.M.P.E, CNRS, Université Paris Est Créteil, UMR 7182, 2-8 rue Henri Dunant, F-94320 Thiais (France); Laboratoire des Sciences des Matériaux et de l' Environnement, Faculté des Sciences de Sfax- Université de Sfax, BP 1171, Sfax, 3018 (Tunisia); Jemmali, M. [Laboratoire des Sciences des Matériaux et de l' Environnement, Faculté des Sciences de Sfax- Université de Sfax, BP 1171, Sfax, 3018 (Tunisia); Chemistry Departement, College of Science and Arts at Ar-Rass, Qassim University, P.O. Box53 (Saudi Arabia); Walha, S. [Laboratoire des Sciences des Matériaux et de l' Environnement, Faculté des Sciences de Sfax- Université de Sfax, BP 1171, Sfax, 3018 (Tunisia); Zehani, K. [C.M.T.R, I.C.M.P.E, CNRS, Université Paris Est Créteil, UMR 7182, 2-8 rue Henri Dunant, F-94320 Thiais (France); Ben Salah, A. [Laboratoire des Sciences des Matériaux et de l' Environnement, Faculté des Sciences de Sfax- Université de Sfax, BP 1171, Sfax, 3018 (Tunisia); Bessais, L. [C.M.T.R, I.C.M.P.E, CNRS, Université Paris Est Créteil, UMR 7182, 2-8 rue Henri Dunant, F-94320 Thiais (France)

    2016-07-05

    The SmNi{sub 5} intermetallic compound has been investigated by arc-melting. Powder X-ray diffraction analysis and Rietveld refinement revealed that the sample crystallized in the hexagonal CaCu{sub 5}-type structure P6/mmm space group with the following lattice parameters: a = 4.9203 (1) Å, c = 3.9662 (1) Å. These lattice parameters for the compound are in good agreement with previous theoretical result and experimental data. The EDX analysis has been performed to confirm the composition of this compound. The chemical bonding in SmNi{sub 5} was analyzed using atomic Hirshfeld surfaces, and this analysis supports the presence of the structural elements and the coordination of Sm (1a), Ni (2c) and Ni (3 g). This study indicates the different types of interatomic interactions between the Sm and Ni atoms and the weak interactions between Sm–Sm atoms were also observed along the c axis. The magnetic properties and magnetocaloric effect (MCE) have been established by the magnetization and isothermal magnetization of different temperature measurements. The magnetization curve as a function of temperature shows a magnetic transition from ferromagnetic to paramagnetic state at the Curie temperature T{sub C} = 29 K. We have studied the MCE phenomena in the vicinity of magnetic phase transitions in terms of magnetic entropy change. The temperature dependence of the magnetization, the magnetic entropy changeΔS{sub M}, as well as the relative cooling power around the second-order magnetic transition and the Arrott plots for the alloys are reported. - Highlights: • The SmNi{sub 5} intermetallic compound has been investigated by arc-melting. • The chemical bonding in SmNi{sub 5} was analyzed using atomic Hirshfeld surfaces. • The second order magnetocaloric material SmNi{sub 5} is investigated.

  8. Influence of surface relaxation of strained layers on atomic resolution ADF imaging.

    Science.gov (United States)

    Beyer, Andreas; Duschek, Lennart; Belz, Jürgen; Oelerich, Jan Oliver; Jandieri, Kakhaber; Volz, Kerstin

    2017-10-01

    Surface relaxation of thin transmission electron microscopy (TEM) specimens of strained layers results in a severe bending of lattice planes. This bending significantly displaces atoms from their ideal channeling positions which has a strong impact on the measured annular dark field (ADF) intensity. With the example of GaAs quantum wells (QW) embedded in a GaP barrier, we model the resulting displacements by elastic theory using the finite element (FE) formalism. Relaxed and unrelaxed super cells served as input for state of the art frozen phonon simulation of atomic resolution ADF images. We systematically investigate the dependencies on the sample´s geometric parameters, i.e. QW width and TEM sample thickness, by evaluating the simulated intensities at the atomic column´s positions as well as at the background positions in between. Depending on the geometry the ADF intensity can be affected in a range several nm from the actual interface. Moreover, we investigate the influence of the surface relaxation on the angular distribution of the scattered intensity. At high scattering angles we observe an intensity reduction at the interface as well as in the GaP barrier due to de-channeling. The amount of intensity reduction at an atomic column is directly proportional to its mean square displacement. On the contrary we find a clearly increased intensity at low angles caused by additional diffuse scattering. We discuss the implications for quantitative evaluations as well as strategies to compensate for the reduced intensities. Copyright © 2017 Elsevier B.V. All rights reserved.

  9. Neutron Diffraction Studies of the Atomic Vibrations of Bulk and Surface Atoms of Nanocrystalline SiC

    Science.gov (United States)

    Stelmakh, S.; Grzanka, E.; Zhao, Y.; Palosz, W.; Palosz, B.

    2004-01-01

    Thermal atomic motions of nanocrystalline Sic were characterized by two temperature atomic factors B(sub core), and B(sub shell). With the use of wide angle neutron diffraction data it was shown that at the diffraction vector above 15A(exp -1) the Wilson plots gives directly the temperature factor of the grain interior (B(sub core)). At lower Q values the slope of the Wilson plot provides information on the relative amplitudes of vibrations of the core and shell atoms.

  10. Atomic force microscopy studies of bioprocess engineering surfaces - imaging, interactions and mechanical properties mediating bacterial adhesion.

    Science.gov (United States)

    James, Sean A; Hilal, Nidal; Wright, Chris J

    2017-07-01

    The detrimental effect of bacterial biofilms on process engineering surfaces is well documented. Thus, interest in the early stages of bacterial biofilm formation; in particular bacterial adhesion and the production of anti-fouling coatings has grown exponentially as a field. During this time, Atomic force microscopy (AFM) has emerged as a critical tool for the evaluation of bacterial adhesion. Due to its versatility AFM offers not only insight into the topographical landscape and mechanical properties of the engineering surfaces, but elucidates, through direct quantification the topographical and biomechnical properties of the foulants The aim of this review is to collate the current research on bacterial adhesion, both theoretical and practical, and outline how AFM as a technique is uniquely equipped to provide further insight into the nanoscale world at the bioprocess engineering surface. Copyright © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  11. Hydrophilization of poly(ether ether ketone) films by surface-initiated atom transfer radical polymerization

    DEFF Research Database (Denmark)

    Fristrup, Charlotte Juel; Jankova Atanasova, Katja; Hvilsted, Søren

    2010-01-01

    Surface-Initiated Atom Transfer Radical Polymerization (SI-ATRP) has been exploited to hydrophilize PEEK. The ketone groups on the PEEK surface were reduced to hydroxyl groups which were converted to bromoisobutyrate initiating sites for SI-ATRP. The modification steps were followed by contact...... angle measurements and XPS. Moreover, ATR FTIR has been used to confirm the formation of initiating groups. Grafting of PEGMA from PEEK was performed in aqueous solution. The presence of the PPEGMA grafts on PEEK was revealed by the thermograms from TGA whereas investigations with AFM rejected changes...... in the surface topography. Two possible applications arose from the hydrophilization of PEEK, metal deposition and protein repellency. The performed modification allowed for successful electroless deposition and good adhesion of nickel as well as copper....

  12. The atomic surface structure of SrTiO3 (001) studied with synchrotron X-rays

    NARCIS (Netherlands)

    Vonk, V.; Konings, S.; van Hummel, G.J.; Harkema, Sybolt; Graafsma, H

    2005-01-01

    The atomic surface structure of single terminated SrTiO3(0 0 1) (1 × 1) is investigated employing surface X-ray diffraction. In order to obtain these surfaces a special treatment is needed consisting of chemical etching and annealing. Since this is done in an aqueous and subsequently oxygen

  13. Prediction of protein retention times in hydrophobic interaction chromatography by robust statistical characterization of their atomic-level surface properties.

    NARCIS (Netherlands)

    Hanke, A.T.; Klijn, M.E.; Verhaert, P.D.; Wielen, van der L.; Ottens, M.; Eppink, M.H.M.; Sandt, van de E.J.A.X.

    2016-01-01

    The correlation between the dimensionless retention times (DRT) of proteins in hydrophobic interaction chromatography (HIC) and their surface properties were investigated. A ternary atomic-level hydrophobicity scale was used to calculate the distribution of local average hydrophobicity across the

  14. Thermal Stability of Metal Nanocrystals: An Investigation of the Surface and Bulk Reconstructions of Pd Concave Icosahedra.

    Science.gov (United States)

    Gilroy, Kyle D; Elnabawy, Ahmed O; Yang, Tung-Han; Roling, Luke T; Howe, Jane; Mavrikakis, Manos; Xia, Younan

    2017-06-14

    Despite the remarkable success in controlling the synthesis of metal nanocrystals, it still remains a grand challenge to stabilize and preserve the shapes or internal structures of metastable kinetic products. In this work, we address this issue by systematically investigating the surface and bulk reconstructions experienced by a Pd concave icosahedron when subjected to heating up to 600 °C in vacuum. We used in situ high-resolution transmission electron microscopy to identify the equilibration pathways of this far-from-equilibrium structure. We were able to capture key structural transformations occurring during the thermal annealing process, which were mechanistically rationalized by implementing self-consistent plane-wave density functional theory (DFT) calculations. Specifically, the concave icosahedron was found to evolve into a regular icosahedron via surface reconstruction in the range of 200-400 °C, and then transform into a pseudospherical crystalline structure through bulk reconstruction when further heated to 600 °C. The mechanistic understanding may lead to the development of strategies for enhancing the thermal stability of metal nanocrystals.

  15. Growth, intermixing, and surface phase formation for zinc tin oxide nanolaminates produced by atomic layer deposition

    Energy Technology Data Exchange (ETDEWEB)

    Hägglund, Carl, E-mail: carl.hagglund@angstrom.uu.se [Department of Chemical Engineering, Stanford University, Stanford, California 94305 and Department of Engineering Sciences, Division of Solid State Electronics, Uppsala University, 75121 Uppsala (Sweden); Grehl, Thomas; Brongersma, Hidde H. [ION-TOF GmbH, Heisenbergstraße 15, 48149 Münster (Germany); Tanskanen, Jukka T.; Mullings, Marja N.; Mackus, Adriaan J. M.; MacIsaac, Callisto; Bent, Stacey Francine, E-mail: sbent@stanford.edu [Department of Chemical Engineering, Stanford University, Stanford, California 94305 (United States); Yee, Ye Sheng [Department of Electrical Engineering, Stanford University, Stanford, California 94305 (United States); Clemens, Bruce M. [Department of Material Science and Engineering, Stanford University, Stanford, California 94305 (United States)

    2016-03-15

    A broad and expanding range of materials can be produced by atomic layer deposition at relatively low temperatures, including both oxides and metals. For many applications of interest, however, it is desirable to grow more tailored and complex materials such as semiconductors with a certain doping, mixed oxides, and metallic alloys. How well such mixed materials can be accomplished with atomic layer deposition requires knowledge of the conditions under which the resulting films will be mixed, solid solutions, or laminated. The growth and lamination of zinc oxide and tin oxide is studied here by means of the extremely surface sensitive technique of low energy ion scattering, combined with bulk composition and thickness determination, and x-ray diffraction. At the low temperatures used for deposition (150 °C), there is little evidence for atomic scale mixing even with the smallest possible bilayer period, and instead a morphology with small ZnO inclusions in a SnO{sub x} matrix is deduced. Postannealing of such laminates above 400 °C however produces a stable surface phase with a 30% increased density. From the surface stoichiometry, this is likely the inverted spinel of zinc stannate, Zn{sub 2}SnO{sub 4}. Annealing to 800 °C results in films containing crystalline Zn{sub 2}SnO{sub 4}, or multilayered films of crystalline ZnO, Zn{sub 2}SnO{sub 4}, and SnO{sub 2} phases, depending on the bilayer period.

  16. Low-Temperature Pd/Zeolite Passive NO x Adsorbers: Structure, Performance, and Adsorption Chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Zheng, Yang [Institute for Integrated; Kovarik, Libor [Institute for Integrated; Engelhard, Mark H. [Institute for Integrated; Wang, Yilin [Institute for Integrated; Wang, Yong [Institute for Integrated; Gao, Feng [Institute for Integrated; Szanyi, János [Institute for Integrated

    2017-07-14

    Pd/zeolite passive NOx adsorber (PNA) materials were prepared with solution ion-exchange between NH4/zeolites (Beta, ZSM-5 and SSZ-13) and PdCl2 solutions. The nature of Pd (dispersion, distribution and oxidation states) in these materials was characterized with Na+ ion-exchange, TEM imaging, CO titration with FTIR and in situ XPS. The NOx trapping and release properties were tested using feeds with different compositions. It is concluded that multiple Pd species coexist in these materials: atomically dispersed Pd in the cationic sites of zeolites, and PdO2 and PdO particles on the external surfaces. While Pd is largely atomically dispersed in ZSM-5, the small pore opening for SSZ-13 inhibits Pd diffusion such that the majority of Pd stays as external surface PdO2 clusters. NOx trapping and release are not simple chemisorption and desorption events, but involve rather complex chemical reactions. In the absence of CO in the feed, cationic Pd(II) sites with oxygen ligands and PdO2 clusters are reduced by NO to Pd(I) and PdO clusters. These reduced sites are the primary NO adsorption sites. In the presence of H2O, the as-formed NO2 desorb immediately. In the presence of CO in the feed, metallic Pd, “naked” Pd2+, and Pd+ sites are responsible for NO adsorption. For Pd adsorption sites with the same oxidation states but in different zeolite frameworks, NO binding energies are not expected to vary greatly. However, NO release temperatures do vary substantially with different zeolite structures. This indicates that NO transport within these materials play an important role in determining release temperatures. Finally, some rational design principles on efficient PNA materials are suggested. The authors gratefully acknowledge the US Department of Energy (DOE), Energy Efficiency and Renewable Energy, Vehicle Technologies Office for the support of this work. The research described in this paper was performed in the Environmental Molecular Sciences Laboratory (EMSL), a

  17. Osmium Atoms and Os2 Molecules Move Faster on Selenium-Doped Compared to Sulfur-Doped Boronic Graphenic Surfaces.

    Science.gov (United States)

    Barry, Nicolas P E; Pitto-Barry, Anaïs; Tran, Johanna; Spencer, Simon E F; Johansen, Adam M; Sanchez, Ana M; Dove, Andrew P; O'Reilly, Rachel K; Deeth, Robert J; Beanland, Richard; Sadler, Peter J

    2015-07-28

    We deposited Os atoms on S- and Se-doped boronic graphenic surfaces by electron bombardment of micelles containing 16e complexes [Os(p-cymene)(1,2-dicarba-closo-dodecarborane-1,2-diselenate/dithiolate)] encapsulated in a triblock copolymer. The surfaces were characterized by energy-dispersive X-ray (EDX) analysis and electron energy loss spectroscopy of energy filtered TEM (EFTEM). Os atoms moved ca. 26× faster on the B/Se surface compared to the B/S surface (233 ± 34 pm·s(-1) versus 8.9 ± 1.9 pm·s(-1)). Os atoms formed dimers with an average Os-Os distance of 0.284 ± 0.077 nm on the B/Se surface and 0.243 ± 0.059 nm on B/S, close to that in metallic Os. The Os2 molecules moved 0.83× and 0.65× more slowly than single Os atoms on B/S and B/Se surfaces, respectively, and again markedly faster (ca. 20×) on the B/Se surface (151 ± 45 pm·s(-1) versus 7.4 ± 2.8 pm·s(-1)). Os atom motion did not follow Brownian motion and appears to involve anchoring sites, probably S and Se atoms. The ability to control the atomic motion of metal atoms and molecules on surfaces has potential for exploitation in nanodevices of the future.

  18. Synthesis of ZnS nanoparticles on a solid surface: Atomic force microscopy study

    International Nuclear Information System (INIS)

    Yuan Huizhen; Lian Wenping; Song Yonghai; Chen Shouhui; Chen Lili; Wang Li

    2010-01-01

    In this work, zinc sulfide (ZnS) nanoparticles had been synthesized on DNA network/mica and mica surface, respectively. The synthesis was carried out by first dropping a mixture of zinc acetate and DNA on a mica surface for the formation of the DNA networks or zinc acetate solution on a mica surface, and subsequently transferring the sample into a heated thiourea solution. The Zn 2+ adsorbed on DNA network/mica or mica surface would react with S 2- produced from thiourea and form ZnS nanoparticles on these surfaces. X-ray diffraction and atomic force microscopy (AFM) were used to characterize the ZnS nanoparticles in detail. AFM results showed that ZnS nanoparticles distributed uniformly on the mica surface and deposited preferentially on DNA networks. It was also found that the size and density of ZnS nanoparticles could be effectively controlled by adjusting reaction temperature and the concentration of Zn 2+ or DNA. The possible growth mechanisms have been discussed in detail.

  19. Characterizing the surface charge of clay minerals with Atomic Force Microscope (AFM

    Directory of Open Access Journals (Sweden)

    Yuan Guo

    2017-05-01

    Full Text Available The engineering properties of clayey soils, including fluid permeability, erosion resistance and cohesive strength, are quite different from those of non-cohesive soils. This is mainly due to their small platy particle shape and the surrounding diffuse double layer structure. By using the Atomic Force Microscopy (AFM, the surface topography and the interaction force between the silicon dioxide tip and the kaolinite/montmorillonite clay minerals have been measured in the 1.0 mM NaCl solution at neutral pH. From this, the surface potential of the clay minerals is determined by mathematical regression analyses using the DLVO model. The length/thickness ratio of kaolinite and montmorillonite particles measured ranges from 8.0 to 15.0. The surface potential and surface charge density vary with particles. The average surface potential of montmorillonite is −62.8 ± 10.6 mV, and the average surface potential of kaolinite is −40.9 ± 15.5 mV. The measured results help to understand the clay sediment interaction, and will be used to develop interparticle force model to simulate sediment transport during erosion process.

  20. Surface modification of nanodiamond through metal free atom transfer radical polymerization

    Energy Technology Data Exchange (ETDEWEB)

    Zeng, Guangjian; Liu, Meiying; Shi, Kexin; Heng, Chunning; Mao, Liucheng; Wan, Qing; Huang, Hongye [Department of Chemistry, Nanchang University, 999 Xuefu Avenue, Nanchang 330031 (China); Deng, Fengjie, E-mail: fengjiedeng@aliyun.com [Department of Chemistry, Nanchang University, 999 Xuefu Avenue, Nanchang 330031 (China); Zhang, Xiaoyong, E-mail: xiaoyongzhang1980@gmail.com [Department of Chemistry, Nanchang University, 999 Xuefu Avenue, Nanchang 330031 (China); Wei, Yen, E-mail: weiyen@tsinghua.edu.cn [Department of Chemistry and the Tsinghua Center for Frontier Polymer Research, Tsinghua University, Beijing, 100084 (China)

    2016-12-30

    Highlights: • Surface modification of ND with water soluble and biocompatible polymers. • Functionalized ND through metal free surface initiated ATRP. • The metal free surface initiated ATRP is rather simple and effective. • The ND-poly(MPC) showed high dispersibility and desirable biocompatibility. - Abstract: Surface modification of nanodiamond (ND) with poly(2-methacryloyloxyethyl phosphorylcholine) [poly(MPC)] has been achieved by using metal free surface initiated atom transfer radical polymerization (SI-ATRP). The ATRP initiator was first immobilized on the surface of ND through direct esterification reaction between hydroxyl group of ND and 2-bromoisobutyryl bromide. The initiator could be employed to obtain ND-poly(MPC) nanocomposites through SI-ATRP using an organic catalyst. The final functional materials were characterized by {sup 1}H nuclear magnetic resonance, transmission electron microscopy, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy and thermo gravimetric analysis in detailed. All of these characterization results demonstrated that ND-poly(MPC) have been successfully obtained via metal free photo-initiated SI-ATRP. The ND-poly(MPC) nanocomposites shown enhanced dispersibility in various solvents as well as excellent biocompatibility. As compared with traditional ATRP, the metal free ATRP is rather simple and effective. More importantly, this preparation method avoided the negative influence of metal catalysts. Therefore, the method described in this work should be a promising strategy for fabrication of polymeric nanocomposites with great potential for different applications especially in biomedical fields.

  1. Surface topography characterization using an atomic force microscope mounted on a coordinate measuring machine

    DEFF Research Database (Denmark)

    De Chiffre, Leonardo; Hansen, H.N; Kofod, N

    1999-01-01

    The paper describes the construction, testing and use of an integrated system for topographic characterization of fine surfaces on parts having relatively big dimensions. An atomic force microscope (AFM) was mounted on a manual three-coordinate measuring machine (CMM) achieving free positioning...... of the AFM probe in space. This means that the limited measuring range of the AFM (40 mu m x 40 mu m x 2.7 um) can be extended by positioning the AFM probe using the movements of the CMM axes (400 mm x 100 mm x 75 mm). Evaluation of the background noise by determining the Sa value of an optical fiat gave...

  2. Spatial spectrograms of vibrating atomic force microscopy cantilevers coupled to sample surfaces

    International Nuclear Information System (INIS)

    Wagner, Ryan; Raman, Arvind; Proksch, Roger

    2013-01-01

    Many advanced dynamic Atomic Force Microscopy (AFM) techniques such as contact resonance, force modulation, piezoresponse force microscopy, electrochemical strain microscopy, and AFM infrared spectroscopy exploit the dynamic response of a cantilever in contact with a sample to extract local material properties. Achieving quantitative results in these techniques usually requires the assumption of a certain shape of cantilever vibration. We present a technique that allows in-situ measurements of the vibrational shape of AFM cantilevers coupled to surfaces. This technique opens up unique approaches to nanoscale material property mapping, which are not possible with single point measurements alone

  3. Electron collisions with atoms, ions, molecules, and surfaces: Fundamental science empowering advances in technology

    Science.gov (United States)

    Bartschat, Klaus; Kushner, Mark J.

    2016-06-01

    Electron collisions with atoms, ions, molecules, and surfaces are critically important to the understanding and modeling of low-temperature plasmas (LTPs), and so in the development of technologies based on LTPs. Recent progress in obtaining experimental benchmark data and the development of highly sophisticated computational methods is highlighted. With the cesium-based diode-pumped alkali laser and remote plasma etching of Si3N4 as examples, we demonstrate how accurate and comprehensive datasets for electron collisions enable complex modeling of plasma-using technologies that empower our high-technology-based society.

  4. Surface-Initiated Atom Transfer Radical Polymerization from Electrospun Mats: An Alternative to Nafion

    DEFF Research Database (Denmark)

    Javakhishvili, Irakli; Dimitrov, Ivaylo; Tynelius, Oskar

    2017-01-01

    Proton exchange membranes for fuel cell applications are synthesized by surface-initiated(SI) atom transfer radical polymerization (ATRP). Poly(vinylidene fluoride-co-chlorotrifluoroethylene)is electrospun into 50 μm thick mat, which is then employed as multifunctionalinitiator for copper......-mediated SI ATRP of 4-styrene sulfonic acid sodium salt. Fine-tuning ofthe ATRP conditions allows adjustment of the membrane’sion exchange capacity by varying the loading of the graftedionomer. Structure and composition of the membranes areinvestigated by spectroscopic means and thermogravimetricanalysis...

  5. The over-step coalescence of carbon atoms on copper surface in the CVD growth of graphene: density functional calculations

    Directory of Open Access Journals (Sweden)

    Yingfeng Li

    2013-05-01

    Full Text Available The ways in which carbon atoms coalesce over the steps on copper (111 surface are ascertained by density functional theory (DFT calculations in the context of chemical vapor deposition (CVD growth of graphene. Two strategies, (1 by putting carbon atoms on and under the steps separately and (2 by importing additional carbon atoms between the ones separated by the steps, have been attempted to investigate if an over-step coalescence of carbon atoms could take place. Based on analyses about the optimized configurations and adsorption energies of carbon atoms nearby the steps, as well as the energy evolution curve of the system throughout the geometry optimizations process, we determined the main way in which graphene grows over the steps continuously: the carbon atoms, adsorbed additionally on the locations between the already existing ones which are separated by the steps, link them (these carbon atoms separated by the steps together. The direct over-step coalescence of the carbon atoms separated by the steps is very difficult, although the energy barrier preventing their coalescence can be weakened by importing carbon atoms on and under the steps gradually. Our results imply potential applications in directing the fabrication of graphene with particular structure by controlling the surface topography of copper substrate.

  6. Attractive interaction between Mn atoms on the GaAs(110) surface observed by scanning tunneling microscopy.

    Science.gov (United States)

    Taninaka, Atsushi; Yoshida, Shoji; Kanazawa, Ken; Hayaki, Eiko; Takeuchi, Osamu; Shigekawa, Hidemi

    2016-06-16

    Scanning tunneling microscopy/spectroscopy (STM/STS) was carried out to investigate the structures of Mn atoms deposited on a GaAs(110) surface at room temperature to directly observe the characteristics of interactions between Mn atoms in GaAs. Mn atoms were paired with a probability higher than the random distribution, indicating an attractive interaction between them. In fact, re-pairing of unpaired Mn atoms was observed during STS measurement. The pair initially had a new structure, which was transformed during STS measurement into one of those formed by atom manipulation at 4 K. Mn atoms in pairs and trimers were aligned in the direction, which is theoretically predicted to produce a high Curie temperature.

  7. Interaction of Pd with steps on α-Al2O3(0001),

    DEFF Research Database (Denmark)

    Lodziana, Zbigniew; Nørskov, Jens Kehlet

    2002-01-01

    Based on density functional calculations, we show that steps on the alpha-Al2O3 (0 0 0 1) surface are enriched in oxygen and that they bind Pd atoms and small clusters much stronger than the terraces. We also show that Pd can diffuse quite freely on an alumina surface and use this to explain why...... STM studies of Pd island nucleation always find metal nanoclusters to be associated with linear defects. (C) 2002 Elsevier Science B.V. All rights reserved....

  8. Modeling of Transmittance Degradation Caused by Optical Surface Contamination by Atomic Oxygen Reaction with Adsorbed Silicones

    Science.gov (United States)

    Snyder, Aaron; Banks, Bruce; Miller, Sharon; Stueber, Thomas; Sechkar, Edward

    2001-01-01

    A numerical procedure is presented to calculate transmittance degradation caused by contaminant films on spacecraft surfaces produced through the interaction of orbital atomic oxygen (AO) with volatile silicones and hydrocarbons from spacecraft components. In the model, contaminant accretion is dependent on the adsorption of species, depletion reactions due to gas-surface collisions, desorption, and surface reactions between AO and silicone producing SiO(x), (where x is near 2). A detailed description of the procedure used to calculate the constituents of the contaminant layer is presented, including the equations that govern the evolution of fractional coverage by specie type. As an illustrative example of film growth, calculation results using a prototype code that calculates the evolution of surface coverage by specie type is presented and discussed. An example of the transmittance degradation caused by surface interaction of AO with deposited contaminant is presented for the case of exponentially decaying contaminant flux. These examples are performed using hypothetical values for the process parameters.

  9. Semiclassical multi-phonon theory for atom-surface scattering: Application to the Cu(111) system.

    Science.gov (United States)

    Daon, Shauli; Pollak, Eli

    2015-05-07

    The semiclassical perturbation theory of Hubbard and Miller [J. Chem. Phys. 80, 5827 (1984)] is further developed to include the full multi-phonon transitions in atom-surface scattering. A practically applicable expression is developed for the angular scattering distribution by utilising a discretized bath of oscillators, instead of the continuum limit. At sufficiently low surface temperature good agreement is found between the present multi-phonon theory and the previous one-, and two-phonon theory derived in the continuum limit in our previous study [Daon, Pollak, and Miret-Artés, J. Chem. Phys. 137, 201103 (2012)]. The theory is applied to the measured angular distributions of Ne, Ar, and Kr scattered from a Cu(111) surface. We find that the present multi-phonon theory substantially improves the agreement between experiment and theory, especially at the higher surface temperatures. This provides evidence for the importance of multi-phonon transitions in determining the angular distribution as the surface temperature is increased.

  10. Silicon surface passivation using thin HfO2 films by atomic layer deposition

    International Nuclear Information System (INIS)

    Gope, Jhuma; Vandana; Batra, Neha; Panigrahi, Jagannath; Singh, Rajbir; Maurya, K.K.; Srivastava, Ritu; Singh, P.K.

    2015-01-01

    Graphical abstract: - Highlights: • HfO 2 films using thermal ALD are studied for silicon surface passivation. • As-deposited thin film (∼8 nm) shows better passivation with surface recombination velocity (SRV) <100 cm/s. • Annealing improves passivation quality with SRV ∼20 cm/s for ∼8 nm film. - Abstract: Hafnium oxide (HfO 2 ) is a potential material for equivalent oxide thickness (EOT) scaling in microelectronics; however, its surface passivation properties particularly on silicon are not well explored. This paper reports investigation on passivation properties of thermally deposited thin HfO 2 films by atomic layer deposition system (ALD) on silicon surface. As-deposited pristine film (∼8 nm) shows better passivation with <100 cm/s surface recombination velocity (SRV) vis-à-vis thicker films. Further improvement in passivation quality is achieved with annealing at 400 °C for 10 min where the SRV reduces to ∼20 cm/s. Conductance measurements show that the interface defect density (D it ) increases with film thickness whereas its value decreases after annealing. XRR data corroborate with the observations made by FTIR and SRV data.

  11. Atomic-Level Simulation Study of n-Hexane Pyrolysis on Silicon Carbide Surfaces.

    Science.gov (United States)

    Sajib, Md Symon Jahan; Samieegohar, Mohammadreza; Wei, Tao; Shing, Katherine

    2017-10-24

    Ethylene production plays a key role in the petrochemical industry. The severe operation conditions of ethylene thermal cracking, such as high-temperature and coke-formation, pose challenges for the development of new corrosion-resistant and coking-resistant materials for ethylene reactor radiant coils tubes (RCTs). We investigated the performance of ceramic materials such as silicon carbide (SiC) in severe pyrolysis conditions by using reactive force field molecular dynamics (ReaxFF MD) simulation method. Our results indicate that β-SiC surface remains fully stable at 1500 K, whereas increased temperature results in melted interface. At 2500 K, fully grown cross-linked-graphene-like polycyclic aromatic hydrocarbon coking structure on SiC surfaces was observed. Such coking was particularly severe in the carbon-side of the surface slab. The coking structures were mainly derived from surface atoms at the initial 3.0 ns, as a result of the loss of interfacial hydroxyl layer and further hydrothermal corrosion. The SiC substrate surface enhances the ethylene cracking rate and also leads to different intermediate-state compounds. Our fundamental research will have significant and broad impact on both petrochemical industry and academic research in materials science, petrochemistry, and combustion chemistry.

  12. The surface phase diagram of Li/Cu(001) explored by helium atom scattering

    Energy Technology Data Exchange (ETDEWEB)

    Huang Congcong; MacLaren, D A; Bacon, R T; Allison, W, E-mail: congcong@slac.stanford.edu [Cavendish Laboratory, University of Cambridge, J J Thomson Avenue, Cambridge CB3 0HE (United Kingdom)

    2011-09-07

    We use helium atom scattering to investigate the structures formed by Li adsorption onto Cu(001) in the 0-2 ML regime. Submonolayer growth at 180 K proceeds through a sequence of ordered overlayers, including a c(2 x 2) structure at 0.5 ML and a series of 'ladder' superlattices around 0.6 ML. Beyond 1 ML, incommensurate, three-dimensional Li islands develop. A quantum close-coupled scattering analysis is performed to study the empirical He-surface potential of the structurally heterogeneous ladder structures. Good agreement with the measured distribution of diffracted intensity is obtained by describing the He-ladder interaction potential as the summation of only six one-dimensional Fourier components. The fitted potential indicates a remarkably flat surface that is punctuated by substantial, striped protrusions in the electron density. The result is consistent with the formation of one-dimensional Li wires, indicating an inhomogeneous metallization process.

  13. Micro and nanostructural characterization of surfaces and interfaces of Portland cement mortars using atomic force microscopy

    International Nuclear Information System (INIS)

    Barreto, M.F.O.; Brandao, P.R.G.

    2014-01-01

    The characterization of Portland cement mortars is very important in the study the interfaces and surfaces that make up the system grout/ceramic block. In this sense, scanning electron microscopy and energy-dispersive (X-ray) spectrometer are important tools in investigating the morphology and chemical aspects. However, more detailed topographic information can be necessary in the characterization process. In this work, the aim was to characterize topographically surfaces and interfaces of mortars applied onto ceramic blocks. This has been accomplished by using the atomic force microscope (AFM) - MFP-3D-SA Asylum Research. To date, the results obtained from this research show that the characterization of cementitious materials with the help of AFM has an important contribution in the investigation and differentiation of hydrated calcium silicates (CSH), calcium hydroxide (Ca(OH)2, ettringite and calcium carbonate by providing morphological and micro topographical data, which are extremely important and reliable for the understanding of cementitious materials. (author)

  14. Adsorption of Atoms of 3 d Metals on the Surfaces of Aluminum and Magnesium Oxide Films

    Science.gov (United States)

    Ramonova, A. G.; Kibizov, D. D.; Kozyrev, E. N.; Zaalishvili, V. B.; Grigorkina, G. S.; Fukutani, K.; Magkoev, T. T.

    2018-01-01

    The adsorption and formation of submonolayer structures of Ti, Cr, Fe, Ni, Cu on the surfaces of aluminum and magnesium oxide films formed on Mo(110) under ultrahigh vacuum conditions are studied via X-ray, ultraviolet photo-, and Auger electron spectroscopy (XPS, UVES, AES); spectroscopy of energy losses of high-resolution electrons (SELHRE); spectroscopy of the backscattering of low-energy ions (SBSLEI); infrared absorption spectroscopy (IAS); and the diffraction of slow electrons (DSE). Individual atoms and small clusters of all the investigated metals deposited on oxides acquire a positive charge, due presumably to interaction with surface defects. As the concentration of adatoms increases when the adsorption centers caused by defects are filled, charge transfer from adatoms to substrates is reduced. This is accompanied by further depolarization caused by the lateral interaction of adatoms.

  15. Atom-specific look at the surface chemical bond using x-ray emission spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Nilsson, A.; Wassdahl, N.; Weinelt, M. [Uppsala Univ. (Sweden)] [and others

    1997-04-01

    CO and N{sub 2} adsorbed on the late transition metals have become prototype systems regarding the general understanding of molecular adsorption. It is in general assumed that the bonding of molecules to transition metals can be explained in terms of the interaction of the frontier HOMO and LUMO molecular orbitals with the d-orbitals. In such a picture the other molecular orbitals should remain essentially the same as in the free molecule. For the adsorption of the isoelectronic molecules CO and N{sub 2} this has led to the so called Blyholder model i.e., a synergetic {sigma} (HOMO) donor and {pi} (LUMO) backdonation bond. The authors results at the ALS show that such a picture is oversimplified. The direct observation and identification of the states related to the surface chemical bond is an experimental challenge. For noble and transition metal surfaces, the adsorption induced states overlap with the metal d valence band. Their signature is therefore often obscured by bulk substrate states. This complication has made it difficult for techniques such as photoemission and inverse photoemission to provide reliable information on the energy of chemisorption induced states and has left questions unanswered regarding the validity of the frontier orbitals concept. Here the authors show how x-ray emission spectroscopy (XES), in spite of its inherent bulk sensitivity, can be used to investigate adsorbed molecules. Due to the localization of the core-excited intermediate state, XE spectroscopy allows an atomic specific separation of the valence electronic states. Thus the molecular contributions to the surface measurements make it possible to determine the symmetry of the molecular states, i.e., the separation of {pi} and {sigma} type states. In all the authors can obtain an atomic view of the electronic states involved in the formation of the chemical bond to the surface.

  16. Assembling three-dimensional nanostructures on metal surfaces with a reversible vertical single-atom manipulation: A theoretical modeling

    International Nuclear Information System (INIS)

    Yang Tianxing; Ye Xiang; Huang Lei; Xie Yiqun; Ke Sanhuang

    2012-01-01

    Highlights: ► We simulate the reversible vertical single-atom manipulations on several metal surfaces. ► We propose a method to predict whether a reversible vertical single-atom manipulation can be successful on several metal surfaces. ► A 3-dimensional Ni nanocluster is assembled on the Ni(1 1 1) surface using a Ni trimer-apex tip. - Abstract: We propose a theoretical model to show that pulling up an adatom from an atomic step requires a weaker force than from the flat surfaces of Al(0 0 1), Ni(1 1 1), Pt(1 1 0) and Au(1 1 0). Single adatom in the atomic step can be extracted vertically by a trimer-apex tip while can be released to the flat surface. This reversible vertical manipulation can then be used to fabricate a supported three-dimensional (3D) nanostructure on the Ni(1 1 1) surface. The present modeling can be used to predict whether the reversible vertical single-atom manipulation and thus the assembling of 3D nanostructures can be achieved on a metal surface.

  17. An effective low Pd-loading catalyst for hydrogen generation from formic acid

    DEFF Research Database (Denmark)

    Huang, Yunjie; Xu, Junlei; Ma, Xin

    2017-01-01

    ) and a functional support (nitrogen modified reduced graphene oxide, N-rGO) were applied to prepare Pd catalyst. It was found that the Ag atoms facilitated the formation of Pd-rich surface in the preparation strategy, in which the reductive N-rGO and a two-step feeding process of metal precursors played important...... roles. In addition, Ag additive was found to benefit catalyst stability. Most interestingly, the obtained low Pd-loading Pd1Ag6/N-rGO catalyst showed a specific Pd loading turnover frequency of 171 mol Pd−1 h−1 and a specific metal cost turnover frequency of 64.2 $−1 h−1, which were predominant among...

  18. Selective hydrodechlorination of 1,2-dichloroethane catalyzed by trace Pd decorated Ag/Al2O3 catalysts prepared by galvanic replacement

    Science.gov (United States)

    Sun, Jingya; Han, Yuxiang; Fu, Heyun; Wan, Haiqin; Xu, Zhaoyi; Zheng, Shourong

    2018-01-01

    Ag catalysts decorated by trace Pd supported on γ-Al2O3 with different structure and chemical properties were prepared using a combined impregnation and galvanic replacement method. For comparison, monometallic Ag/γ-Al2O3 and Pd/γ-Al2O3 catalysts were prepared using the impregnation method. Gas-phase catalytic hydrodechlorination of 1,2-dichloroethane to ethylene was investigated on those catalysts. The structures and chemical compositions of bimetallic Pd-Ag particles in the catalysts were controlled by adjusting Pd replacement amount. The as-prepared catalysts were characterized by X-ray diffraction, transmission electron microscopy, UV-vis diffuse reflectance spectroscopy, X-ray photoelectron spectroscopy, and in-situ FTIR spectroscopy of CO adsorption. The results demonstrated that contiguous Pd sites dominated in the monometallic Pd/γ-Al2O3 catalyst, while Pd atoms were separately decorated on the surface of Ag particles in the bimetallic Pd-Ag/γ-Al2O3 catalysts when Pd replacement amount was below 0.30 wt.%. At Pd replacement amount of 0.30 wt.%, Pd ensembles with contiguous Pd sites developed in the bimetallic catalyst. Thus, monometallic Pd/γ-Al2O3 catalyst displayed negligible ethylene selectivity toward the catalytic hydrodechlorination of 1,2-dichloroethane, while bimetallic Pd-Ag/γ-Al2O3 catalyst with a Pd replacement amount of 0.13 wt.% exhibited 94.6% of ethylene selectivity. Furthermore, selectivity to incompletely dechlorinated byproduct chloroethylene decreased with Pd replacement amount, due to the enhanced decoration effect of Pd on large Ag ensembles. Findings in this work provide a promising bimetallic catalyst prepared by galvanic replacement for the selective catalytic hydrodechlorination of 1,2-dichloroethane.

  19. Tailoring Silica-alumina Supported Pt-Pd As Poison Tolerant Catalyst For Aromatics Hydrogenation

    Energy Technology Data Exchange (ETDEWEB)

    Yu, Yanzhe; Gutierrez, Oliver Y.; Haller, Gary L.; Colby, Robert J.; Kabius, Bernd C.; Rob van Veen, J. A.; Jentys, Andreas; Lercher, Johannes A.

    2013-08-01

    The tailoring of the physicochemical and catalytic properties of mono- and bimetallic Pt-Pd catalysts supported on amorphous silica-alumina is studied. Electron energy loss spectroscopy and extended X-ray absorption fine structure analyses indicated that bimetallic Pt-Pd and relatively large monometallic Pd particles were formed, whereas the X-ray absorption near edge structure provided direct evidence for the electronic deficiency of the Pt atoms. The heterogeneous distribution of metal particles was also shown by high resolution transmission electron microscopy. The average structure of the bimetallic particles (Pt-rich core and Pd-rich shell) and the presence of Pd particles led to surface Pd enrichment, which was independently shown by IR spectra of adsorbed CO. The specific metal distribution, average size, and surface composition of the Pt-Pd particles depend to a large extent on the metal precursors. In the presence of NH3 ligands, Pt-Pd particles with a fairly homogeneous bulk and surface metal distribution were formed. Also high Lewis acid site concentration of the carrier leads to more homogeneous bimetallic particles. All catalysts were active for the hydrogenation of tetralin in the absence and presence of quinoline and dibenzothiophene (DBT). Monometallic Pt catalysts had the highest hydrogenation activity in poison-free and quinoline-containing feed. When DBT was present, bimetallic Pt-Pd catalysts with the most homogenous metal distribution showed the highest activity. The higher resistance of bimetallic catalysts towards sulfur poisoning compared to their monometallic Pt counterparts results from the weakened metal-sulfur bond on the electron deficient Pt atoms. Thus, increasing the fraction of electron deficient Pt on the surface of the bimetallic particles increases the efficiency of the catalyst in the presence of sulfur.

  20. C-C Coupling on Single-Atom-Based Heterogeneous Catalyst.

    Science.gov (United States)

    Zhang, Xiaoyan; Sun, Zaicheng; Wang, Bin; Tang, Yu; Nguyen, Luan; Li, Yuting; Tao, Franklin Feng

    2018-01-24

    Compared to homogeneous catalysis, heterogeneous catalysis allows for ready separation of products from the catalyst and thus reuse of the catalyst. C-C coupling is typically performed on a molecular catalyst which is mixed with reactants in liquid phase during catalysis. This homogeneous mixing at a molecular level in the same phase makes separation of the molecular catalyst extremely challenging and costly. Here we demonstrated that a TiO 2 -based nanoparticle catalyst anchoring singly dispersed Pd atoms (Pd 1 /TiO 2 ) is selective and highly active for more than 10 Sonogashira C-C coupling reactions (R≡CH + R'X → R≡R'; X = Br, I; R' = aryl or vinyl). The coupling between iodobenzene and phenylacetylene on Pd 1 /TiO 2 exhibits a turnover rate of 51.0 diphenylacetylene molecules per anchored Pd atom per minute at 60 °C, with a low apparent activation barrier of 28.9 kJ/mol and no cost of catalyst separation. DFT calculations suggest that the single Pd atom bonded to surface lattice oxygen atoms of TiO 2 acts as a site to dissociatively chemisorb iodobenzene to generate an intermediate phenyl, which then couples with phenylacetylenyl bound to a surface oxygen atom. This coupling of phenyl adsorbed on Pd 1 and phenylacetylenyl bound to O ad of TiO 2 forms the product molecule, diphenylacetylene.

  1. Effect of the Pd/MWCNTs anode catalysts preparation methods on their morphology and activity in a direct formic acid fuel cell

    Science.gov (United States)

    Lesiak, B.; Mazurkiewicz, M.; Malolepszy, A.; Stobinski, L.; Mierzwa, B.; Mikolajczuk-Zychora, A.; Juchniewicz, K.; Borodzinski, A.; Zemek, J.; Jiricek, P.

    2016-11-01

    Impact of Pd/MWCNTs catalysts preparation method on the catalysts morphology and activity in a formic acid electrooxidation reaction was investigated. Three reduction methods of Pd precursor involving reduction in a high pressure microwave reactor (Pd1), reduction with NaBH4 (Pd2) and microwave-assisted polyol method (Pd3) were used in this paper. Crystallites size and morphology were studied using the scanning transmission electron microscopy (STEM), X-ray diffraction (XRD), whereas elemental composition, Pd chemical state and functional groups content by the X-ray photoelectron spectroscopy (XPS). The prepared catalysts were tested in a direct formic acid fuel cell (DFAFC) as an anode material. The catalytic activity was correlated with a mean fraction of the total Pd atoms exposed at the surface (FE). The value of FE was calculated from the crystallites size distribution determined by the STEM measurements. Non-linear dependence of a current density versus FE, approaching the maximum at FE≈0.25 suggests that the catalytic process proceeded at Pd nanocrystallites faces, with inactive edges and corners. Pd2 catalyst exhibited highest activity due to its smallest Pd crystallites (3.2 nm), however the absence of Pd crystallites aggregation and low content of carbon in PdCx phase, i.e. x = 4 at.% may also affect the observed.

  2. Path-integral theory of the scattering of 4He atoms at the surface of liquid 4He

    International Nuclear Information System (INIS)

    Swanson, D.R.; Edwards, D.O.

    1988-01-01

    The path-integral theory of the scattering of a 4 He atom near the free surface of liquid 4 He, which was originally formulated by Echenique and Pendry, has been recalculated with use of a physically realistic static potential and atom-ripplon interaction outside the liquid. The static potential and atom-ripplon interaction are based on the variational calculation of Edwards and Fatouros. An important assumption in the path-integral theory is the ''impulse approximation'': that the motion of the scattered atom is very fast compared with the motion of the surface due to ripplons. This is found to be true only for ripplons with wave vectors smaller than q/sub m/∼0.2 A/sup -1/. If ripplons above q/sub m/ made an important contribution to the scattering of the atom there would be a substantial dependence of the elastic reflection coefficient on the angle of incidence of the atom. Since this is not observed experimentally, it is argued that ripplons above q/sub m/ give a negligible effect and should be excluded from the calculation. With this modification the theory gives a good fit to the experimental reflection coefficient as a function of the momentum and angle of incidence of the atom. The new version of the theory indicates that there is a substantial probability that an atom may reach the surface of the liquid without exciting any ripplons. The theory is not valid when the atom enters the liquid but analysis of the experiments shows that, once inside the liquid, the atom has a negligible chance of being scattered out again

  3. Crossed beam reactive scattering of oxygen atoms and surface scattering studies of gaseous condensation

    International Nuclear Information System (INIS)

    Sibener, S.J.

    1979-09-01

    A high pressure, radio frequency discharge nozzle beam source was developed for the production of very intense (greater than or equal to 10 18 atoms sr -1 sec -1 ) supersonic beams of oxygen atoms. This source is capable of producing seeded beams of ground state O( 3 P/sub J/) atoms when dilute oxygen-argon mixtures are used, with molecular dissociation levels exceeding 80% being realized for operation at pressures up to 350 torr. When dilute oxygen-helium mixtures are employed both ground state O( 3 P/sub J/) and excited state O( 1 D 2 ) atoms are present in the terminal beam, with molecular dissociation levels typically exceeding 60% being achieved for operation at pressures up to 200 torr. Atomic oxygen mean translational energies from 0.14 to 0.50 eV were obtained using the seeded beams technique, with Mach numbers as high as 10 (FWHM Δ v/v approx. = 20%) being realized. The IC1, CF 3 I, C 6 H 6 , and C 6 D 6 reactions are discussed in detail. The IC1 and CF 3 I studies have enabled us to determine an improved value for the bond energy of the IO radical: D/sub o/(IO) = 55 +- 2 kcal/mole. The IO product angular and velocity distributions have been used to generate center-of-mass flux contour maps, which indicate that these two reactions proceed via relatively long-lived collision complexes whose mean lifetimes are slightly shorter than their respective rotational periods. The O( 3 P/sub J/) + C 6 H 6 and C 6 D 6 reactions were studied in order to elucidate the reaction mechanism, and, in particular, to identify the primary reaction products produced in these reactions. Finally, a series of beam-surface scattering experiments are described which examined the internal and translational energy dependence of molecular condensation probabilities for collisions involving either CC1 4 or SF 6 and their respective condensed phases. 117 references

  4. Rational Design of Hyperbranched Nanowire Systems for Tunable Superomniphobic Surfaces Enabled by Atomic Layer Deposition

    Energy Technology Data Exchange (ETDEWEB)

    Bielinski, Ashley R.; Boban, Mathew; He, Yang; Kazyak, Eric; Lee, Duck H.; Wang, Chongmin; Tuteja, Anish; Dasgupta, Neil P.

    2017-01-24

    A method for tunable control of geometry in hyperbranched ZnO nanowire (NW) systems is reported, which enables the rational design and fabrication of superomniphobic surfaces. Branched NWs with tunable density and orientation were grown via a sequential hydrothermal process, in which atomic layer deposition (ALD) was used for NW seeding, disruption of epitaxy, and selective blocking of NW nucleation. This approach allows for the rational design and optimization of three-level hierarchical structures, in which the geometric parameters of each level of hierarchy can be individually controlled. We demonstrate the coupled relationships between geometry and contact angle for a variety of liquids, which is supported by mathematical models of structural superomniphobicity. The highest performing superomniphobic surface was designed with three levels of hierarchy and achieved the following advancing/receding contact angles, water: 172°/170°, hexadecane: 166°/156°, octane: 162°/145°, and heptane: 160°/130°. Low surface tension liquids were shown to bounce off the surface from a height of 7 cm without breaking through and wetting. This approach demonstrates the power of ALD as an enabling technique for hierarchical materials by design, spanning the macro, micro, and nano length scales.

  5. Excellent c-Si surface passivation by low-temperature atomic layer deposited titanium oxide

    International Nuclear Information System (INIS)

    Liao, Baochen; Hoex, Bram; Aberle, Armin G.; Bhatia, Charanjit S.; Chi, Dongzhi

    2014-01-01

    In this work, we demonstrate that thermal atomic layer deposited (ALD) titanium oxide (TiO x ) films are able to provide a—up to now unprecedented—level of surface passivation on undiffused low-resistivity crystalline silicon (c-Si). The surface passivation provided by the ALD TiO x films is activated by a post-deposition anneal and subsequent light soaking treatment. Ultralow effective surface recombination velocities down to 2.8 cm/s and 8.3 cm/s, respectively, are achieved on n-type and p-type float-zone c-Si wafers. Detailed analysis confirms that the TiO x films are nearly stoichiometric, have no significant level of contaminants, and are of amorphous nature. The passivation is found to be stable after storage in the dark for eight months. These results demonstrate that TiO x films are also capable of providing excellent passivation of undiffused c-Si surfaces on a comparable level to thermal silicon oxide, silicon nitride, and aluminum oxide. In addition, it is well known that TiO x has an optimal refractive index of 2.4 in the visible range for glass encapsulated solar cells, as well as a low extinction coefficient. Thus, the results presented in this work could facilitate the re-emergence of TiO x in the field of high-efficiency silicon wafer solar cells.

  6. Topographical characterization of Ar-bombarded Si(1 1 1) surfaces by atomic force microscopy

    CERN Document Server

    Niebieskikwiat, D G; Pregliasco, G R; Gayone, J E; Grizzi, O; Sanchez, E A

    2002-01-01

    We used atomic force microscopy to study the topographical changes induced on Si(1 1 1) surfaces by 10-22 keV Ar sup + bombardment. The irradiation was carried on normal to the surface with doses in the 1-60x10 sup 1 sup 6 ions/cm sup 2 range. We observed a first generation of blisters at a critical dose around 3x10 sup 1 sup 6 ions/cm sup 2 , which flakes off at 19x10 sup 1 sup 6 ions/cm sup 2 , and a second generation of smaller blisters between 35 and 45x10 sup 1 sup 6 ions/cm sup 2. Measurements of the mean surface height show that at low irradiation doses the surface inflates because of voids produced by Ar sup + implantation. For doses greater than 20x10 sup 1 sup 6 Ar sup + /cm sup 2 the height decreases linearly because of sputtering, with a slope corresponding to a sputtering yield of 1.4. Finally, we present electron spectra produced during grazing proton bombardment of samples whose topography has been modified by Ar irradiation.

  7. Excellent c-Si surface passivation by low-temperature atomic layer deposited titanium oxide

    Science.gov (United States)

    Liao, Baochen; Hoex, Bram; Aberle, Armin G.; Chi, Dongzhi; Bhatia, Charanjit S.

    2014-06-01

    In this work, we demonstrate that thermal atomic layer deposited (ALD) titanium oxide (TiOx) films are able to provide a—up to now unprecedented—level of surface passivation on undiffused low-resistivity crystalline silicon (c-Si). The surface passivation provided by the ALD TiOx films is activated by a post-deposition anneal and subsequent light soaking treatment. Ultralow effective surface recombination velocities down to 2.8 cm/s and 8.3 cm/s, respectively, are achieved on n-type and p-type float-zone c-Si wafers. Detailed analysis confirms that the TiOx films are nearly stoichiometric, have no significant level of contaminants, and are of amorphous nature. The passivation is found to be stable after storage in the dark for eight months. These results demonstrate that TiOx films are also capable of providing excellent passivation of undiffused c-Si surfaces on a comparable level to thermal silicon oxide, silicon nitride, and aluminum oxide. In addition, it is well known that TiOx has an optimal refractive index of 2.4 in the visible range for glass encapsulated solar cells, as well as a low extinction coefficient. Thus, the results presented in this work could facilitate the re-emergence of TiOx in the field of high-efficiency silicon wafer solar cells.

  8. Electrode surface engineering by atomic layer deposition: A promising pathway toward better energy storage

    KAUST Repository

    Ahmed, Bilal

    2016-04-29

    Research on electrochemical energy storage devices including Li ion batteries (LIBs), Na ion batteries (NIBs) and supercapacitors (SCs) has accelerated in recent years, in part because developments in nanomaterials are making it possible to achieve high capacities and energy and power densities. These developments can extend battery life in portable devices, and open new markets such as electric vehicles and large-scale grid energy storage. It is well known that surface reactions largely determine the performance and stability of electrochemical energy storage devices. Despite showing impressive capacities and high energy and power densities, many of the new nanostructured electrode materials suffer from limited lifetime due to severe electrode interaction with electrolytes or due to large volume changes. Hence control of the surface of the electrode material is essential for both increasing capacity and improving cyclic stability of the energy storage devices.Atomic layer deposition (ALD) which has become a pervasive synthesis method in the microelectronics industry, has recently emerged as a promising process for electrochemical energy storage. ALD boasts excellent conformality, atomic scale thickness control, and uniformity over large areas. Since ALD is based on self-limiting surface reactions, complex shapes and nanostructures can be coated with excellent uniformity, and most processes can be done below 200. °C. In this article, we review recent studies on the use of ALD coatings to improve the performance of electrochemical energy storage devices, with particular emphasis on the studies that have provided mechanistic insight into the role of ALD in improving device performance. © 2016 Elsevier Ltd.

  9. The computer simulation of the structure of transition metal surface alloys

    International Nuclear Information System (INIS)

    Bilic, A.; King, B.V.; O'Connor, D.J.

    1999-01-01

    In recent years interest has arisen in connection with the thin alloy films of Al and Pd. Such films are created by deposition of ≥ 0.5 ML of Al onto Pd(001) and annealing to 750-950 K. The structure has been investigated using low-energy ion scattering (LEIS) and shows a p(2x2)-p4g clock reconstruction. A structure was proposed consisting of a clock-rotated Pd top layer over a c(2x2) Al-Pd underlayer. This paper presents a simulation study of the structure and energetics of Al dissolution into the Pd(001) surface using the embedded atom method (EAM)

  10. Optimization of Pd-B/γ-Al2O3 catalyst preparation for palm oil hydrogenation by response surface methodology (RSM

    Directory of Open Access Journals (Sweden)

    A. M. Alshaibani

    2014-03-01

    Full Text Available Response surface methodology was used to design and evaluate the experimental variables for Pd-B/γ-Al2O3 catalyst preparation. The catalyst was prepared by impregnation and chemical reduction. Thirteen different samples of the catalyst were prepared at different KOH concentrations and annealed at various temperatures, before applying them in palm oil hydrogenation. Hydrogenation was performed on a 0.12% Pd-B/γ-Al2O3 catalyst at a temperature of 393 K, hydrogen pressure of 500 kPa and agitation of 500 rpm for 1 h. The iodine value (IV and trans fatty acids (TFAs content responses were measured for each hydrogenated palm oil sample. The predicted models were verified for both responses and found to be statistically adequate. An optimization study was performed on the catalyst preparation variables for minimizing both IV and TFAs content. The Pd-B/γ-Al2O3 prepared under optimized conditions exhibited 47% higher conversion and 22% lower trans-isomerization selectivity than Escat 1241 commercial catalyst. The Pd-B/γ-Al2O3 catalyst preparation variables have a noticeable effect on palm oil hydrogenation conversion and trans-isomerization selectivity.

  11. Probing the surface charge on the basal planes of Kaolinite particles with high resolution Atomic Force Microscopy

    NARCIS (Netherlands)

    Kumar, Naveen; Andersson, M.P.; van den Ende, Henricus T.M.; Mugele, Friedrich Gunther; Sîretanu, Igor

    2017-01-01

    High-resolution atomic force microscopy is used to map the surface charge on the basal planes of kaolinite nanoparticles in an ambient solution of variable pH and NaCl or CaCl2 concentration. Using DLVO theory with charge regulation, we determine from the measured force–distance curves the surface

  12. Surface passivation of nano-textured fluorescent SiC by atomic layer deposited TiO2

    DEFF Research Database (Denmark)

    Lu, Weifang; Ou, Yiyu; Jokubavicius, Valdas

    2016-01-01

    Nano-textured surfaces have played a key role in optoelectronic materials to enhance the light extraction efficiency. In this work, morphology and optical properties of nano-textured SiC covered with atomic layer deposited (ALD) TiO2 were investigated. In order to obtain a high quality surface...

  13. Impact of Materials Processing on Microstructural Evolution and Hydrogen Isotope Storage Properties of Pd-Rh Alloy Powders.

    Energy Technology Data Exchange (ETDEWEB)

    Yee, Joshua K [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

    2015-02-01

    Cryomilled Pd - 10Rh was investiga ted as potential solid - state storage material of hydrogen. Pd - 10Rh was first atomized, and then subsequently cryomilled. The cryomilled Pd - 10Rh was then examined using microstructural characterization techniques including op tical microscopy, electron microscopy, and X - ray diffraction. Pd - 10Rh particles were significantly flattened, increasing the apparent surface area. Microstructural refinement was observed in the cryomilled Pd - 10Rh, generating grains at the nanom etric scale through dislocation - based activity. Hydrogen sorption properties were also characterized, generating both capacity as well as kinetics measurements. It was found that the microstructural refinement due to cryomilling did not play a significant role on hyd rogen sorption properties until the smallest grain size (on the order of %7E25 nm) was achieved. Additionally, the increased surface area and other changes in particle morphology were associated with cryomilling changed the kinetics of hydrogen absorption.

  14. Probing anisotropic surface properties and interaction forces of chrysotile rods by atomic force microscopy and rheology.

    Science.gov (United States)

    Yang, Dingzheng; Xie, Lei; Bobicki, Erin; Xu, Zhenghe; Liu, Qingxia; Zeng, Hongbo

    2014-09-16

    Understanding the surface properties and interactions of nonspherical particles is of both fundamental and practical importance in the rheology of complex fluids in various engineering applications. In this work, natural chrysotile, a phyllosilicate composed of 1:1 stacked silica and brucite layers which coil into cylindrical structure, was chosen as a model rod-shaped particle. The interactions of chrysotile brucite-like basal or bilayered edge planes and a silicon nitride tip were measured using an atomic force microscope (AFM). The force-distance profiles were fitted using the classical Derjaguin-Landau-Verwey-Overbeek (DLVO) theory, which demonstrates anisotropic and pH-dependent surface charge properties of brucite-like basal plane and bilayered edge surface. The points of zero charge (PZC) of the basal and edge planes were estimated to be around pH 10-11 and 6-7, respectively. Rheology measurements of 7 vol % chrysotile (with an aspect ratio of 14.5) in 10 mM NaCl solution showed pH-dependent yield stress with a local maximum around pH 7-9, which falls between the two PZC values of the edge and basal planes of the rod particles. On the basis of the surface potentials of the edge and basal planes obtained from AFM measurements, theoretical analysis of the surface interactions of edge-edge, basal-edge, and basal-basal planes of the chrysotile rods suggests the yield stress maximum observed could be mainly attributed to the basal-edge attractions. Our results indicate that the anisotropic surface properties (e.g., charges) of chrysotile rods play an important role in the particle-particle interaction and rheological behavior, which also provides insight into the basic understanding of the colloidal interactions and rheology of nonspherical particles.

  15. Ultracold atoms on atom chips

    DEFF Research Database (Denmark)

    Krüger, Peter; Hofferberth, S.; Haller, E.

    2005-01-01

    Miniaturized potentials near the surface of atom chips can be used as flexible and versatile tools for the manipulation of ultracold atoms on a microscale. The full scope of possibilities is only accessible if atom-surface distances can be reduced to microns. We discuss experiments in this regime...

  16. Atom-resolved surface chemistry using scanning tunneling microscopy (STM) and spectroscopy (STS)

    International Nuclear Information System (INIS)

    Avouris, P.

    1989-01-01

    The author shows that by using STM and STS one can study chemistry with atomic resolution. The author uses two examples: the reaction of Si(111)-(7x7) with (a) NH 3 and (b) decaborane (DB). In case (a) the authors can directly observe the spatial distribution of the reaction. He determined which surface atoms have reacted and how the products of the reaction are distributed. He found that the different dangling-bond sites have significantly different reactivities and explain these differences in terms of the local electronic structure. In case (b) the 7x7 reconstruction is eliminated and at high temperatures, (√3 x √3) R30 degree reconstructions are observed. Depending on the amount of DB and the annealing temperature the √3 structures contain variable numbers of B and Si adatoms on T 4 -sites. Calculations show that the structure involving B adatoms, although kinetically favored, is not the lowest energy configuration. The lowest energy state involves B in a substitutional site under a Si adatom

  17. Secondary atomization of water and isooctane drops impinging on tilted heated surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Moreira, A.L.N.; Moita, A.S. [Technical University of Lisbon, Department of Mechanical Engineering, Instituto Superior Tecnico, Lisbon (Portugal); Cossali, E.; Marengo, M.; Santini, M. [Universita degli Studi di Bergamo, Department of Industrial Engineering, Dalmine (Italy)

    2007-08-15

    The present paper reports an experimental study aimed at characterizing the effects of heat transfer on the secondary atomization, which occurs during droplet impact on hot surfaces at conditions reproducing those occurring at fuel injection in internal combustion engines. The experiments consider single isooctane and water droplets impacting at different angles on a stainless steel surface with known roughness and encompass a range of Weber numbers from 240 to 600 and heat transfer regimes from the film-vaporization up to the Leidenfrost regime. The mechanisms of secondary breakup are inferred from the temporal evolution of the morphology of the impact imaged with a CCD camera, together with instantaneous measurements of droplet size and velocity. The combination of a technique for image processing with a phase Doppler instrument allows evaluating extended size distributions from 5.5 {mu}m up to a few millimetres and to cover the full range of secondary droplet sizes observed at all heat transfer regimes and impaction angles. Temporal evolution of the size and velocity distributions are then determined. The experiments are reported at impact conditions at which disintegration does not occur at ambient temperature. So, any alteration observed in droplet impact behavior is thermally induced. The analysis is relevant for port fuel injection systems, where droplets injected to impact on the back surface of the valves, behave differently depending on fuel properties, particularly when the use of alcohols is considered, even as an additive to gasoline. (orig.)

  18. Atomic layer deposition in nanostructured photovoltaics: tuning optical, electronic and surface properties

    Science.gov (United States)

    Palmstrom, Axel F.; Santra, Pralay K.; Bent, Stacey F.

    2015-07-01

    Nanostructured materials offer key advantages for third-generation photovoltaics, such as the ability to achieve high optical absorption together with enhanced charge carrier collection using low cost components. However, the extensive interfacial areas in nanostructured photovoltaic devices can cause high recombination rates and a high density of surface electronic states. In this feature article, we provide a brief review of some nanostructured photovoltaic technologies including dye-sensitized, quantum dot sensitized and colloidal quantum dot solar cells. We then introduce the technique of atomic layer deposition (ALD), which is a vapor phase deposition method using a sequence of self-limiting surface reaction steps to grow thin, uniform and conformal films. We discuss how ALD has established itself as a promising tool for addressing different aspects of nanostructured photovoltaics. Examples include the use of ALD to synthesize absorber materials for both quantum dot and plasmonic solar cells, to grow barrier layers for dye and quantum dot sensitized solar cells, and to infiltrate coatings into colloidal quantum dot solar cell to improve charge carrier mobilities as well as stability. We also provide an example of monolayer surface modification in which adsorbed ligand molecules on quantum dots are used to tune the band structure of colloidal quantum dot solar cells for improved charge collection. Finally, we comment on the present challenges and future outlook of the use of ALD for nanostructured photovoltaics.

  19. Surface reaction mechanisms during ozone and oxygen plasma assisted atomic layer deposition of aluminum oxide.

    Science.gov (United States)

    Rai, Vikrant R; Vandalon, Vincent; Agarwal, Sumit

    2010-09-07

    We have elucidated the reaction mechanism and the role of the reactive intermediates in the atomic layer deposition (ALD) of aluminum oxide from trimethyl aluminum in conjunction with O(3) and an O(2) plasma. In situ attenuated total reflection Fourier transform infrared spectroscopy data show that both -OH groups and carbonates are formed on the surface during the oxidation cycle. These carbonates, once formed on the surface, are stable to prolonged O(3) exposure in the same cycle. However, in the case of plasma-assisted ALD, the carbonates decompose upon prolonged O(2) plasma exposure via a series reaction kinetics of the type, A (CH(3)) --> B (carbonates) --> C (Al(2)O(3)). The ratio of -OH groups to carbonates on the surface strongly depends on the oxidizing agent, and also the duration of the oxidation cycle in plasma-assisted ALD. However, in both O(3) and O(2) plasma cycles, carbonates are a small fraction of the total number of reactive sites compared to the hydroxyl groups.

  20. Atomic layer deposition in nanostructured photovoltaics: tuning optical, electronic and surface properties.

    Science.gov (United States)

    Palmstrom, Axel F; Santra, Pralay K; Bent, Stacey F

    2015-08-07

    Nanostructured materials offer key advantages for third-generation photovoltaics, such as the ability to achieve high optical absorption together with enhanced charge carrier collection using low cost components. However, the extensive interfacial areas in nanostructured photovoltaic devices can cause high recombination rates and a high density of surface electronic states. In this feature article, we provide a brief review of some nanostructured photovoltaic technologies including dye-sensitized, quantum dot sensitized and colloidal quantum dot solar cells. We then introduce the technique of atomic layer deposition (ALD), which is a vapor phase deposition method using a sequence of self-limiting surface reaction steps to grow thin, uniform and conformal films. We discuss how ALD has established itself as a promising tool for addressing different aspects of nanostructured photovoltaics. Examples include the use of ALD to synthesize absorber materials for both quantum dot and plasmonic solar cells, to grow barrier layers for dye and quantum dot sensitized solar cells, and to infiltrate coatings into colloidal quantum dot solar cell to improve charge carrier mobilities as well as stability. We also provide an example of monolayer surface modification in which adsorbed ligand molecules on quantum dots are used to tune the band structure of colloidal quantum dot solar cells for improved charge collection. Finally, we comment on the present challenges and future outlook of the use of ALD for nanostructured photovoltaics.

  1. Surface modification of nanodiamond through metal free atom transfer radical polymerization

    Science.gov (United States)

    Zeng, Guangjian; Liu, Meiying; Shi, Kexin; Heng, Chunning; Mao, Liucheng; Wan, Qing; Huang, Hongye; Deng, Fengjie; Zhang, Xiaoyong; Wei, Yen

    2016-12-01

    Surface modification of nanodiamond (ND) with poly(2-methacryloyloxyethyl phosphorylcholine) [poly(MPC)] has been achieved by using metal free surface initiated atom transfer radical polymerization (SI-ATRP). The ATRP initiator was first immobilized on the surface of ND through direct esterification reaction between hydroxyl group of ND and 2-bromoisobutyryl bromide. The initiator could be employed to obtain ND-poly(MPC) nanocomposites through SI-ATRP using an organic catalyst. The final functional materials were characterized by 1H nuclear magnetic resonance, transmission electron microscopy, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy and thermo gravimetric analysis in detailed. All of these characterization results demonstrated that ND-poly(MPC) have been successfully obtained via metal free photo-initiated SI-ATRP. The ND-poly(MPC) nanocomposites shown enhanced dispersibility in various solvents as well as excellent biocompatibility. As compared with traditional ATRP, the metal free ATRP is rather simple and effective. More importantly, this preparation method avoided the negative influence of metal catalysts. Therefore, the method described in this work should be a promising strategy for fabrication of polymeric nanocomposites with great potential for different applications especially in biomedical fields.

  2. Highly sensitive work function hydrogen gas sensor based on PdNPs/SiO2/Si structure at room temperature

    Science.gov (United States)

    Behzadi pour, G.; Fekri aval, L.

    In this study, fabrication of highly sensitive PdNPs/SiO2/Si hydrogen gas sensor using experimental and theoretical methods has been investigated. Using chemical method the PdNPs are synthesized and characterized by X-ray diffraction (XRD). The average size of PdNPs is 11 nm. The thickness of the oxide film was 20 nm and the surface of oxide film analyzed using Atomic-force microscopy (AFM). The C-V curve for the PdNPs/SiO2/Si hydrogen gas sensor in 1% hydrogen concentration and at the room temperature has been reported. The response time and recovery time for 1% hydrogen concentration at room temperature were 1.2 s and 10 s respectively. The response (R%) for PdNPs/SiO2/Si MOS capacitor hydrogen sensor was 96%. The PdNPs/SiO2/Si MOS capacitor hydrogen sensor showed very fast response and recovery times compared to SWCNTs/PdNPs, graphene/PdNPs, nanorod/PdNPs and nanowire/PdNPs hydrogen gas sensors.

  3. Highly sensitive work function hydrogen gas sensor based on PdNPs/SiO2/Si structure at room temperature

    Directory of Open Access Journals (Sweden)

    G. Behzadi pour

    Full Text Available In this study, fabrication of highly sensitive PdNPs/SiO2/Si hydrogen gas sensor using experimental and theoretical methods has been investigated. Using chemical method the PdNPs are synthesized and characterized by X-ray diffraction (XRD. The average size of PdNPs is 11 nm. The thickness of the oxide film was 20 nm and the surface of oxide film analyzed using Atomic-force microscopy (AFM. The C-V curve for the PdNPs/SiO2/Si hydrogen gas sensor in 1% hydrogen concentration and at the room temperature has been reported. The response time and recovery time for 1% hydrogen concentration at room temperature were 1.2 s and 10 s respectively. The response (R% for PdNPs/SiO2/Si MOS capacitor hydrogen sensor was 96%. The PdNPs/SiO2/Si MOS capacitor hydrogen sensor showed very fast response and recovery times compared to SWCNTs/PdNPs, graphene/PdNPs, nanorod/PdNPs and nanowire/PdNPs hydrogen gas sensors. Keywords: Sensitive, Oxide film, Capacitive, Resistance

  4. Thermosensitive Nanocables Prepared by Surface-Initiated Atom Transfer Radical Polymerization

    Directory of Open Access Journals (Sweden)

    Wei Qingshan

    2008-01-01

    Full Text Available Abstract Thermosensitive nanocables consisting of Au nanowire cores and poly(N-isopropylacrylamide sheaths (denoted as Au/PNIPAAm were synthesized by surface-initiated atom transfer radical polymerization (SI-ATRP. The formation of PNIPAAm sheath was verified by Fourier transform infrared (FTIR and hydrogen nuclear magnetic resonance (1H NMR spectroscopy. Transmission electron microscope (TEM results confirmed the core/shell structure of nanohybrids. The thickness and density of PNIPAAm sheaths can be adjusted by controlling the amount of cross-linker during the polymerization. Signature temperature response was observed from Au/cross-linked-PNIPAAm nanocables. Such smart nanocables show immense potentials as building blocks for novel thermosensitive nanodevices in future.

  5. [Determination of ru, rh and Pd in 30% trialkyl phosphine oxide (TRPO)-kerosene by inductively coupled plasma-atomic emission spectrum (ICP-AES)].

    Science.gov (United States)

    Wang, Jian-Chen; Zhang, Lin

    2013-07-01

    The determination method of Ru, Rh and Pd in 30% TRPO-kerosene ICP-AES was studied by using aqueous calibration reference solution and choosing ethanol as diluent. The effects of the contents of 30% TRPO-kerosene and aqueous solution and the concentration of HNO3 in 30% TRPO-kerosene on the intensities of Ru, Rh and Pd were described. The optimized condition for preparing samples and calibration solutions was chosen as follows: The contents of 30% TRPO-kerosene and aqueous phase were 10% (V/V) and 5% (V/V) respectively and the concentration of HNO3 30% TRPO-kerosene was 0.20 mol x L(-1). The determination method of Au, Ru and Pd was set up according to the above condition. The detection limit, precision and recovery ratio of Ru, Rh and Pd are well. The method is not only used in determination of Au, Ru and Pd in 30% TRPO-kerosene, but also used in other organic phases.

  6. Atomic and molecular adsorption on transition-metal carbide (111) surfaces from density-functional theory: a trend study of surface electronic factors

    DEFF Research Database (Denmark)

    Vojvodic, Aleksandra; Ruberto, C.; Lundqvist, Bengt

    2010-01-01

    This study explores atomic and molecular adsorption on a number of early transition-metal carbides (TMCs) in NaCl structure by means of density-functional theory calculations. The investigated substrates are the TM-terminated TMC(111) surfaces, of interest because of the presence of different types......, surface relaxations, Bader charges, and surface-localized densities of states (DOSs). Detailed comparisons between surface and bulk DOSs reveal the existence of transition-metal localized SRs (TMSRs) in the pseudogap and of several C-localized SRs (CSRs) in the upper valence band on all considered TMC(111......) surfaces. The spatial extent and the dangling bond nature of these SRs are supported by real-space analyses of the calculated Kohn-Sham wavefunctions. Then, atomic and molecular adsorption energies, geometries, and charge transfers are presented. An analysis of the adsorbate-induced changes in surface DOSs...

  7. PREFACE: International Conference on Many Particle Spectroscopy of Atoms, Molecules, Clusters and Surfaces (MPS2014)

    Science.gov (United States)

    Ancarani, Lorenzo Ugo

    2015-04-01

    This volume contains a collection of contributions from the invited speakers at the 2014 edition of the International Conference on Many Particle Spectroscopy of Atoms, Molecules, Clusters and Surfaces held in Metz, France, from 15th to 18th July 2014. This biennial conference alternates with the ICPEAC satellite International Symposium on (e,2e), Double Photoionization and Related Topics, and is concerned with experimental and theoretical studies of radiation interactions with matter. These include many-body and electron-electron correlation effects in excitation, and in single and multiple ionization of atoms, molecules, clusters and surfaces with various projectiles: electrons, photons and ions. More than 80 scientists, from 19 different countries around the world, came together to discuss the most recent progress on these topics. The scientific programme included 28 invited talks and a poster session extending over the three days of the meeting. Amongst the 51 posters, 11 have been selected and were advertised through short talks. Besides, Professor Nora Berrah gave a talk in memory of Professor Uwe Becker who sadly passed away shortly after co-chairing the previous edition of this conference. Financial support from the Institut Jean Barriol, Laboratoire SRSMC, Groupement de Recherche THEMS (CNRS), Ville de Metz, Metz Métropole, Conseil Général de la Moselle and Région Lorraine is gratefully acknowledged. Finally, I would like to thank the members of the local committee and the staff of the Université de Lorraine for making the conference run smoothly, the International Advisory Board for building up the scientific programme, the sessions chairpersons, those who gave their valuable time in carefully refereeing the articles of this volume and last, but not least, all participants for contributing to lively and fruitful discussions throughout the meeting.

  8. Features of static and dynamic friction profiles in one and two dimensions on polymer and atomically flat surfaces using atomic force microscopy

    International Nuclear Information System (INIS)

    Watson, G S; Watson, J A

    2008-01-01

    In this paper we correlate the Atomic Force Microscope probe movement with surface location while scanning in the imaging and Force versus distance modes. Static and dynamic stick-slip processes are described on a scale of nanometres to microns on a range of samples. We demonstrate the limits and range of the tip apex being fixed laterally in the force versus distance mode and static friction slope dependence on probe parameters. Micron scale static and dynamic friction can be used to purposefully manipulate soft surfaces to produce well defined frictional gradients

  9. Effect of post heat-treatment of composition-controlled PdFe nanoparticles for oxygen reduction reaction

    Science.gov (United States)

    Kang, Yun Sik; Choi, Kwang-Hyun; Ahn, Docheon; Lee, Myeong Jae; Baik, Jaeyoon; Chung, Dong Young; Kim, Mi-Ju; Lee, Stanfield Youngwon; Kim, Minhyoung; Shin, Heejong; Lee, Kug-Seung; Sung, Yung-Eun

    2016-01-01

    Composition-controlled and carbon-supported PdFe nanoparticles (NPs) were prepared via a modified chemical synthesis after heat-treatment at high temperature under a reductive atmosphere. This novel synthesis, which combines the polyol reduction method and hydride method, was used to obtain monodispersed PdFe NPs. In addition, to induce structural modifications, the as-prepared PdFe NPs received heat-treatment under a reductive atmosphere. Structural characterization, including high-resolution powder diffraction (HRPD), X-ray photoelectron spectroscopy (XPS), and X-ray absorption spectroscopy (XAS) analysis, indicated that heat-treated PdFe NPs exhibited a higher degree of alloying and surface Pd atomic composition compared with as-prepared ones. Furthermore, new crystalline phases were detected after heat-treatment. Thanks to the structural alterations, heat-treated PdFe NPs showed ∼3 and ∼18 times higher mass- and area-normalized oxygen reduction reaction (ORR) activities, respectively than commercial Pt/C. Single cell testing with heat-treated PdFe catalysts exhibited a ∼2.5 times higher mass-normalized maximum power density than the reference cell. Surface structure analyses, including cyclic voltammetry (CV), COad oxidation, and XPS, revealed that, after heat-treatment, a downshift of the Pd d-band center occurred, which led to a decrease in the affinity of Pd for oxygen species, resulting in more favorable ORR kinetics.

  10. Global optimization of bimetallic cluster structures. II. Size-matched Ag-Pd, Ag-Au, and Pd-Pt systems

    Science.gov (United States)

    Rossi, Giulia; Ferrando, Riccardo; Rapallo, Arnaldo; Fortunelli, Alessandro; Curley, Benjamin C.; Lloyd, Lesley D.; Johnston, Roy L.

    2005-05-01

    Genetic algorithm global optimization of Ag-Pd, Ag-Au, and Pd-Pt clusters is performed. The 34- and 38-atom clusters are optimized for all compositions. The atom-atom interactions are modeled by a semiempirical potential. All three systems are characterized by a small size mismatch and a weak tendency of the larger atoms to segregate at the surface of the smaller ones. As a result, the global minimum structures exhibit a larger mixing than in Ag-Cu and Ag-Ni clusters. Polyicosahedral structures present generally favorable energetic configurations, even though they are less favorable than in the case of the size-mismatched systems. A comparison between all the systems studied here and in the previous paper (on size-mismatched systems) is presented.

  11. Effect of flattened surface morphology of anodized aluminum oxide templates on the magnetic properties of nanoporous Co/Pt and Co/Pd thin multilayered films

    Science.gov (United States)

    Nguyen, T. N. Anh; Fedotova, J.; Kasiuk, J.; Bayev, V.; Kupreeva, O.; Lazarouk, S.; Manh, D. H.; Vu, D. L.; Chung, S.; Åkerman, J.; Altynov, V.; Maximenko, A.

    2018-01-01

    For the first time, nanoporous Al2O3 templates with smoothed surface relief characterized by flattened interpore areas were used in the fabrication of Co/Pd and Co/Pt multilayers (MLs) with strong perpendicular magnetic anisotropy (PMA). Alternating gradient magnetometry (AGM) revealed perfectly conserved PMA in the Co/Pd and Co/Pt porous MLs (antidot arrays) with a ratio of remanent magnetization (Mr) to saturation magnetization (MS) of about 0.99, anisotropy fields (Ha) of up to 2.6 kOe, and a small deviation angle of 8° between the easy magnetization axis and the normal to the film surface. The sufficient magnetic hardening of the porous MLs with enhanced coercive field HC of up to ∼1.9 kOe for Co/Pd and ∼1.5 kOe for Co/Pt MLs, as compared to the continuous reference samples (∼1.5-2 times), is associated with the pinning of the magnetic moments on the nanopore edges. Application of the Stoner-Wohlfarth model for fitting the experimental M/MS(H) curves yielded clear evidence of the predominantly coherent rotation mechanism of magnetization reversal in the porous films.

  12. Protective capping and surface passivation of III-V nanowires by atomic layer deposition

    Energy Technology Data Exchange (ETDEWEB)

    Dhaka, Veer, E-mail: veer.dhaka@aalto.fi; Perros, Alexander; Kakko, Joona-Pekko; Haggren, Tuomas; Lipsanen, Harri [Department of Micro- and Nanosciences, Micronova, Aalto University, P.O. Box 13500, FI-00076 (Finland); Naureen, Shagufta; Shahid, Naeem [Research School of Physics & Engineering, Department of Electronic Materials Engineering, Australian National University, Canberra ACT 2601 (Australia); Jiang, Hua; Kauppinen, Esko [Department of Applied Physics and Nanomicroscopy Center, Aalto University, P.O. Box 15100, FI-00076 (Finland); Srinivasan, Anand [School of Information and Communication Technology, KTH Royal Institute of Technology, Electrum 229, S-164 40 Kista (Sweden)

    2016-01-15

    Low temperature (∼200 °C) grown atomic layer deposition (ALD) films of AlN, TiN, Al{sub 2}O{sub 3}, GaN, and TiO{sub 2} were tested for protective capping and surface passivation of bottom-up grown III-V (GaAs and InP) nanowires (NWs), and top-down fabricated InP nanopillars. For as-grown GaAs NWs, only the AlN material passivated the GaAs surface as measured by photoluminescence (PL) at low temperatures (15K), and the best passivation was achieved with a few monolayer thick (2Å) film. For InP NWs, the best passivation (∼2x enhancement in room-temperature PL) was achieved with a capping of 2nm thick Al{sub 2}O{sub 3}. All other ALD capping layers resulted in a de-passivation effect and possible damage to the InP surface. Top-down fabricated InP nanopillars show similar passivation effects as InP NWs. In particular, capping with a 2 nm thick Al{sub 2}O{sub 3} layer increased the carrier decay time from 251 ps (as-etched nanopillars) to about 525 ps. Tests after six months ageing reveal that the capped nanostructures retain their optical properties. Overall, capping of GaAs and InP NWs with high-k dielectrics AlN and Al{sub 2}O{sub 3} provides moderate surface passivation as well as long term protection from oxidation and environmental attack.

  13. Protective capping and surface passivation of III-V nanowires by atomic layer deposition

    Directory of Open Access Journals (Sweden)

    Veer Dhaka

    2016-01-01

    Full Text Available Low temperature (∼200 °C grown atomic layer deposition (ALD films of AlN, TiN, Al2O3, GaN, and TiO2 were tested for protective capping and surface passivation of bottom-up grown III-V (GaAs and InP nanowires (NWs, and top-down fabricated InP nanopillars. For as-grown GaAs NWs, only the AlN material passivated the GaAs surface as measured by photoluminescence (PL at low temperatures (15K, and the best passivation was achieved with a few monolayer thick (2Å film. For InP NWs, the best passivation (∼2x enhancement in room-temperature PL was achieved with a capping of 2nm thick Al2O3. All other ALD capping layers resulted in a de-passivation effect and possible damage to the InP surface. Top-down fabricated InP nanopillars show similar passivation effects as InP NWs. In particular, capping with a 2 nm thick Al2O3 layer increased the carrier decay time from 251 ps (as-etched nanopillars to about 525 ps. Tests after six months ageing reveal that the capped nanostructures retain their optical properties. Overall, capping of GaAs and InP NWs with high-k dielectrics AlN and Al2O3 provides moderate surface passivation as well as long term protection from oxidation and environmental attack.

  14. Catalytic Activity and Stability of Oxides: The Role of Near-Surface Atomic Structures and Compositions

    KAUST Repository

    Feng, Zhenxing

    2016-05-05

    Conspectus Electrocatalysts play an important role in catalyzing the kinetics for oxygen reduction and oxygen evolution reactions for many air-based energy storage and conversion devices, such as metal–air batteries and fuel cells. Although noble metals have been extensively used as electrocatalysts, their limited natural abundance and high costs have motivated the search for more cost-effective catalysts. Oxides are suitable candidates since they are relatively inexpensive and have shown reasonably high activity for various electrochemical reactions. However, a lack of fundamental understanding of the reaction mechanisms has been a major hurdle toward improving electrocatalytic activity. Detailed studies of the oxide surface atomic structure and chemistry (e.g., cation migration) can provide much needed insights for the design of highly efficient and stable oxide electrocatalysts. In this Account, we focus on recent advances in characterizing strontium (Sr) cation segregation and enrichment near the surface of Sr-substituted perovskite oxides under different operating conditions (e.g., high temperature, applied potential), as well as their influence on the surface oxygen exchange kinetics at elevated temperatures. We contrast Sr segregation, which is associated with Sr redistribution in the crystal lattice near the surface, with Sr enrichment, which involves Sr redistribution via the formation of secondary phases. The newly developed coherent Bragg rod analysis (COBRA) and energy-modulated differential COBRA are uniquely powerful ways of providing information about surface and interfacial cation segregation at the atomic scale for these thin film electrocatalysts. In situ ambient pressure X-ray photoelectron spectroscopy (APXPS) studies under electrochemical operating conditions give additional insights into cation migration. Direct COBRA and APXPS evidence for surface Sr segregation was found for La1–xSrxCoO3−δ and (La1–ySry)2CoO4±δ/La1–xSrxCoO3

  15. Boron Nitride Nanoporous Membranes with High Surface Charge by Atomic Layer Deposition.

    Science.gov (United States)

    Weber, Matthieu; Koonkaew, Boonprakrong; Balme, Sebastien; Utke, Ivo; Picaud, Fabien; Iatsunskyi, Igor; Coy, Emerson; Miele, Philippe; Bechelany, Mikhael

    2017-05-17

    In this work, we report the design and the fine-tuning of boron nitride single nanopore and nanoporous membranes by atomic layer deposition (ALD). First, we developed an ALD process based on the use of BBr 3 and NH 3 as precursors in order to synthesize BN thin films. The deposited films were characterized in terms of thickness, composition, and microstructure. Next, we used the newly developed process to grow BN films on anodic aluminum oxide nanoporous templates, demonstrating the conformality benefit of BN prepared by ALD, and its scalability for the manufacturing of membranes. For the first time, the ALD process was then used to tune the diameter of fabricated single transmembrane nanopores by adjusting the BN thickness and to enable studies of the fundamental aspects of ionic transport on a single nanopore. At pH = 7, we estimated a surface charge density of 0.16 C·m -2 without slip and 0.07 C·m -2 considering a reasonable slip length of 3 nm. Molecular dynamics simulations performed with experimental conditions confirmed the conductivities and the sign of surface charges measured. The high ion transport results obtained and the ability to fine-tune nanoporous membranes by such a scalable method pave the way toward applications such as ionic separation, energy harvesting, and ultrafiltration devices.

  16. Quantum dynamics of STM and laser induced desorption of atoms and molecules from surfaces

    CERN Document Server

    Boendgen, G

    2001-01-01

    The manipulation of atoms and molecules at solid surfaces by electronic excitations with electrons (or holes) emitted from the tip of a scanning tunneling microscope (STM) or with laser radiation is both of applied and fundamental interest, e.g. for micro- and nanostructuring of materials, the clarification of elementary (catalytic) reaction mechanisms and for the question of how to treat the quantum dynamics of a laser or STM driven 'system' (the adsorbate) in contact with a dissipative (energy-withdrawing) 'bath' (the substrate). Desorption induced by electronic transitions (DIET) and its variant DIMET (M = multiple) are among the simplest possible 'reactions' of adsorbate-surface systems; usually involving extremely short-lived electronically excited intermediates. In this thesis, the ultra-short dynamics of directly (localised to the adsorbate-substrate complex) and indirectly (i.e., through the substrate) stimulated DIET and DIMET processes was studied for Si(100)-(2x1):H(D) and Pt(111):NO. Isotope effec...

  17. Surface passivation of efficient nanotextured black silicon solar cells using thermal atomic layer deposition.

    Science.gov (United States)

    Wang, Wei-Cheng; Lin, Che-Wei; Chen, Hsin-Jui; Chang, Che-Wei; Huang, Jhih-Jie; Yang, Ming-Jui; Tjahjono, Budi; Huang, Jian-Jia; Hsu, Wen-Ching; Chen, Miin-Jang

    2013-10-09

    Efficient nanotextured black silicon solar cells passivated by an Al2O3 layer are demonstrated. The broadband antireflection of the nanotextured black silicon solar cells was provided by fabricating vertically aligned silicon nanowire (SiNW) arrays on the n(+) emitter. A highly conformal Al2O3 layer was deposited upon the SiNW arrays by the thermal atomic layer deposition (ALD) based on the multiple pulses scheme. The nanotextured black silicon wafer covered with the Al2O3 layer exhibited a low total reflectance of ∼1.5% in a broad spectrum from 400 to 800 nm. The Al2O3 passivation layer also contributes to the suppressed surface recombination, which was explored in terms of the chemical and field-effect passivation effects. An 8% increment of short-circuit current density and 10.3% enhancement of efficiency were achieved due to the ALD Al2O3 surface passivation and forming gas annealing. A high efficiency up to 18.2% was realized in the ALD Al2O3-passivated nanotextured black silicon solar cells.

  18. Electronic passivation of silicon surfaces by thin films of atomic layer deposited gallium oxide

    International Nuclear Information System (INIS)

    Allen, T. G.; Cuevas, A.

    2014-01-01

    This paper proposes the application of gallium oxide (Ga 2 O 3 ) thin films to crystalline silicon solar cells. Effective passivation of n- and p-type crystalline silicon surfaces has been achieved by the application of very thin Ga 2 O 3 films prepared by atomic layer deposition using trimethylgallium (TMGa) and ozone (O 3 ) as the reactants. Surface recombination velocities as low as 6.1 cm/s have been recorded with films less than 4.5 nm thick. A range of deposition parameters has been explored, with growth rates of approximately 0.2 Å/cycle providing optimum passivation. The thermal activation energy for passivation of the Si-Ga 2 O 3 interface has been found to be approximately 0.5 eV. Depassivation of the interface was observed for prolonged annealing at increased temperatures. The activation energy for depassivation was measured to be 1.9 eV.

  19. Atomic Layer-Deposited TiO2 Coatings on NiTi Surface

    Science.gov (United States)

    Vokoun, D.; Racek, J.; Kadeřávek, L.; Kei, C. C.; Yu, Y. S.; Klimša, L.; Šittner, P.

    2018-02-01

    NiTi shape-memory alloys may release poisonous Ni ions at the alloys' surface. In an attempt to prepare a well-performing surface layer on an NiTi sample, the thermally grown TiO2 layer, which formed during the heat treatment of NiTi, was removed and replaced with a new TiO2 layer prepared using the atomic layer deposition (ALD) method. Using x-ray photoelectron spectroscopy, it was found that the ALD layer prepared at as low a temperature as 100 °C contained Ti in oxidation states + 4 and + 3. As for static corrosion properties of the ALD-coated NiTi samples, they further improved compared to those covered by thermally grown oxide. The corrosion rate of samples with thermally grown oxide was 1.05 × 10-5 mm/year, whereas the corrosion rate of the ALD-coated samples turned out to be about five times lower. However, cracking of the ALD coating occurred at about 1.5% strain during the superelastic mechanical loading in tension taking place via the propagation of a localized martensite band.

  20. Predicting Ligand Binding Sites on Protein Surfaces by 3-Dimensional Probability Density Distributions of Interacting Atoms

    Science.gov (United States)

    Jian, Jhih-Wei; Elumalai, Pavadai; Pitti, Thejkiran; Wu, Chih Yuan; Tsai, Keng-Chang; Chang, Jeng-Yih; Peng, Hung-Pin; Yang, An-Suei

    2016-01-01

    Predicting ligand binding sites (LBSs) on protein structures, which are obtained either from experimental or computational methods, is a useful first step in functional annotation or structure-based drug design for the protein structures. In this work, the structure-based machine learning algorithm ISMBLab-LIG was developed to predict LBSs on protein surfaces with input attributes derived from the three-dimensional probability density maps of interacting atoms, which were reconstructed on the query protein surfaces and were relatively insensitive to local conformational variations of the tentative ligand binding sites. The prediction accuracy of the ISMBLab-LIG predictors is comparable to that of the best LBS predictors benchmarked on several well-established testing datasets. More importantly, the ISMBLab-LIG algorithm has substantial tolerance to the prediction uncertainties of computationally derived protein structure models. As such, the method is particularly useful for predicting LBSs not only on experimental protein structures without known LBS templates in the database but also on computationally predicted model protein structures with structural uncertainties in the tentative ligand binding sites. PMID:27513851

  1. Surface smoothing effect of an amorphous thin film deposited by atomic layer deposition on a surface with nano-sized roughness

    Directory of Open Access Journals (Sweden)

    W. S. Lau

    2014-02-01

    Full Text Available Previously, Lau (one of the authors pointed out that the deposition of an amorphous thin film by atomic layer deposition (ALD on a substrate with nano-sized roughness probably has a surface smoothing effect. In this letter, polycrystalline zinc oxide deposited by ALD onto a smooth substrate was used as a substrate with nano-sized roughness. Atomic force microscopy (AFM and cross-sectional transmission electron microscopy (XTEM were used to demonstrate that an amorphous aluminum oxide thin film deposited by ALD can reduce the surface roughness of a polycrystalline zinc oxide coated substrate.

  2. Nanoscale fabrication and characterization of chemically modified silicon surfaces using conductive atomic force microscopy in liquids

    Science.gov (United States)

    Kinser, Christopher Reagan

    This dissertation examines the modification and characterization of hydrogen-terminated silicon surfaces in organic liquids. Conductive atomic force microscope (cAFM) lithography is used to fabricate structures with sub-100 nm line width on H:Si(111) in n-alkanes, 1-alkenes, and 1-alkanes. Nanopatterning is accomplished by applying a positive (n-alkanes and 1-alkenes) or a negative (1-alkanes) voltage pulse to the silicon substrate with the cAFM tip connected to ground. The chemical and kinetic behavior of the patterned features is characterized using AFM, lateral force microscopy, time-of-flight secondary ion mass spectroscopy (TOF SIMS), and chemical etching. Features patterned in hexadecane, 1-octadecene, and undecylenic acid methyl ester exhibited chemical and kinetic behavior consistent with AFM field induced oxidation. The oxide features are formed due to capillary condensation of a water meniscus at the AFM tip-sample junction. A space-charge limited growth model is proposed to explain the observed growth kinetics. Surface modifications produced in the presence of neat 1-dodecyne and 1-octadecyne exhibited a reduced lateral force compared to the background H:Si(111) substrate and were resistant to a hydrofluoric acid etch, characteristics which indicate that the patterned features are not due to field induced oxidation and which are consistent with the presence of the methyl-terminated 1-alkyne bound directly to the silicon surface through silicon-carbon bonds. In addition to the cAFM patterned surfaces, full monolayers of undecylenic acid methyl ester (SAM-1) and undec-10-enoic acid 2-bromoethyl ester (SAM-2) were grown on H:Si(111) substrates using ultraviolet light. The structure and chemistry of the monolayers were characterized using AFM, TOF SIMS, X-ray photoelectron spectroscopy (XPS), X-ray reflectivity (XRR), X-ray standing waves (XSW), and X-ray fluorescence (XRF). These combined analyses provide evidence that SAM-1 and SAM-2 form dense monolayers

  3. Analysis of Field Emission of Fabricated Nanogap in Pd Strips for Surface Conduction Electron-Emitter Displays

    Science.gov (United States)

    Lo, Hsiang-Yu; Li, Yiming; Tsai, Chih-Hao; Pan, Fu-Ming

    2008-04-01

    We study the field emission (FE) property of a nanometer-scale gap structure in a palladium strip, which was fabricated by hydrogen absorption under high-pressure treatment. A vigorous cracking process could be accompanied by extensive atomic migration during the hydrogen treatment. A three-dimensional finite-difference time-domain particle-in-cell method is adopted to simulate the electron emission in a surface-conduction electron-emitter display (SED) device. Examinations of conducting characteristics, FE efficiency, the local field around the emitter, and the current density on the anode plate with one FE emitter are conducted. The image of a light spot is successfully produced on a phosphor plate, which implies that the explored electrode with nanometer separation possesses a potential SED application. Experimental observation and numerical simulation show that the proposed structure can be used as a surface conduction electron emitter and has a high FE efficiency with low turn-on voltage and a different electron emission mechanism. This study benefits the advanced SED design for a new type of electron source.

  4. Significant change of local atomic configurations at surface of reduced activation Eurofer steels induced by hydrogenation treatments

    Energy Technology Data Exchange (ETDEWEB)

    Greculeasa, S.G.; Palade, P.; Schinteie, G. [National Institute for Materials Physics, P.O. Box MG-7, 77125, Bucharest-Magurele (Romania); Kuncser, A.; Stanciu, A. [National Institute for Materials Physics, P.O. Box MG-7, 77125, Bucharest-Magurele (Romania); University of Bucharest, Faculty of Physics, 77125, Bucharest-Magurele (Romania); Lungu, G.A. [National Institute for Materials Physics, P.O. Box MG-7, 77125, Bucharest-Magurele (Romania); Porosnicu, C.; Lungu, C.P. [National Institute for Laser, Plasma and Radiation Physics, 77125, Bucharest-Magurele (Romania); Kuncser, V., E-mail: kuncser@infim.ro [National Institute for Materials Physics, P.O. Box MG-7, 77125, Bucharest-Magurele (Romania)

    2017-04-30

    Highlights: • Engineering of Eurofer slab properties by hydrogenation treatments. • Hydrogenation modifies significantly the local atomic configurations at the surface. • Hydrogenation increases the expulsion of the Cr atoms toward the very surface. • Approaching binomial atomic distribution by hydrogenation in the next surface 100 nm. - Abstract: Reduced-activation steels such as Eurofer alloys are candidates for supporting plasma facing components in tokamak-like nuclear fusion reactors. In order to investigate the impact of hydrogen/deuterium insertion in their crystalline lattice, annealing treatments in hydrogen atmosphere have been applied on Eurofer slabs. The resulting samples have been analyzed with respect to local structure and atomic configuration both before and after successive annealing treatments, by X-ray diffractometry (XRD), scanning electron microscopy and energy dispersive spectroscopy (SEM-EDS), X-ray photoelectron spectroscopy (XPS) and conversion electron Mössbauer spectroscopy (CEMS). The corroborated data point out for a bcc type structure of the non-hydrogenated alloy, with an average alloy composition approaching Fe{sub 0.9}Cr{sub 0.1} along a depth of about 100 nm. EDS elemental maps do not indicate surface inhomogeneities in concentration whereas the Mössbauer spectra prove significant deviations from a homogeneous alloying. The hydrogenation increases the expulsion of the Cr atoms toward the surface layer and decreases their oxidation, with considerable influence on the surface properties of the steel. The hydrogenation treatment is therefore proposed as a potential alternative for a convenient engineering of the surface of different Fe-Cr based alloys.

  5. Hydrogel brushes grafted from stainless steel via surface-initiated atom transfer radical polymerization for marine antifouling

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Jingjing, E-mail: jjwang1@hotmail.com; Wei, Jun

    2016-09-30

    Highlights: • Crosslinked hydrogel brushes were grafted from SS surfaces for marine antifouling. • All brush-coated SS surfaces could effectively reduce the adhesion of biofouling. • The antifouling efficacy increased with the crosslinking density of hydrogels. - Abstract: Crosslinked hydrogel brushes were grafted from stainless steel (SS) surfaces for marine antifouling. The brushes were prepared by surface-initiated atom transfer radical polymerization (SI-ATRP) of 2-methacryloyloxyethyl phosphorylcholine (MPC) and poly(ethylene glycol) methyl ether methacrylate (PEGMA) respectively with different fractions of crosslinker in the feed. The grafted layers prepared with different thickness were characterized by X-ray photoelectron spectroscopy (XPS), atomic force microscopy (AFM), ellipsometry and water contact angle measurements. With the increase in the fraction of crosslinker in the feed, the thickness of the grafted layer increased and the surface became smooth. All the brush-coated SS surfaces could effectively reduce the adhesion of bacteria and microalgae and settlement of barnacle cyprids, as compared to the pristine SS surface. The antifouling efficacy of the PEGMA polymer (PPEGMA)-grafted surface was higher than that of the MPC polymer (PMPC)-grafted surfaces. Furthermore, the crosslinked hydrogel brush-grafted surfaces exhibited better fouling resistance than the non-crosslinked polymer brush-grafted surfaces, and the antifouling efficacy increased with the crosslinking density. These hydrogel coatings of low toxicity and excellent anti-adhesive characteristics suggested their useful applications as environmentally friendly antifouling coatings.

  6. Air–water interface of submerged superhydrophobic surfaces imaged by atomic force microscopy

    Directory of Open Access Journals (Sweden)

    Markus Moosmann

    2017-08-01

    Full Text Available Underwater air retention of superhydrophobic hierarchically structured surfaces is of increasing interest for technical applications. Persistent air layers (the Salvinia effect are known from biological species, for example, the floating fern Salvinia or the backswimmer Notonecta. The use of this concept opens up new possibilities for biomimetic technical applications in the fields of drag reduction, antifouling, anticorrosion and under water sensing. Current knowledge regarding the shape of the air–water interface is insufficient, although it plays a crucial role with regards to stability in terms of diffusion and dynamic conditions. Optical methods for imaging the interface have been limited to the micrometer regime. In this work, we utilized a nondynamic and nondestructive atomic force microscopy (AFM method to image the interface of submerged superhydrophobic structures with nanometer resolution. Up to now, only the interfaces of nanobubbles (acting almost like solids have been characterized by AFM at these dimensions. In this study, we show for the first time that it is possible to image the air–water interface of submerged hierarchically structured (micro-pillars surfaces by AFM in contact mode. By scanning with zero resulting force applied, we were able to determine the shape of the interface and thereby the depth of the water penetrating into the underlying structures. This approach is complemented by a second method: the interface was scanned with different applied force loads and the height for zero force was determined by linear regression. These methods open new possibilities for the investigation of air-retaining surfaces, specifically in terms of measuring contact area and in comparing different coatings, and thus will lead to the development of new applications.

  7. Investigation of integrin expression on the surface of osteoblast-like cells by atomic force microscopy

    Energy Technology Data Exchange (ETDEWEB)

    Caneva Soumetz, Federico [Department of Communication, Computer and System Sciences, University of Genova, Via Opera Pia, 13-16145 Genova (Italy); Saenz, Jose F. [Biophysical and Electronic Engineering Department, University of Genova, Via All' Opera Pia 11a, 16145 Genova (Italy); Pastorino, Laura; Ruggiero, Carmelina [Department of Communication, Computer and System Sciences, University of Genova, Via Opera Pia, 13-16145 Genova (Italy); Nosi, Daniele [Department of Anatomy, Histology and Forensic Medicine, Bio-photonic Laboratory, University of Florence, viale Morgagni, 85 Firenze, CAP 50134 Florence (Italy); Raiteri, Roberto, E-mail: rr@unige.it [Biophysical and Electronic Engineering Department, University of Genova, Via All' Opera Pia 11a, 16145 Genova (Italy)

    2010-03-15

    The transforming growth factor {beta}1 (TGF-{beta}1) is a human cytokine which has been demonstrated to modulate cell surface integrin repertoire. In this work integrin expression in response to TGF-{beta}1 stimulation has been investigated on the surface of human osteoblast-like cells. We used atomic force microscopy (AFM) and confocal laser scanning microscopy to assess integrin expression and to evaluate their distribution over the dorsal side of the plasma membrane. AFM probes have been covalently functionalised with monoclonal antibodies specific to the {beta}1 integrin subunit. Force curves have been collected in order to obtain maps of the interaction between the immobilized antibody and the respective cell membrane receptors. Adhesion peaks have been automatically detected by means of an ad hoc developed data analysis software. The specificity of the detected interactions has been assessed by adding free antibody in the solution and monitoring the dramatic decrease in the recorded interactions. In addition, the effect of TGF-{beta}1 treatment on both the fluorescence signal and the adhesion events has been tested. The level of expression of the {beta}1 integrin subunit was enhanced by TGF-{beta}1. As a further analysis, the adhesion force of the single living cells to the substrate was measured by laterally pushing the cell with the AFM tip and measuring the force necessary to displace it. The treatment with TGF-{beta}1 resulted in a decrease of the cell/substrate adhesion force. Results obtained by AFM have been validated by confocal laser scanning microscopy thus demonstrating the high potential of the AFM technique for the investigation of cell surface receptors distribution and trafficking at the nanoscale.

  8. Investigation of integrin expression on the surface of osteoblast-like cells by atomic force microscopy

    International Nuclear Information System (INIS)

    Caneva Soumetz, Federico; Saenz, Jose F.; Pastorino, Laura; Ruggiero, Carmelina; Nosi, Daniele; Raiteri, Roberto

    2010-01-01

    The transforming growth factor β1 (TGF-β1) is a human cytokine which has been demonstrated to modulate cell surface integrin repertoire. In this work integrin expression in response to TGF-β1 stimulation has been investigated on the surface of human osteoblast-like cells. We used atomic force microscopy (AFM) and confocal laser scanning microscopy to assess integrin expression and to evaluate their distribution over the dorsal side of the plasma membrane. AFM probes have been covalently functionalised with monoclonal antibodies specific to the β1 integrin subunit. Force curves have been collected in order to obtain maps of the interaction between the immobilized antibody and the respective cell membrane receptors. Adhesion peaks have been automatically detected by means of an ad hoc developed data analysis software. The specificity of the detected interactions has been assessed by adding free antibody in the solution and monitoring the dramatic decrease in the recorded interactions. In addition, the effect of TGF-β1 treatment on both the fluorescence signal and the adhesion events has been tested. The level of expression of the β1 integrin subunit was enhanced by TGF-β1. As a further analysis, the adhesion force of the single living cells to the substrate was measured by laterally pushing the cell with the AFM tip and measuring the force necessary to displace it. The treatment with TGF-β1 resulted in a decrease of the cell/substrate adhesion force. Results obtained by AFM have been validated by confocal laser scanning microscopy thus demonstrating the high potential of the AFM technique for the investigation of cell surface receptors distribution and trafficking at the nanoscale.

  9. Characterization of semiconductor surfaces and interfaces by high energy ion scattering

    International Nuclear Information System (INIS)

    Narusawa, Tadashi; Kobayashi, K.L.I.; Nakashima, Hisao

    1984-01-01

    The use of surface peak, which appears in MeV ion channeling experiments, is demonstrated as a local probe for direct and quantitative measurements of atomic displacements smaller than --0.1A. The atomic structures of GaAs(001)-c(4x4) clean surface and hydrogen-absorbed (1x1) surface are analyzed by this technique as well as the interface atomic structures of GaAs(001)-SiOsub(x) and Si(111)-Pd systems. (author)

  10. Organometallic Bonding in an Ullmann-Type On-Surface Chemical Reaction Studied by High-Resolution Atomic Force Microscopy.

    Science.gov (United States)

    Kawai, Shigeki; Sadeghi, Ali; Okamoto, Toshihiro; Mitsui, Chikahiko; Pawlak, Rémy; Meier, Tobias; Takeya, Jun; Goedecker, Stefan; Meyer, Ernst

    2016-10-01

    The on-surface Ullmann-type chemical reaction synthesizes polymers by linking carbons of adjacent molecules on solid surfaces. Although an organometallic compound is recently identified as the reaction intermediate, little is known about the detailed structure of the bonded organometallic species and its influence on the molecule and the reaction. Herein atomic force microscopy at low temperature is used to study the reaction with 3,9-diiododinaphtho[2,3-b:2',3'-d]thiophene (I-DNT-VW), which is polymerized on Ag(111) in vacuum. Thermally sublimated I-DNT-VW picks up a Ag surface atom, forming a CAg bond at one end after removing an iodine. The CAg bond is usually short-lived, and a CAgC organometallic bond immediately forms with an adjacent molecule. The existence of the bonded Ag atoms strongly affects the bending angle and adsorption height of the molecular unit. Density functional theory calculations reveal the bending mechanism, which reveals that charge from the terminus of the molecule is transferred via the Ag atom into the organometallic bond and strengths the local adsorption to the substrate. Such deformations vanish when the Ag atoms are removed by annealing and CC bonds are established. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  11. Adsorption of guaiacol on Fe (110) and Pd (111) from first principles

    Science.gov (United States)

    Hensley, Alyssa J. R.; Wang, Yong; McEwen, Jean-Sabin

    2016-06-01

    The catalytic properties of surfaces are highly dependent upon the effect said surfaces have on the geometric and electronic structure of adsorbed reactants, products, and intermediates. It is therefore crucial to have a surface-level understanding of the adsorption of the key species in a reaction in order to design active and selective catalysts. Here, we study the adsorption of guaiacol on Fe (110) and Pd (111) using dispersion-corrected density functional theory calculations as both of these metals are of interest as hydrodeoxygenation catalysts for the conversion of bio-oils to useable biofuels. Both vertical (via the oxygen functional groups) and horizontal (via the aromatic ring) adsorption configurations were examined and the resulting adsorption and molecular distortion energies showed that the vertical sites were only physisorbed while the horizontal sites were chemisorbed on both metal surfaces. A comparison of guaiacol's horizontal adsorption on Fe (110) and Pd (111) showed that guaiacol had a stronger adsorption on Pd (111) while the Fe (110) surface distorted the Csbnd O bonds to a greater degree. Electronic analyses on the horizontal systems showed that the greater adsorption strength for guaiacol on Pd (111) was likely due to the greater charge transfer between the aromatic ring and the surface Pd atoms. Additionally, the greater distortion of the Csbnd O bonds in adsorbed guaiacol on Fe (110) is likely due to the greater degree of interaction between the oxygen and surface Fe atoms. Overall, our results show that the Fe (110) surface has a greater degree of interaction with the functional groups and the Pd (111) surface has a greater degree of interaction with the aromatic ring.

  12. Nanoflowers of PdRu on PEDOT for Electrooxidation of Glycerol and Its Analysis

    International Nuclear Information System (INIS)

    Dash, Sthitaprajna; Munichandraiah, N.

    2015-01-01

    Graphical abstract: - Abstract: Poly(3,4-ethylenedioxythiophene) (PEDOT) supported PdRu catalysts with various Pd:Ru atomic ratios are prepared by one step electrodeposition method. The catalysts are characterised by several physicochemical techniques. The morphology depends on Pd:Ru ratio. The nanoflowers of Pd 5 Ru catalyst are deposited on PEDOT surface in an alloy form. Cyclic voltammetry experiments indicate that Ru improves the catalytic activity of Pd for glycerol oxidation significantly. However, the oxidation of glycerol is not observed on Ru-PEDOT/C electrode. Amongst all compositions, Pd 5 Ru nanoflowers on PEDOT exhibit the highest electrocatalytic activity and stability. Cyclic voltammetry and differential pulse voltammetry experiments are performed for the analysis of glycerol. Pd 5 Ru-PEDOT/C electrode is highly sensitive towards glycerol detection with sensitivity of 99.8 μA cm −2 μM −1 and low detection limit of 0.1 μM. Thus, electrochemically deposited nanoflowers Pd 5 Ru on PEDOT are efficient catalysts for direct glycerol oxidation as well as for analysis in alkaline media.

  13. Adsorption of selenium atoms at the Si(1 1 1)-7 x 7 surface: A combination of scanning tunnelling microscopy and density functional theory studies

    International Nuclear Information System (INIS)

    Wu, S.Q.; Zhou Yinghui; Wu Qihui; Pakes, C.I.; Zhu Zizhong

    2011-01-01

    Graphical abstract: A selenium atom, which adsorbs at site close to a Si adatom and bonds with this Si adatom and one of its backbonding Si atoms on the Si(1 1 1)-7 x 7 surface, will break the Si-Si bond and consequently disorder the Si reconstruction surface. Research highlights: → STM and DFT are used to study the adsorption properties of Se atoms on a Si surface. → The adsorption site of Se atom on the Si surface has been identified. → The electronic effect of Se atom on the adsorbed Si surface has been ivestigaed. → The Se atom weakens the bond between two Si atom bonding with the Se atom. - Abstract: The adsorption of selenium (Se) atoms at the Si(1 1 1)-7 x 7 surface has been investigated using both scanning tunnelling microscopy (STM) and density functional theory calculations. A single Se atom prefers to adsorb at sites close to a Si adatom and bonds with this Si adatom and one of its backbonding Si atoms. The adsorption sites are referred to as A*-type sites in this article. The density of the conduction band (empty states) of the Si adatom increases as a result of the adsorption of a Se atom, which causes the Si adatom to become brighter in the empty state STM images. At the same time, the adsorption of the Se atom weakens the bonding between the Si adatom and its backbonding Si atom due to the charge transfer from them to the Se atom, and consequently destructs the ordered Si(1 1 1)-7 x 7 surface with increasing Se coverage.

  14. Effect of different surface treatments and retainer designs on the retention of posterior Pd-Ag porcelain-fused-to-metal resin-bonded fixed partial dentures.

    Science.gov (United States)

    Chen, Xiwen; Zhang, Yixin; Zhou, Jinru; Chen, Chenfeng; Zhu, Zhimin; Li, Lei

    2018-02-01

    The aim of this study was to investigate the adhesive property of palladium-silver alloy (Pd-Ag) and the simulated clinical performance of Pd-Ag porcelain-fused-to-metal (PFM), resin-bonded, fixed partial dentures (RBFPDs). A total of 40 Pd-Ag discs (diameter=5 mm) were prepared and divided into the following four groups (n=10): a) No sandblasting, used as a control; and b, 50 µm; c, 110 µm; and d, 250 µm aluminum oxide (Al 2 O 3 ) particles, respectively. Another 50 discs were pre-sandblasted and divided into five groups (n=10) subjected to different treatments: e) Sandblasting, used as a control; f) silane; g) alloy primer; h) silica coating + silane and i) silica coating + alloy primer. All 90 discs were bonded to enamel with Panavia F 2.0 and then subjected to shear bond strength (SBS) testing. The fracture surfaces were examined by scanning electron microscopy. Next, 40 missing maxillary second premolar models were restored with one of the four following RBFPD designs (n=10): I) A premolar occlusal bar combined with molar double rests (MDR); II) both occlusal bars with a wing (OBB); III) a premolar occlusal bar combined with a molar dental band (MDB); and IV) two single rests adjacent to the edentulous space with a wing (SRB) used as a control. All specimens were aged with thermal cycling and mechanical loading. Subsequently, they were loaded until broken. The data were analyzed by one-way analysis of variance. Al 2 O 3 (250 µm) abrasion provided the highest SBS (P<0.05). The alloy primer and silica + silane exhibited increased SBS. Furthermore, fracture analysis revealed that the failure mode varied among the different treatments. Whereas MDB exhibited the highest retention (P<0.05), that of OBB was greater than that of MDR (P<0.05), and the control exhibited the lowest retention. Abrasion with Al 2 O 3 (250 µm) effectively increased the adhesive property of Pd-Ag. Additionally, treatment with the alloy primer and silica coating + silane was able to

  15. Effect of the Pd/MWCNTs anode catalysts preparation methods on their morphology and activity in a direct formic acid fuel cell

    Energy Technology Data Exchange (ETDEWEB)

    Lesiak, B., E-mail: blesiak-orlowska@ichf.edu.pl [Institute of Physical Chemistry, Polish Academy of Sciences, Kasprzaka 44/52, 01-224 Warszawa (Poland); Mazurkiewicz, M.; Malolepszy, A. [Faculty of Chemical and Process Engineering, Warsaw University of Technology, Waryńskiego 1, 00-645 Warszawa (Poland); Stobinski, L. [Institute of Physical Chemistry, Polish Academy of Sciences, Kasprzaka 44/52, 01-224 Warszawa (Poland); Faculty of Chemical and Process Engineering, Warsaw University of Technology, Waryńskiego 1, 00-645 Warszawa (Poland); Mierzwa, B.; Mikolajczuk-Zychora, A.; Juchniewicz, K.; Borodzinski, A. [Institute of Physical Chemistry, Polish Academy of Sciences, Kasprzaka 44/52, 01-224 Warszawa (Poland); Zemek, J.; Jiricek, P. [Institute of Physics, Academy of Sciences of the Czech Republic, 162-53 Prague 6, Cukrovarnicka 10 (Czech Republic)

    2016-11-30

    Highlights: • Catalysts properties studied by XRD, STEM, XPS methods. • Differences in Pd particle size, content of Pd, functional groups, PdC{sub x.}. • Catalytic activity studied in a Direct Formic Acid Fuel Cell. • Highest activity–catalyst prepared using a strong reducing agent (NaBH{sub 4}). - Abstract: Impact of Pd/MWCNTs catalysts preparation method on the catalysts morphology and activity in a formic acid electrooxidation reaction was investigated. Three reduction methods of Pd precursor involving reduction in a high pressure microwave reactor (Pd1), reduction with NaBH{sub 4} (Pd2) and microwave-assisted polyol method (Pd3) were used in this paper. Crystallites size and morphology were studied using the scanning transmission electron microscopy (STEM), X-ray diffraction (XRD), whereas elemental composition, Pd chemical state and functional groups content by the X-ray photoelectron spectroscopy (XPS). The prepared catalysts were tested in a direct formic acid fuel cell (DFAFC) as an anode material. The catalytic activity was correlated with a mean fraction of the total Pd atoms exposed at the surface (FE). The value of FE was calculated from the crystallites size distribution determined by the STEM measurements. Non-linear dependence of a current density versus FE, approaching the maximum at FE≈0.25 suggests that the catalytic process proceeded at Pd nanocrystallites faces, with inactive edges and corners. Pd2 catalyst exhibited highest activity due to its smallest Pd crystallites (3.2 nm), however the absence of Pd crystallites aggregation and low content of carbon in PdC{sub x} phase, i.e. x = 4 at.% may also affect the observed.

  16. Effect of local metal microstructure on adsorption on bimetallic surfaces: Atomic nitrogen on Ni/Pt(111)

    Science.gov (United States)

    Guo, Wei; Vlachos, Dionisios G.

    2013-05-01

    The adsorption of atomic nitrogen on Ni/Pt(111) surface bimetallics has been investigated as a function of the local microstructure of Ni and Pt atoms via density functional theory (DFT) calculations. Microstructures include surface and subsurface Ni atoms on Pt(111) as limiting cases, and also small clusters of Ni in the first and/or second layer of Pt. It is shown that the binding energy of N can be approximated as a perturbation from that on the host metal (Pt) with a linear short-ranged correction from the guest metal (Ni) that accounts for the coordination environment of nitrogen up to the 3rd nearest Ni neighbor. This model is rationalized with the d-band center theory. Coverage effects are also included. The model can be parameterized with a limited number of DFT calculations and applied to other bimetallic catalysts to estimate the coverage dependent binding energy on complex metal microstructures.

  17. Aerobic Oxidation of Cyclohexane on Catalysts Based on Twinned and Single-Crystal Au75Pd25 Bimetallic Nanocrystals.

    Science.gov (United States)

    Wang, Liangbing; Zhao, Songtao; Liu, Chenxuan; Li, Chen; Li, Xu; Li, Hongliang; Wang, Youcheng; Ma, Chao; Li, Zhenyu; Zeng, Jie

    2015-05-13

    Bimetallic Au75Pd25 nanocrystals with shapes of icosahedron and octahedron were synthesized by adding different amounts of iodide ions, and were employed as catalysts for solvent-free aerobic oxidation of cyclohexane. Although both icosahedrons and octahedrons were bounded by {111} facets, the turnover frequency number of Au75Pd25 icosahedrons reached 15,106 h(-1), almost three times as high as that of Au75Pd25 octahedrons. The conversion of cyclohexane reached 28.1% after 48 h using Au75Pd25 icosahedrons, with the selectivity of 84.3% to cyclohexanone. Density functional theory calculations along with X-ray photoelectron spectroscopy examinations reveal that the excellent catalytic performance of AuPd icosahedrons could be ascribed to twin-induced strain and highly negative charge density of Au atoms on the surface.

  18. Atom-by-atom assembly

    International Nuclear Information System (INIS)

    Hla, Saw Wai

    2014-01-01

    Atomic manipulation using a scanning tunneling microscope (STM) tip enables the construction of quantum structures on an atom-by-atom basis, as well as the investigation of the electronic and dynamical properties of individual atoms on a one-atom-at-a-time basis. An STM is not only an instrument that is used to ‘see’ individual atoms by means of imaging, but is also a tool that is used to ‘touch’ and ‘take’ the atoms, or to ‘hear’ their movements. Therefore, the STM can be considered as the ‘eyes’, ‘hands’ and ‘ears’ of the scientists, connecting our macroscopic world to the exciting atomic world. In this article, various STM atom manipulation schemes and their example applications are described. The future directions of atomic level assembly on surfaces using scanning probe tips are also discussed. (review article)

  19. Growth mechanisms for Si epitaxy on O atomic layers: Impact of O-content and surface structure

    Energy Technology Data Exchange (ETDEWEB)

    Jayachandran, Suseendran, E-mail: suseendran.jayachandran@imec.be [Imec, Kapeldreef 75, 3001 Leuven (Belgium); KU Leuven (University of Leuven), Department of Metallurgy and Materials, Castle Arenberg 44, B-3001 Leuven (Belgium); Billen, Arne [Imec, Kapeldreef 75, 3001 Leuven (Belgium); KU Leuven (University of Leuven), Department of Chemistry, Celestijnenlaan 200F, B-3001 Leuven (Belgium); Douhard, Bastien; Conard, Thierry; Meersschaut, Johan; Moussa, Alain; Caymax, Matty; Bender, Hugo [Imec, Kapeldreef 75, 3001 Leuven (Belgium); Vandervorst, Wilfried [Imec, Kapeldreef 75, 3001 Leuven (Belgium); KU Leuven (University of Leuven), Department of Physics and Astronomy, Celestijnenlaan 200D, B-3001 Leuven (Belgium); Heyns, Marc [Imec, Kapeldreef 75, 3001 Leuven (Belgium); KU Leuven (University of Leuven), Department of Metallurgy and Materials, Castle Arenberg 44, B-3001 Leuven (Belgium); Delabie, Annelies [Imec, Kapeldreef 75, 3001 Leuven (Belgium); KU Leuven (University of Leuven), Department of Chemistry, Celestijnenlaan 200F, B-3001 Leuven (Belgium)

    2016-10-30

    Highlights: • O{sub 3} or O{sub 2} exposures on H-Si(100) result in O ALs with different surface structures. • Si-EPI on O AL using O{sub 3} process is by direct epitaxial growth mechanism. • Si-EPI on O AL using O{sub 2} process is by epitaxial lateral overgrowth mechanism. • Distortions by O AL, SiH{sub 4} flux rate and Si thickness has an impact on Si-EPI quality. - Abstract: The epitaxial growth of Si layers on Si substrates in the presence of O atoms is generally considered a challenge, as O atoms degrade the epitaxial quality by generating defects. Here, we investigate the growth mechanisms for Si epitaxy on O atomic layers (ALs) with different O-contents and structures. O ALs are deposited by ozone (O{sub 3}) or oxygen (O{sub 2}) exposure on H-terminated Si at 50 °C and 300 °C respectively. Epitaxial Si is deposited by chemical vapor deposition using silane (SiH{sub 4}) at 500 °C. After O{sub 3} exposure, the O atoms are uniformly distributed in Si-Si dimer/back bonds. This O layer still allows epitaxial seeding of Si. The epitaxial quality is enhanced by lowering the surface distortions due to O atoms and by decreasing the arrival rate of SiH{sub 4} reactants, allowing more time for surface diffusion. After O{sub 2} exposure, the O atoms are present in the form of SiO{sub x} clusters. Regions of hydrogen-terminated Si remain present between the SiO{sub x} clusters. The epitaxial seeding of Si in these structures is realized on H-Si regions, and an epitaxial layer grows by a lateral overgrowth mechanism. A breakdown in the epitaxial ordering occurs at a critical Si thickness, presumably by accumulation of surface roughness.

  20. A Force field for tricalcium aluminate to characterize surface properties, initial hydration, and organically modified interfaces in atomic resolution

    OpenAIRE

    Mishra, Ratan K.; Fernández Carrasco, Lucía; Flatt, Robert J.; Heinz, Hendrik

    2014-01-01

    Tricalcium aluminate (C3A) is a major phase of Portland cement clinker and some dental root filling cements. An accurate all-atom force field is introduced to examine structural, surface, and hydration properties as well as organic interfaces to overcome challenges using current laboratory instrumentation. Molecular dynamics simulation demonstrates excellent agreement of computed structural, thermal, mechanical, and surface properties with available experimental data. The parameters are integ...

  1. Quasiclassical Studies of Eley-Rideal and Hot Atom Reactions on Surface: H(D)→D(H)+Cu(111)

    International Nuclear Information System (INIS)

    Vurdu, C.D.

    2004-01-01

    Randomly distributed hydrogen adsorbates on the surface of Cu(1 1 1) are used to form 0.50, 0.25 and 0.15 monolayers of coverages to simulate D(H)→H(D) + Cu(111) system at 30 K and 94 K surface temperatures. The interaction of this system is mimicked by a LEPS function which is parameterized by using the energy points which were calculated by a density-functional theory method and the generalized gradient approximation for the exchange-correlation energy for various configurations of one a,nd two hydrogen atoms on the Cu(111) surface. Our results on H 2 , D 2 , and HD formations via Eley-Redial and hot-atom mechanisms will be presented at these temperatures. Probabilities for the rotational, vibrational, total and translational energy distributions of the products are calculated. In addition traping onto the surface, inelastic reflection of the incident projectile and penetration of the adsorbate or projectile atom into the slab is analyzed. Hot-atom pathways for product formations are shown to make significant contributions

  2. Lateral gas phase diffusion length of boron atoms over Si/B surfaces during CVD of pure boron layers

    NARCIS (Netherlands)

    Mohammadi, V.; Nihtianov, S.

    2016-01-01

    The lateral gas phase diffusion length of boron atoms, LB, along silicon and boron surfaces during chemical vapor deposition(CVD) using diborane (B2H6) is reported. The value of LB is critical for reliable and uniform boron layer coverage. The presented information was obtained experimentally and

  3. An atomic force microscopy study on the transition from mushrooms to octopus surface ''micelles'' by changing the solvent quality

    NARCIS (Netherlands)

    Stamouli, A.; Pelletier, E.; Koutsos, V; van der Vegte, E.W.; Hadziioannou, G

    1996-01-01

    Atomic force microscopy (AFM) is used to study the behavior of a diblock copolymer onto a solid surface while the solvent quality is changed. In a first step, the copolymer poly(2-vinylpyridine)/polystyrene (P2VP/PS) is adsorbed onto mica from a selective solvent (the PS block is well solvated and

  4. Atomic structure of screw dislocations intersecting the Au(111) surface: A combined scanning tunneling microscopy and molecular dynamics study

    DEFF Research Database (Denmark)

    Engbæk, Jakob; Schiøtz, Jakob; Dahl-Madsen, Bjarke

    2006-01-01

    The atomic-scale structure of naturally occurring screw dislocations intersecting a Au(111) surface has been investigated both experimentally by scanning tunneling microscopy (STM) and theoretically using molecular dynamics (MD) simulations. The step profiles of 166 dislocations were measured using...

  5. MM99.50 - Surface Topography Characterization Using an Atomic Force Microscope Mounted on a Coordinate Measuring Machine

    DEFF Research Database (Denmark)

    Chiffre, Leonardo De; Hansen, Hans Nørgaard; Kofod, Niels

    1999-01-01

    The paper describes the construction, testing and use of an integrated system for topographic characterization of fine surfaces on parts having relatively big dimensions. An atomic force microscope (AFM) was mounted on a manual three-coordinate measuring machine (CMM) achieving free positioning...

  6. Measurements on hydrophobic and hydrophilic surfaces using a porous gamma alumina nanoparticle aggregate mounted on Atomic Force Microscopy cantilevers

    NARCIS (Netherlands)

    Das, Theerthankar; Becker, Thomas; Nair, Balagopal N.

    2010-01-01

    Atomic Force Microscopy (AFM) measurements are extensively used for a detailed understanding of molecular and surface forces. In this study, we present a technique for measuring such forces, using an AFM cantilever attached with a porous gamma alumina nanoparticle aggregate. The modified cantilever

  7. Surface segregation of the metal impurity to the (1 0 0) surface of fcc ...

    Indian Academy of Sciences (India)

    The surface segregation energies for a single metal impurity to the (100) surface of nine fcc metals (Cu, Ag, Au, Ni, Pd, Pt, Rh, Al and Ir) have been calculated using the MAEAM and molecular dynamics .... function (termed as a cut-off potential) while the separated distance between atoms varies in the range r2e to rc [33]:.

  8. Investigation of the adsorption of amino acids on Pd(1 1 1): A density functional theory study

    International Nuclear Information System (INIS)

    James, Joanna N.; Han, Jeong Woo; Sholl, David S.

    2014-01-01

    Graphical abstract: - Highlights: • Density functional theory calculations have been performed to study the adsorption of glycine, alanine, norvaline, valine, proline, cysteine, and serine on Pd(1 1 1). • The common structural framework for the adsorption of most amino acids onto Pd(1 1 1) is in a tridentate fashion via a nitrogen atom and two oxygen atoms. • The shifts in vibrational frequencies associated with NHH and COO support the adsorption patterns of amino acids we examined. • The adsorption strength of amino acids depends on how much the molecules deform during the adsorption process. - Abstract: Density functional theory calculations have been used to study the adsorption of glycine, alanine, norvaline, valine, proline, cysteine, and serine on Pd(1 1 1). Most amino acids except cysteine adsorb onto the surface in a tridentate fashion through a nitrogen atom and both oxygen atoms. For cysteine, an additional bond is formed with the surface due to the strong affinity of the sulfur atom, resulting in a significantly larger adsorption energy. The adsorption patterns of amino acids we examined are supported by the shifts in vibrational frequencies associated with NHH and COO. The adsorption strength of amino acids depends on how much the molecules deform during the adsorption process. Understanding the adsorption of amino acids on Pd(1 1 1) provides fundamental information for future consideration of the interactions between their derivatives or more complicated biomolecules and metal surfaces

  9. The method of local increments for the calculation of adsorption energies of atoms and small molecules on solid surfaces. Part I. A single Cu atom on the polar surfaces of ZnO.

    Science.gov (United States)

    Schmitt, Ilka; Fink, Karin; Staemmler, Volker

    2009-12-21

    The method of local increments is used in connection with the supermolecule approach and an embedded cluster model to calculate the adsorption energy of single Cu atoms at different adsorption sites at the polar surfaces of ZnO. Hartree-Fock calculations for the full system, adsorbed atom and solid surface, and for the fragments are the first step in this approach. In the present study, restricted open-shell Hartree-Fock (ROHF) calculations are performed since the Cu atom possesses a singly-occupied 4s orbital. The occupied Hartree-Fock orbitals are then localized by means of the Foster-Boys localization procedure. The correlation energies are expanded into a series of many-body increments which are evaluated separately and independently. In this way, the very time-consuming treatment of large systems is replaced with a series of much faster calculations for small subunits. In the present application, these subunits consist of the orbitals localized at the different atoms. Three adsorption situations with rather different bonding characteristics have been studied: a Cu atom atop a threefold-coordinated O atom of an embedded Zn(4)O(4) cluster, a Cu atom in an O vacancy site at the O-terminated ZnO(000-1) surface, and a Cu atom in a Zn vacancy site at the Zn-terminated ZnO(0001) surface. The following properties are analyzed in detail: convergence of the many-body expansion, contributions of the different n-body increments to the adsorption energy, treatment of the singly-occupied orbital as "localized" or "delocalized". Big savings in computer time can be achieved by this approach, particularly if only the localized orbitals in the individual increment under consideration are described by a large correlation adapted basis set, while all other orbitals are treated by a medium-size Hartree-Fock-type basis set. In this way, the method of local increments is a powerful alternative to the widely used methods like DFT or RI-MP2.

  10. Hyperthermal (10-500 eV) collisions of noble gases with Ni(100) surface. Comparison between light and heavy atom collisions

    International Nuclear Information System (INIS)

    Kim, C.

    1995-01-01

    Collisional events between 10-500 eV atomic beams (He, Ne, Ar, Kr, and Xe) and a Ni(100) surface are investigated by the classical trajectory method. The calculation employs a molecular dynamics approach combined with a Langevin method for treating energy dissipation to infinite solid. We find that low energy collisions of heavy atoms (Xe and Kr) are characterized by extensive many-body interactions with top layer surface atoms. On the other hand, light atom (Ne and He) collisions can be approximated as a sequence of binary collisions even at these energies. Such a difference in the collisional nature gives rise to the following consequences. Low energy heavy atoms transfer energy mostly to the surface atoms during 45 angle collision. They scatter from the surface with a narrow angular distribution centered in a supraspecular direction. The ratio of the scattered to incident particle energy rapidly decreases with increasing beam energy of heavy atoms. The sputtering yield for Ni atoms by heavy atom bombardment increases quite linearly with beam energy, which is attributed to a linear proportionality between the beam energy and the energy transfered to a surface. Near the threshold energy sputtering can occur more efficiently by light atom bombardment. The energy transfer ratio to solid continuously increases with beam energy for light atoms. For heavy projectiles, on the other hand, this ratio reaches a maximum at the energy of ca, 100 eV, above which it stays nearly constant but slightly decreases. ((orig.))

  11. Stabilizing small molecules on metal oxide surfaces using atomic layer deposition.

    Science.gov (United States)

    Hanson, Kenneth; Losego, Mark D; Kalanyan, Berç; Parsons, Gregory N; Meyer, Thomas J

    2013-10-09

    Device lifetimes and commercial viability of dye-sensitized solar cells (DSSCs) and dye-sensitized photoelectrosynthesis cells (DSPECs) are dependent on the stability of the surface bound molecular chromophores and catalysts. Maintaining the integrity of the solution-metal oxide interface is especially challenging in DSPECs for water oxidation where it is necessary to perform high numbers of turnovers, under irradiation in an aqueous environment. In this study, we describe the atomic layer deposition (ALD) of TiO2 on nanocrystalline TiO2 prefunctionalized with the dye molecule [Ru(bpy)2(4,4'-(PO3H2)bpy)](2+) (RuP) as a strategy to stabilize surface bound molecules. The resulting films are over an order of magnitude more photostable than untreated films and the desorption rate constant exponentially decreases with increased thickness of ALD TiO2 overlayers. However, the injection yield for TiO2-RuP with ALD TiO2 also decreases with increasing overlayer thickness. The combination of decreased injection yield and 95% quenched emission suggests that the ALD TiO2 overlayer acts as a competitive electron acceptor from RuP*, effectively nonproductively quenching the excited state. The ALD TiO2 also increases back electron transfer rates, relative to the untreated film, but is independent of overlayer thickness. The results for TiO2-RuP with an ALD TiO2 overlayer are compared with similar films having ALD Al2O3 overlayers.

  12. Combining confocal and atomic force microscopy to quantify single-virus binding to mammalian cell surfaces.

    Science.gov (United States)

    Newton, Richard; Delguste, Martin; Koehler, Melanie; Dumitru, Andra C; Laskowski, Pawel R; Müller, Daniel J; Alsteens, David

    2017-11-01

    Over the past five years, atomic force microscopy (AFM)-based approaches have evolved into a powerful multiparametric tool set capable of imaging the surfaces of biological samples ranging from single receptors to membranes and tissues. One of these approaches, force-distance curve-based AFM (FD-based AFM), uses a probing tip functionalized with a ligand to image living cells at high-resolution and simultaneously localize and characterize specific ligand-receptor binding events. Analyzing data from FD-based AFM experiments using appropriate probabilistic models allows quantification of the kinetic and thermodynamic parameters that describe the free-energy landscape of the ligand-receptor bond. We have recently developed an FD-based AFM approach to quantify the binding events of single enveloped viruses to surface receptors of living animal cells while simultaneously observing them by fluorescence microscopy. This approach has provided insights into the early stages of the interaction between a virus and a cell. Applied to a model virus, we probed the specific interaction with cells expressing viral cognate receptors and measured the affinity of the interaction. Furthermore, we observed that the virus rapidly established specific multivalent interactions and found that each bond formed in sequence strengthened the attachment of the virus to the cell. Here we describe detailed procedures for probing the specific interactions of viruses with living cells; these procedures cover tip preparation, cell sample preparation, step-by-step FD-based AFM imaging and data analysis. Experienced microscopists should be able to master the entire set of protocols in 1 month.

  13. Controllable surfaces of path interference in the multiphoton ionization of atoms by a weak trichromatic field

    Energy Technology Data Exchange (ETDEWEB)

    Mercouris, Theodoros [Theoretical and Physical Chemistry Institute, National Hellenic Research Foundation, 48 Vasileos Constantinou Avenue, Athens 11635 (Greece); Nicolaides, Cleanthes A [Theoretical and Physical Chemistry Institute, National Hellenic Research Foundation, 48 Vasileos Constantinou Avenue, Athens 11635 (Greece)

    2005-10-01

    Multiphoton detachment rates for the H{sup -} {sup 1}S ground state irradiated by a weak trichromatic ac field consisting of the fundamental frequency {omega} 0.272 eV and its second, third or fourth higher harmonics were computed from first principles. The weak intensities are in the range of 10{sup 7}-10{sup 8} W cm{sup -2}. The calculations incorporated systematically electronic structure and electron correlation effects. They were done by implementing a time-independent, nonperturbative many-electron, many-photon theory (MEMPT) which obtains cycle-averaged complex eigenvalues, whose real part gives the field-induced energy shift, {delta}, and the imaginary part is the multiphoton ionization rate, {gamma}. Through analysis, plausible arguments and computation, we show that when the intensities are weak the dependence of {gamma} on phase differences is simple. Specifically, {gamma}s are depicted in the form of plane surfaces, with minor ripples due to higher order ionization paths, in terms of trigonometric functions of the phase differences. This dependence is likely to be applicable to other atomic systems as well, and to provide a definition of the weak field regime in the trichromatic case. When the field intensities are such that higher order ionization paths become important, these dependences break down and we reach the strong field regime.

  14. MDM2-MDM4 molecular interaction investigated by atomic force spectroscopy and surface plasmon resonance.

    Science.gov (United States)

    Moscetti, Ilaria; Teveroni, Emanuela; Moretti, Fabiola; Bizzarri, Anna Rita; Cannistraro, Salvatore

    Murine double minute 2 (MDM2) and 4 (MDM4) are known as the main negative regulators of p53, a tumor suppressor. They are able to form heterodimers that are much more effective in the downregulation of p53. Therefore, the MDM2-MDM4 complex could be a target for promising therapeutic restoration of p53 function. To this aim, a deeper understanding of the molecular mechanisms underlining the heterodimerization is needed. The kinetic and thermodynamic characterization of the MDM2-MDM4 complex was performed with two complementary approaches: atomic force spectroscopy and surface plasmon resonance. Both techniques revealed an equilibrium dissociation constant (KD ) in the micromolar range for the MDM2-MDM4 heterodimer, similar to related complexes involved in the p53 network. Furthermore, the MDM2-MDM4 complex is characterized by a relatively high free energy, through a single energy barrier, and by a lifetime in the order of tens of seconds. New insights into the MDM2-MDM4 interaction could be highly important for developing innovative anticancer drugs focused on p53 reactivation.

  15. Spin moments, orbital moments and magnetic anisotropy of finite-length Co wires deposited on Pd(110)

    International Nuclear Information System (INIS)

    Felix-Medina, R; Dorantes-Davila, J; Pastor, G M

    2002-01-01

    The ground-state spin moments (S z ), orbital moments (L z ) and magnetic anisotropy energy (MAE) of Co N one-dimensional (1D) clusters (N≤12) deposited on the Pd(110) surface are determined in the framework of a self-consistent, real-space tight-binding method. Remarkably large total magnetic moments per Co atom, M z =(2(S z )+(L z ))/N=2.8-2.9 μ B , are obtained, which can be understood as the result of three physically distinct effects. The first and leading contribution is given by the local spin moments (S iz ) at the Co atoms i=1, N (2(S iz ) Co ≅1.6 μ B ). Second, significant spin moments are induced at the Pd atoms i > N close to the Co-Pd interface, which amount to about 25% of M z (2(S iz ) Pd =0.2-0.3 μ B ). Finally, enhanced orbital magnetic moments (L iz ) are responsible for approximately 20% of M z . In the case of the Co atoms, (L iz ) Co =0.28-0.33 μ B is almost a factor of three larger than the Co bulk orbital moment, while in Pd atoms (L iz ) Pd =0.05 μ B represents about 15% of the total local moment μ iz =2(S iz )+(L iz ). These results and the associated MAEs are analysed from a local perspective. The role of the cluster-surface interactions is discussed by comparison with the corresponding results for free-standing wires. Particularly in the case of monatomic 1D Co chains we observe that the lowest-energy magnetization direction (easy axis) changes from in line to off plane upon deposition on Pd(110). Wire-substrate hybridizations are therefore crucial for the magneto-anisotropic behaviour of 1D magnetic nanostructures on metallic substrates

  16. Atom and Amine Adsorption on Flat and Stepped Gold Surfaces & Structure, Stability and Spin Ordering in Manganese Sulfide Clusters

    Science.gov (United States)

    Lewoczko, April D.

    In part I, we investigate gold catalysis in the chemistry of organonitrogen compounds. We examine the adsorption of oxygen, nitrogen and sulfur atoms on the gold (111), (100) and (211) surfaces using density functional theory (DFT). Sulfur atoms bind most strongly, followed by oxygen and nitrogen atoms with stronger adsorption for greater coordination to the surface. We see a trend of stronger adsorption to undercoordinated gold, but find it is non-universal with the adsorption strength trend: (111) > (211) > (100). We consider the diffusion of oxygen, nitrogen and sulfur adatoms and find facile long-range diffusion of oxygen atoms on the (100) surface. Lastly, we compare the adsorption of methylamine on gold to that of a selection of alkylamines, methanol and methanethiol. In each case, the ontop site is preferred with stronger adsorption at low coordinated gold. At oxygen atom coverages of 0.125 -- 0.25 ML on Au (111), we find cooperative adsorption of methylamine and oxygen atoms. Energetic costs for adsorbate tilt from the surface normal and rotation about the gold-nitrogen bond are calculated. While methylamine rotation is barrierless on the (111) and (211) surfaces, it has a low energetic barrier for the 0.125 ML and 0.25 ML O atom pre-covered Au (111) surfaces. In part II, we interpret the experimental mass spectrum of small gas phase manganese sulfide clusters using DFT and elucidate the role of ionicity and spin ordering in sizes with special stability, i.e. magic clusters. We first consider nine low lying minima (MnS)6 structures and reveal antiferromagnetic (AFM) spin ordering with a ˜0.1 eV/pair AFM energy benefit and a ˜0.1 A shrinkage of average Mn-Mn distances over clusters with ferromagnetic (FM) spin ordering. We calculate energetic barriers for interconversion between the two lowest lying (MnS)6 isomers and predict an elevated cluster melting temperature due to increased configurational entropy in a pre-melted state. Second, we demonstrate the

  17. Observation of core-level binding energy shifts between (100) surface and bulk atoms of epitaxial CuInSe{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Nelson, A.J. [Colorado School of Mines, Golden, CO (United States); Berry, G.; Rockett, A. [Univ. of Illinois, Urbana-Champaign, IL (United States)] [and others

    1997-04-01

    Core-level and valence band photoemission from semiconductors has been shown to exhibit binding energy differences between surface atoms and bulk atoms, thus allowing one to unambiguously distinguish between the two atomic positions. Quite clearly, surface atoms experience a potential different from the bulk due to the lower coordination number - a characteristic feature of any surface is the incomplete atomic coordination. Theoretical accounts of this phenomena are well documented in the literature for III-V and II-VI semiconductors. However, surface state energies corresponding to the equilibrium geometry of (100) and (111) surfaces of Cu-based ternary chalcopyrite semiconductors have not been calculated or experimental determined. These compounds are generating great interest for optoelectronic and photovoltaic applications, and are an isoelectronic analog of the II-VI binary compound semiconductors. Surface core-level binding energy shifts depend on the surface cohesive energies, and surface cohesive energies are related to surface structure. For ternary compound semiconductor surfaces, such as CuInSe{sub 2}, one has the possibility of variations in surface stoichiometry. Applying standard thermodynamical calculations which consider the number of individual surface atoms and their respective chemical potentials should allow one to qualitatively determine the magnitude of surface core-level shifts and, consequently, surface state energies.

  18. First-principles study of the adsorption properties of atoms and molecules on UN2 (001) surface

    Science.gov (United States)

    Xu, Mengjuan; Liu, Guangdong; Ao, Bingyun; Chen, Piheng; Hu, Wangyu; Deng, Huiqiu

    2017-09-01

    Uranium nitrides are one kind of accident-tolerant fuels and have been paid more attention recently. With the first-principles Density-Functional Theory (DFT) calculations, the adsorptions properties of some typical atoms, molecules and radical (including O, H, H2, O2, H2O and OH) adsorbed on the UN2 (001) surface have been studied in the present work. The preferred sites and stable configurations for those adsorbates on the UN2 (001) surface have been obtained. It's found that O or H atom prefers to be adsorbed at the bridge site; O2 adsorption will dissociate into two O atoms and occupy the nearest neighbor bridge sites; the interaction between H2 molecule and the UN2 (001) surface is very weak; OH prefers to occupy the bridge site with its O-H bond vertical to the surface; the surface adsorption of H2O is non-dissociated and adsorption energies are dependent on the initial structures and adsorption modes.

  19. Ejection of fast recoil atoms from solids under ion bombardment (medium-energy ion scattering by solid surfaces: Pt. 3)

    International Nuclear Information System (INIS)

    Dodonoy, A.I.; Mashkova, E.S.; Molchanov, V.A.

    1989-01-01

    This paper is the third part of our review surface scattering. Part I, which was devoted to the scattering of ions by the surfaces of disordered solids, was published in 1972; Part II, concerning scattering by crystal surfaces, was published in 1974. Since the publication of these reviews the material contained in them has become obsolete in many respects. A more recent account of the status of the problem has been given in a number of studies, including the book by E.S. Mashkova and V.A. Molchanov, Medium-Energy Ion Scattering by Solid Surfaces (Atomizdat, Moscow, 1980), than extended version of which was published by North-Holland in 1985. We note, however, that at the time these reviews were written the study of fast recoil atoms had not been carried out systematically; the problem was studied only as a by-product of surface scattering and sputtering. For this reason, in the above-mentioned works and in other reviews the data relating to recoil atoms were considered only occasionally. In recent years there have appeared a number of works - theoretical, experimental and computer -specially devoted to the study of the ejection of recoil atoms under ion bombardment. A number of interesting effects, which are due to the crystal structure of the target, have been discovered. It therefore, appeared desirable to us to systematize the available material and to present it as Part III of our continuing review. (author)

  20. Model polymer etching and surface modification by a time modulated RF plasma jet: role of atomic oxygen and water vapor

    International Nuclear Information System (INIS)

    Luan, P; Knoll, A J; Wang, H; Oehrlein, G S; Kondeti, V S S K; Bruggeman, P J

    2017-01-01

    The surface interaction of a well-characterized time modulated radio frequency (RF) plasma jet with polystyrene, poly(methyl methacrylate) and poly(vinyl alcohol) as model polymers is investigated. The RF plasma jet shows fast polymer etching but mild chemical modification with a characteristic carbonate ester and NO formation on the etched surface. By varying the plasma treatment conditions including feed gas composition, environment gaseous composition, and treatment distance, we find that short lived species, especially atomic O for Ar/1% O 2 and 1% air plasma and OH for Ar/1% H 2 O plasma, play an essential role for polymer etching. For O 2 containing plasma, we find that atomic O initiates polymer etching and the etching depth mirrors the measured decay of O atoms in the gas phase as the nozzle-surface distance increases. The etching reaction probability of an O atom ranging from 10 −4 to 10 −3 is consistent with low pressure plasma research. We also find that adding O 2 and H 2 O simultaneously into Ar feed gas quenches polymer etching compared to adding them separately which suggests the reduction of O and OH density in Ar/O 2 /H 2 O plasma. (letter)

  1. Analytical Model of the Nonlinear Dynamics of Cantilever Tip-Sample Surface Interactions for Various Acoustic-Atomic Force Microscopies

    Science.gov (United States)

    Cantrell, John H., Jr.; Cantrell, Sean A.

    2008-01-01

    A comprehensive analytical model of the interaction of the cantilever tip of the atomic force microscope (AFM) with the sample surface is developed that accounts for the nonlinearity of the tip-surface interaction force. The interaction is modeled as a nonlinear spring coupled at opposite ends to linear springs representing cantilever and sample surface oscillators. The model leads to a pair of coupled nonlinear differential equations that are solved analytically using a standard iteration procedure. Solutions are obtained for the phase and amplitude signals generated by various acoustic-atomic force microscope (A-AFM) techniques including force modulation microscopy, atomic force acoustic microscopy, ultrasonic force microscopy, heterodyne force microscopy, resonant difference-frequency atomic force ultrasonic microscopy (RDF-AFUM), and the commonly used intermittent contact mode (TappingMode) generally available on AFMs. The solutions are used to obtain a quantitative measure of image contrast resulting from variations in the Young modulus of the sample for the amplitude and phase images generated by the A-AFM techniques. Application of the model to RDF-AFUM and intermittent soft contact phase images of LaRC-cp2 polyimide polymer is discussed. The model predicts variations in the Young modulus of the material of 24 percent from the RDF-AFUM image and 18 percent from the intermittent soft contact image. Both predictions are in good agreement with the literature value of 21 percent obtained from independent, macroscopic measurements of sheet polymer material.

  2. Mapping of Proteomic Composition on the Surfaces of Bacillus spores by Atomic Force Microscopy-based Immunolabeling

    Energy Technology Data Exchange (ETDEWEB)

    Plomp, M; Malkin, A J

    2008-06-02

    Atomic force microscopy provides a unique capability to image high-resolution architecture and structural dynamics of pathogens (e.g. viruses, bacteria and bacterial spores) at near molecular resolution in native conditions. Further development of atomic force microscopy in order to enable the correlation of pathogen protein surface structures with specific gene products is essential to understand the mechanisms of the pathogen life cycle. We have applied an AFM-based immunolabeling technique for the proteomic mapping of macromolecular structures through the visualization of the binding of antibodies, conjugated with nanogold particles, to specific epitopes on Bacillus spore surfaces. This information is generated while simultaneously acquiring the surface morphology of the pathogen. The immunospecificity of this labeling method was established through the utilization of specific polyclonal and monoclonal antibodies that target spore coat and exosporium epitopes of Bacillus atrophaeus and Bacillus anthracis spores.

  3. Revisiting magnetism of capped Au and ZnO nanoparticles: Surface band structure and atomic orbital with giant magnetic moment

    Energy Technology Data Exchange (ETDEWEB)

    Hernando, Antonio; Crespo, Patricia [Instituto de Magnetismo Aplicado, UCM-CSIC-ADIF, Las Rozas. P.O. Box 155, 28230 Madrid (Spain); Dept. Fisica de Materiales, Universidad Complutense, Madrid (Spain); Garcia, Miguel Angel [Instituto de Ceramica y Vidrio, CSIC, C/ Kelsen, 5, Madrid 28049 (Spain); Coey, Michael [Trinity College Dublin, Dublin (Ireland); Ayuela, Andres; Echenique, Pedro Miguel [Centro de Fisica de Materiales, CFM-MPC CSIC-UPV/EHU, Donostia International Physics Center (DIPC), 20018 San Sebastian (Spain); Departamento de Fisica de Materiales, Fac. de Quimicas, Universidad del Pais Vasco UPV-EHU, 20018 San Sebastian (Spain)

    2011-10-15

    In this article we review the exotic magnetism of nanoparticles (NPs) formed by substances that are not magnetic in bulk as described with generality in Section 1. In particular, the intrinsic character of the magnetism observed on capped Au and ZnO NPs is analysed. X-ray magnetic circular dichroism (XMCD) analysis has shown that the magnetic moments are intrinsic and lie in the Au and Zn atoms, respectively, as analysed in Section 2, where the general theoretical ideas are also revisited. Since impurity atoms bonded to the surface act as donor or acceptor of electrons that occupy the surface states, the anomalous magnetic response is analysed in terms of the surface band in Section 3. Finally, Section 4 summarizes our last theoretical proposal. (Copyright copyright 2011 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  4. Atomic structure of a stable high-index Ge surface: G2(103)-(4x1)

    DEFF Research Database (Denmark)

    Seehofer, L.; Bunk, O.; Falkenberg, G.

    1997-01-01

    Based on scanning tunneling microscopy and surface X-ray diffraction, we propose a complex structural model for the Ge(103)-(4 x 1) reconstruction. Each unit cell contains two (103) double steps, which gives rise to the formation of stripes of Ge atoms oriented in the [] direction....... The stripes and the spaces between them are covered with threefold-coordinated Ge adatoms. Charge is transferred from the bulk-like edge atoms of the double steps to the adatoms. The formation of the reconstruction can be explained in terms of stress relief, charge transfer, and minimization of the dangling...

  5. Surface modification of thermoplastic poly(vinyl alcohol)/saponite nanocomposites via surface-initiated atom transfer radical polymerization enhanced by air dielectric discharges barrier plasma treatment

    International Nuclear Information System (INIS)

    Zhen Weijun; Lu Canhui

    2012-01-01

    To improve the water resistance of thermoplastic poly(vinyl alcohol)/saponite nanocomposites (TPVA), a simple two-step method was developed for the covalent immobilization of atom transfer radical polymerization (ATRP) initiators on the TPVA surfaces enhanced by air dielectric barrier discharges (DBD) plasma treatment, and hydrophobic poly(methyl methacrylate) (PMMA) brushes were then grafted onto the surface of TPVA via surface-initiated atom transfer radical polymerization (SI-ATRP). The chemical composition, morphology and hydrophobicity of the modified TPVA surfaces were characterized by X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM), respectively. The water resistance of the surface-functionalized PMMA was evaluated by the contact angle and water adsorption method. It was shown that air DBD plasma treatment activated the TPVA surface and accelerated the immobilization of ATRP initiator on the TPVA surface. Compared with TPVA control, TPVA modified by SI-ATRP can be grafted well-defined and covalently tethered network PMMA brushes onto the surface and the hydrophobicity of TPVA were significantly enhanced.

  6. Short-range surface plasmonics: Localized electron emission dynamics from a 60-nm spot on an atomically flat single-crystalline gold surface.

    Science.gov (United States)

    Frank, Bettina; Kahl, Philip; Podbiel, Daniel; Spektor, Grisha; Orenstein, Meir; Fu, Liwei; Weiss, Thomas; Horn-von Hoegen, Michael; Davis, Timothy J; Meyer Zu Heringdorf, Frank-J; Giessen, Harald

    2017-07-01

    We experimentally and theoretically visualize the propagation of short-range surface plasmon polaritons using atomically flat single-crystalline gold platelets on silicon substrates. We study their excitation and subfemtosecond dynamics via normal-incidence two-photon photoemission electron microscopy. By milling a plasmonic disk and grating structure into a single-crystalline gold platelet, we observe nanofocusing of the short-range surface plasmon polariton. Localized two-photon ultrafast electron emission from a spot with a smallest dimension of 60 nm is observed. Our novel approach opens the door toward reproducible plasmonic nanofocusing devices, which do not degrade upon high light intensity or heating due to the atomically flat surface without any tips, protrusions, or holes. Our nanofoci could also be used as local emitters for ultrafast electron bunches in time-resolved electron microscopes.

  7. Unusual Activity Trend for CO Oxidation on Pd(x)Au(140-x)@Pt Core@Shell Nanoparticle Electrocatalysts.

    Science.gov (United States)

    Luo, Long; Zhang, Liang; Henkelman, Graeme; Crooks, Richard M

    2015-07-02

    A theoretical and experimental study of the electrocatalytic oxidation of CO on PdxAu140-x@Pt dendrimer-encapsulated nanoparticle (DEN) catalysts is presented. These nanoparticles are comprised of a core having an average of 140 atoms and a Pt monolayer shell. The CO oxidation activity trend exhibits an unusual koppa shape as the number of Pd atoms in the core is varied from 0 to 140. Calculations based on density functional theory suggest that the koppa-shaped trend is driven primarily by structural changes that affect the CO binding energy on the surface. Specifically, a pure Au core leads to deformation of the Pt shell and a compression of the Pt lattice. In contrast, Pd, from the pure Pd cores, tends to segregate on the DEN surface, forming an inverted configuration having Pt within the core and Pd in the shell. With a small addition of Au, however, the alloy PdAu cores stabilize the core@shell structures by preventing Au and Pd from escaping to the particle surface.

  8. Local triboelectrification of an n-GaAs surface using the tip of an atomic-force microscope

    Energy Technology Data Exchange (ETDEWEB)

    Brunkov, P. N., E-mail: brunkov@mail.ioffe.ru; Goncharov, V. V.; Rudinsky, M. E.; Gutkin, A. A.; Gordeev, N. Yu.; Lantratov, V. M.; Kalyuzhnyy, N. A.; Mintairov, S. A.; Sokolov, R. V.; Konnikov, S. G. [Russian Academy of Sciences, Ioffe Physical-Technical Institute (Russian Federation)

    2013-09-15

    The method of scanning Kelvin-probe microscopy is used to show that the effect of triboelectrification is observed when the tip of an atomic-force microscope interacts with the surface of n-GaAs epitaxial layers. The sign of the change in the potential indicates that the sample surface after triboelectrification becomes more negative. The observed specific features of the phenomena can be attributed to the thermally activated generation of point defects in the vicinity of the sample surface due to deformation caused by the tip.

  9. The hydrophilic-to-hydrophobic transition in glassy silica is driven by the atomic topology of its surface

    Science.gov (United States)

    Yu, Yingtian; Krishnan, N. M. Anoop; Smedskjaer, Morten M.; Sant, Gaurav; Bauchy, Mathieu

    2018-02-01

    The surface reactivity and hydrophilicity of silicate materials are key properties for various industrial applications. However, the structural origin of their affinity for water remains unclear. Here, based on reactive molecular dynamics simulations of a series of artificial glassy silica surfaces annealed at various temperatures and subsequently exposed to water, we show that silica exhibits a hydrophilic-to-hydrophobic transition driven by its silanol surface density. By applying topological constraint theory, we show that the surface reactivity and hydrophilic/hydrophobic character of silica are controlled by the atomic topology of its surface. This suggests that novel silicate materials with tailored reactivity and hydrophilicity could be developed through the topological nanoengineering of their surface.

  10. Epitaxial ferromagnetic Fe3Si on GaAs(111)A with atomically smooth surface and interface

    International Nuclear Information System (INIS)

    Liu, Y. C.; Hung, H. Y.; Kwo, J.; Chen, Y. W.; Lin, Y. H.; Cheng, C. K.; Hong, M.; Tseng, S. C.; Hsu, C. H.; Chang, M. T.; Lo, S. C.

    2015-01-01

    Single crystal ferromagnetic Fe 3 Si(111) films were grown epitaxially on GaAs(111)A by molecular beam epitaxy. These hetero-structures possess extremely low surface roughness of 1.3 Å and interfacial roughness of 1.9 Å, measured by in-situ scanning tunneling microscope and X-ray reflectivity analyses, respectively, showing superior film quality, comparing to those attained on GaAs(001) in previous publications. The atomically smooth interface was revealed by the atomic-resolution Z (atomic number)-contrast scanning transmission electron microscopy (STEM) images using the correction of spherical aberration (Cs)-corrected electron probe. Excellent crystallinity and perfect lattice match were both confirmed by high resolution x-ray diffraction. Measurements of magnetic property for the Fe 3 Si/GaAs(111) yielded a saturation moment of 990 emu/cm 3 with a small coercive field ≤1 Oe at room temperature

  11. Intimately coupled hybrid of graphitic carbon nitride nanoflakelets with reduced graphene oxide for supporting Pd nanoparticles: A stable nanocatalyst with high catalytic activity towards formic acid and methanol electrooxidation

    International Nuclear Information System (INIS)

    Zhang, Wenyao; Yao, Qiushi; Wu, Xiaodong; Fu, Yongsheng; Deng, Kaiming; Wang, Xin

    2016-01-01

    Highlights: • Intimately coupled hybrid of g-C 3 N 4 nanoflakelets with rGO is fabricated via an in situ chemical synthesis approach. • The detailed forming process of CNNF-G composite is carefully investigated. • The Pd-CNNF-G composite exhibits exceptional catalytic activity and durability. • The real fuel cells have been assembled to evaluate the performance of the electrocatalysts. • The effects of g-C 3 N 4 nanoflakelets on Pd atom were investigated by DFT computations. - Abstract: A novel nitrogen-rich support material (CNNF-G) consisting of graphitic carbon nitride (g-C 3 N 4 ) nanoflakelets (CNNF) and reduced graphene oxide (rGO) is designed and fabricated for loading Pd nanoparticles. Structural characterizations indicates that the CNNF is formed via splitting decomposition of the g-C 3 N 4 polymer on rGO at higher temperatures and the resulting CNNF is intimately coupled to the rGO sheets. The CNNF can provide more exposed edge sites and active nitrogen species for the high dispersion of Pd NPs. It is found that the Pd NPs with an average diameter of 3.92 nm are uniformly dispersed on CNNF-G sheets. DFT computations reveal that CNNF can trap Pd adatom and thus act as a Pd nucleation site at which Pd atoms tend to accumulate to form Pd clusters. The Pd-CNNF-G nanocatalyst exhibits excellent electrocatalytic activity for both formic acid and methanol oxidation reactions, including large electrochemically active surface area (ECSA) values, significantly high forward peak current densities, and reliable stability and durability, far outperforming the Pd-graphene, commercial activated carbon-supported Pd catalyst or Pd-carbon nanotubes. Such a stable Pd/CNNF-G nanocatalyst may bring new design opportunities for high-performance direct formic acid fuel cell (DFAFC) and direct methanol fuel cell (DMFC) in the future.

  12. H2 INTERACTION WITH BIMETALLIC DIMERS SUPPORTED ON THE MgO(100) SURFACE: A DFT CLUSTER MODEL STUDY

    OpenAIRE

    PIOTR MATCZAK

    2012-01-01

    The interaction between the H2 molecule and the PdAg, PdAu, PtAg and PtAu bimetallic dimers deposited on the MgO(100) surface is investigated using density functional theory (DFT). The bimetallic dimers, whose molecular axes are considered to be perpendicular to the support surface, are adsorbed on top of an oxygen atom. Within this adsorption mode, the dimers prefer the orientation in which their Pd or Pt end is closer to the oxygen atom. The Ag and Au ends of the MgO-supported dimers captur...

  13. Synthesis of Environmentally Responsive Polymers by Atom Transfer Radical Polymerization: Generation of Reversible Hydrophilic and Hydrophobic Surfaces

    Directory of Open Access Journals (Sweden)

    Vikas Mittal

    2010-05-01

    Full Text Available Environmentally responsive poly(N-isopropylacrylamide brushes were grafted from the surface of polymer particles or flat surfaces in order to generate reversible hydrophilic and hydrophobic surfaces. The use of atom transfer radical polymerization was demonstrated for the grafting of polymer brushes as it allows efficient control on the amount of grafted polymer. The polymer particles were generated with or without surfactant in the emulsion polymerization and their surface could be modified with the atom transfer