Transmission-lattice based geometric phase analysis for evaluating the dynamic deformation of a liquid surface.

Science.gov (United States)

Shi, Wenxiong; Huang, Xianfu; Liu, Zhanwei

2014-05-05

Quantitatively measuring a dynamic liquid surface often presents a challenge due to high transparency, fluidity and specular reflection. Here, a novel Transmission-Lattice based Geometric Phase Analysis (TLGPA) method is introduced. In this method, a special lattice is placed underneath a liquid to be tested and, when viewed from above, the phase of the transmission-lattice image is modulated by the deformation of the liquid surface. Combining this with multi-directional Newton iteration algorithms, the dynamic deformation field of the liquid surface can be calculated from the phase variation of a series of transmission-lattice images captured at different moments. The developed method has the advantage of strong self-adaption ability to initial lattice rotational errors and this is discussed in detail. Dynamic 3D ripples formation and propagation was investigated and the results obtained demonstrated the feasibility of the method.

Free surface entropic lattice Boltzmann simulations of film condensation on vertical hydrophilic plates

DEFF Research Database (Denmark)

Hygum, Morten Arnfeldt; Karlin, Iliya; Popok, Vladimir

2015-01-01

A model for vapor condensation on vertical hydrophilic surfaces is developed using the entropic lattice Boltzmann method extended with a free surface formulation of the evaporation–condensation problem. The model is validated with the steady liquid film formation on a flat vertical wall. It is sh......A model for vapor condensation on vertical hydrophilic surfaces is developed using the entropic lattice Boltzmann method extended with a free surface formulation of the evaporation–condensation problem. The model is validated with the steady liquid film formation on a flat vertical wall...

Density functional theory study the effects of oxygen-containing functional groups on oxygen molecules and oxygen atoms adsorbed on carbonaceous materials.

Science.gov (United States)

Qi, Xuejun; Song, Wenwu; Shi, Jianwei

2017-01-01

Density functional theory was used to study the effects of different types of oxygen-containing functional groups on the adsorption of oxygen molecules and single active oxygen atoms on carbonaceous materials. During gasification or combustion reactions of carbonaceous materials, oxygen-containing functional groups such as hydroxyl(-OH), carbonyl(-CO), quinone(-O), and carboxyl(-COOH) are often present on the edge of graphite and can affect graphite's chemical properties. When oxygen-containing functional groups appear on a graphite surface, the oxygen molecules are strongly adsorbed onto the surface to form a four-member ring structure. At the same time, the O-O bond is greatly weakened and easily broken. The adsorption energy value indicates that the adsorption of oxygen molecules changes from physisorption to chemisorption for oxygen-containing functional groups on the edge of a graphite surface. In addition, our results indicate that the adsorption energy depends on the type of oxygen-containing functional group. When a single active oxygen atom is adsorbed on the bridge site of graphite, it gives rise to a stable epoxy structure. Epoxy can cause deformation of the graphite lattice due to the transition of graphite from sp2 to sp3 after the addition of an oxygen atom. For quinone group on the edge of graphite, oxygen atoms react with carbon atoms to form the precursor of CO2. Similarly, the single active oxygen atoms of carbonyl groups can interact with edge carbon atoms to form the precursor of CO2. The results show that oxygen-containing functional groups on graphite surfaces enhance the activity of graphite, which promotes adsorption on the graphite surface.

Ab initio lattice dynamics of metal surfaces

International Nuclear Information System (INIS)

Heid, R.; Bohnen, K.-P.

2003-01-01

Dynamical properties of atoms on surfaces depend sensitively on their bonding environment and thus provide valuable insight into the local geometry and chemical binding at the boundary of a solid. Density-functional theory provides a unified approach to the calculation of structural and dynamical properties from first principles. Its high accuracy and predictive power for lattice dynamical properties of semiconductor surfaces has been demonstrated in a previous article by Fritsch and Schroeder (Phys. Rep. 309 (1999) 209). In this report, we review the state-of-the-art of these ab initio approaches to surface dynamical properties of metal surfaces. We give a brief introduction to the conceptual framework with focus on recent advances in computational procedures for the ab initio linear-response approach, which have been a prerequisite for an efficient treatment of surface dynamics of noble and transition metals. The discussed applications to clean and adsorbate-covered surfaces demonstrate the high accuracy and reliability of this approach in predicting detailed microscopic properties of the phonon dynamics for a wide range of metallic surfaces

A determination of the variation in the lattice parameters of Bi2Sr2CaCu2O8+x (Bi-2212) as a function of temperature and oxygen content

International Nuclear Information System (INIS)

Babaei pour, M.; Ross, D.K.

2005-01-01

The variation of the lattice parameters of Bi-2212 has been measured using a high-temperature neutron diffraction technique. The samples have been doped with oxygen at different pressures from 2 to 400 mbar and at different temperatures from room temperature to 750 deg. C. It was found that the lattice parameters of Bi-2212 were dependent on temperature and oxygen content, increasing with temperature but decreasing with oxygen content. The values derived for the thermal expansion coefficient in an oxygen partial pressure of 400 mbar were compared with previous data from powder diffraction measurements at comparable oxygen pressure

Late Archean Surface Ocean Oxygenation (Invited)

Science.gov (United States)

Kendall, B.; Reinhard, C.; Lyons, T. W.; Kaufman, A. J.; Anbar, A. D.

2009-12-01

Oxygenic photosynthesis must have evolved by 2.45-2.32 Ga, when atmospheric oxygen abundances first rose above 0.001% present atmospheric level (Great Oxidation Event; GOE). Biomarker evidence for a time lag between the evolution of cyanobacterial oxygenic photosynthesis and the GOE continues to be debated. Geochemical signatures from sedimentary rocks (redox-sensitive trace metal abundances, sedimentary Fe geochemistry, and S isotopes) represent an alternative tool for tracing the history of Earth surface oxygenation. Integrated high-resolution chemostratigraphic profiles through the 2.5 Ga Mt. McRae Shale (Pilbara Craton, Western Australia) suggest a ‘whiff’ of oxygen in the surface environment at least 50 M.y. prior to the GOE. However, the geochemical data from the Mt. McRae Shale does not uniquely constrain the presence or extent of Late Archean ocean oxygenation. Here, we present high-resolution chemostratigraphic profiles from 2.6-2.5 Ga black shales (upper Campbellrand Subgroup, Kaapvaal Craton, South Africa) that provide the earliest direct evidence for an oxygenated ocean water column. On the slope beneath the Campbellrand - Malmani carbonate platform (Nauga Formation), a mildly oxygenated water column (highly reactive iron to total iron ratios [FeHR/FeT] ≤ 0.4) was underlain by oxidizing sediments (low Re and Mo abundances) or mildly reducing sediments (high Re but low Mo abundances). After drowning of the carbonate platform (Klein Naute Formation), the local bottom waters became anoxic (FeHR/FeT > 0.4) and intermittently sulphidic (pyrite iron to highly reactive iron ratios [FePY/FeHR] > 0.8), conducive to enrichment of both Re and Mo in sediments, followed by anoxic and Fe2+-rich (ferruginous) conditions (high FeT, FePY/FeHR near 0). Widespread surface ocean oxygenation is suggested by Re enrichment in the broadly correlative Klein Naute Formation and Mt. McRae Shale, deposited ~1000 km apart in the Griqualand West and Hamersley basins

Surface interaction of polyimide with oxygen ECR plasma

International Nuclear Information System (INIS)

Naddaf, M.; Balasubramanian, C.; Alegaonkar, P.S.; Bhoraskar, V.N.; Mandle, A.B.; Ganeshan, V.; Bhoraskar, S.V.

2004-01-01

Polyimide (Kapton-H), was subjected to atomic oxygen from an electron cyclotron resonance plasma. An optical emission spectrometer was used to characterize the atomic oxygen produced in the reactor chamber. The energy of the ions was measured using a retarding field analyzer, placed near the substrate. The density of atomic oxygen in the plasma was estimated using a nickel catalytic probe. The surface wettability of the polyimide samples monitored by contact angle measurements showed considerable improvement when treated with plasma. X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopic studies showed that the atomic oxygen in the plasma is the main specie affecting the surface chemistry and adhesion properties of polyimide. The improvement in the surface wettability is attributed to the high degree of cross-linking and large concentration of polar groups generated in the surface region of polyimide, after plasma treatment. The changes in the surface region of polyimide were observed by atomic force microscopic analysis

Surface interaction of polyimide with oxygen ECR plasma

Science.gov (United States)

Naddaf, M.; Balasubramanian, C.; Alegaonkar, P. S.; Bhoraskar, V. N.; Mandle, A. B.; Ganeshan, V.; Bhoraskar, S. V.

2004-07-01

Polyimide (Kapton-H), was subjected to atomic oxygen from an electron cyclotron resonance plasma. An optical emission spectrometer was used to characterize the atomic oxygen produced in the reactor chamber. The energy of the ions was measured using a retarding field analyzer, placed near the substrate. The density of atomic oxygen in the plasma was estimated using a nickel catalytic probe. The surface wettability of the polyimide samples monitored by contact angle measurements showed considerable improvement when treated with plasma. X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopic studies showed that the atomic oxygen in the plasma is the main specie affecting the surface chemistry and adhesion properties of polyimide. The improvement in the surface wettability is attributed to the high degree of cross-linking and large concentration of polar groups generated in the surface region of polyimide, after plasma treatment. The changes in the surface region of polyimide were observed by atomic force microscopic analysis.

Surface-assisted DNA self-assembly: An enzyme-free strategy towards formation of branched DNA lattice

International Nuclear Information System (INIS)

Bhanjadeo, Madhabi M.; Nayak, Ashok K.; Subudhi, Umakanta

2017-01-01

DNA based self-assembled nanostructures and DNA origami has proven useful for organizing nanomaterials with firm precision. However, for advanced applications like nanoelectronics and photonics, large-scale organization of self-assembled branched DNA (bDNA) into periodic lattices is desired. In this communication for the first time we report a facile method of self-assembly of Y-shaped bDNA nanostructures on the cationic surface of Aluminum (Al) foil to prepare periodic two dimensional (2D) bDNA lattice. Particularly those Y-shaped bDNA structures having smaller overhangs and unable to self-assemble in solution, they are easily assembled on the surface of Al foil in the absence of ligase. Field emission scanning electron microscopy (FESEM) analysis shows homogenous distribution of two-dimensional bDNA lattices across the Al foil. When the assembled bDNA structures were recovered from the Al foil and electrophoresed in nPAGE only higher order polymeric bDNA structures were observed without a trace of monomeric structures which confirms the stability and high yield of the bDNA lattices. Therefore, this enzyme-free economic and efficient strategy for developing bDNA lattices can be utilized in assembling various nanomaterials for functional molecular components towards development of DNA based self-assembled nanodevices. - Highlights: • Al foil surface-assisted self-assembly of monomeric structures into larger branched DNA lattice. • FESEM study confirms the uniform distribution of two-dimensional bDNA lattice structures across the surface of Al foil. • Enzyme-free and economic strategy to prepare higher order structures from simpler DNA nanostructures have been confirmed by recovery assay. • Use of well proven sequences for the preparation of pure Y-shaped monomeric DNA nanostructure with high yield.

Dislocation behavior of surface-oxygen-concentration controlled Si wafers

International Nuclear Information System (INIS)

Asazu, Hirotada; Takeuchi, Shotaro; Sannai, Hiroya; Sudo, Haruo; Araki, Koji; Nakamura, Yoshiaki; Izunome, Koji; Sakai, Akira

2014-01-01

We have investigated dislocation behavior in the surface area of surface-oxygen-concentration controlled Si wafers treated by a high temperature rapid thermal oxidation (HT-RTO). The HT-RTO process allows us to precisely control the interstitial oxygen concentration ([O i ]) in the surface area of the Si wafers. Sizes of rosette patterns, generated by nano-indentation and subsequent thermal annealing at 900 °C for 1 h, were measured for the Si wafers with various [O i ]. It was found that the rosette size decreases in proportion to the − 0.25 power of [O i ] in the surface area of the Si wafers, which were higher than [O i ] of 1 × 10 17 atoms/cm 3 . On the other hand, [O i ] of lower than 1 × 10 17 atoms/cm 3 did not affect the rosette size very much. These experimental results demonstrate the ability of the HT-RTO process to suppress the dislocation movements in the surface area of the Si wafer. - Highlights: • Surface-oxygen-concentration controlled Si wafers have been made. • The oxygen concentration was controlled by high temperature rapid thermal oxidation. • Dislocation behavior in the surface area of the Si wafers has been investigated. • Rosette size decreased with increasing of interstitial oxygen atoms. • The interstitial oxygen atoms have a pinning effect of dislocations at the surface

Oxygen ordering in Nb(1 1 0) films

International Nuclear Information System (INIS)

Hellwig, O.; Zabel, H.

2003-01-01

Synchrotron X-ray diffraction (XRD) during the atmospheric oxidation of epitaxial Nb(1 1 0) films at elevated temperature reveals the formation of highly ordered oxygen phases within the Nb lattice. The oxygen is stored on interstitial lattice sites without destroying the basic BCC structure of the Nb host lattice. However the lattice exhibits an out-of-plane lattice expansion of up to 4.3%. During oxidation we observe the formation of a non-ordered lattice gas phase succeeded by a well-defined sequence of oxygen superstructures until finally the whole film is consumed by the formation of amorphous Nb 2 O 5 . We show that XRD is an excellent tool to monitor the exact evolution of the different oxygen phases. In addition we demonstrate that UHV post-annealing of partially oxidized films can be used to rearrange the oxygen within the sample while keeping the overall amount of oxygen constant

Microstructural and surface modifications and hydroxyapatite coating of Ti-6Al-4V triply periodic minimal surface lattices fabricated by selective laser melting.

Science.gov (United States)

Yan, Chunze; Hao, Liang; Hussein, Ahmed; Wei, Qingsong; Shi, Yusheng

2017-06-01

Ti-6Al-4V Gyroid triply periodic minimal surface (TPMS) lattices were manufactured by selective laser melting (SLM). The as-built Ti-6Al-4V lattices exhibit an out-of-equilibrium microstructure with very fine α' martensitic laths. When subjected to the heat treatment of 1050°C for 4h followed by furnace cooling, the lattices show a homogenous and equilibrium lamellar α+β microstructure with less dislocation and crystallographic defects compared with the as-built α' martensite. The as-built lattices present very rough strut surfaces bonded with plenty of partially melted metal particles. The sand blasting nearly removed all the bonded metal particles, but created many tiny cracks. The HCl etching eliminated these tiny cracks, and subsequent NaOH etching resulted in many small and shallow micro-pits and develops a sodium titanate hydrogel layer on the surfaces of the lattices. When soaked in simulated body fluid (SBF), the Ti-6Al-4V TPMS lattices were covered with a compact and homogeneous biomimetic hydroxyapatite (HA) layer. This work proposes a new method for making Ti-6Al-4V TPMS lattices with a homogenous and equilibrium microstructure and biomimetic HA coating, which show both tough and bioactive characteristics and can be promising materials usable as bone substitutes. Copyright © 2017 Elsevier B.V. All rights reserved.

Surface acoustic wave oxygen pressure sensor

Science.gov (United States)

Oglesby, Donald M. (Inventor); Upchurch, Billy T. (Inventor); Leighty, Bradley D. (Inventor)

1994-01-01

A transducer for the measurement of absolute gas-state oxygen pressure from pressures of less than 100 Pa to atmospheric pressure (1.01 x 10(exp 5) Pa) is based on a standard surface acoustic wave (SAW) device. The piezoelectric material of the SAW device is coated with a compound which will selectively and reversibly bind oxygen. When oxygen is bound by the coating, the mass of the coating increases by an amount equal to the mass of the bound oxygen. Such an increase in the mass of the coating causes a corresponding decrease in the resonant frequency of the SAW device.

Simulating condensation on microstructured surfaces using Lattice Boltzmann Method

Science.gov (United States)

Alexeev, Alexander; Vasyliv, Yaroslav

2017-11-01

We simulate a single component fluid condensing on 2D structured surfaces with different wettability. To simulate the two phase fluid, we use the athermal Lattice Boltzmann Method (LBM) driven by a pseudopotential force. The pseudopotential force results in a non-ideal equation of state (EOS) which permits liquid-vapor phase change. To account for thermal effects, the athermal LBM is coupled to a finite volume discretization of the temperature evolution equation obtained using a thermal energy rate balance for the specific internal energy. We use the developed model to probe the effect of surface structure and surface wettability on the condensation rate in order to identify microstructure topographies promoting condensation. Financial support is acknowledged from Kimberly-Clark.

Oxygen adsorption on Pt(110)-(1x2): new high-coverage structures

DEFF Research Database (Denmark)

Helveg, Stig; Lorensen, Henrik Qvist; Horch, Sebastian

1999-01-01

From an interplay between scanning tunneling microscopy (STM) experiments and density functional theory (DFT) calculations, a comprehensive picture is obtained for oxygen adsorption on the Pt(110)-(1 x 2) surface, from single isolated oxygen atoms chemisorbed in FCC sites along the platinum ridges...... adsorption and platinum lattice distortions. (C) 1999 Elsevier Science B.V. All rights reserved....

Thermochemical Properties of the Lattice Oxygen in W,Mn-Containing Mixed Oxide Catalysts for the Oxidative Coupling of Methane

Science.gov (United States)

Lomonosov, V. I.; Gordienko, Yu. A.; Sinev, M. Yu.; Rogov, V. A.; Sadykov, V. A.

2018-03-01

Mixed NaWMn/SiO2 oxide, samples containing individual components (Na, W, Mn) and their double combinations (Na-W, Na-Mn, W-Mn) supported on silica were studied by temperature programmed reduction (TPR) and desorption (TPD), and heat flow calorimetry during their reoxidation with molecular oxygen in pulse mode. The NaWMn/SiO2 mixed oxide was shown to contain two different types of reactive lattice oxygen. The weakly-bonded oxygen can be reversibly released from the oxide in a flow of inert gas in the temperature range of 575‒900°C, while the strongly-bonded oxygen can be removed during the reduction of the sample with hydrogen at 700-900°C. The measured thermal effect of oxygen consumption for these two oxygen forms are 185 and 350 kJ/mol, respectively. The amount of oxygen removed at reduction ( 443 μmol/g) considerably exceeded the amount desorbed in an inert gas flow ( 56 μmol/g). The obtained results suggest that the reversible oxygen desorption is due to the redox process in which manganese ions are involved, while during the temperature programmed reduction, mainly oxygen bonded with tungsten is removed.

Surface representations of Wilson loop expectations in lattice gauge theory

International Nuclear Information System (INIS)

Brydges, D.C.; Giffen, C.; Durhuus, B.; Froehlich, J.

1986-01-01

Expectations of Wilson loops in lattice gauge theory with gauge group G=Z 2 , U(1) or SU(2) are expressed as weighted sums over surfaces with boundary equal to the loops labelling the observables. For G=Z 2 and U(1), the weights are all positive. For G=SU(2), the weights can have either sign depending on the Euler characteristic of the surface. Our surface (or flux sheet-) representations are partial resummations of the strong coupling expansion and provide some qualitative understanding of confinement. The significance of flux sheets with nontrivial topology for permanent confinement in the SU(2)-theory is elucidated. (orig.)

2D surface optical lattice formed by plasmon polaritons with application to nanometer-scale molecular deposition.

Science.gov (United States)

Yin, Yanning; Xu, Supeng; Li, Tao; Yin, Yaling; Xia, Yong; Yin, Jianping

2017-08-10

Surface plasmon polaritons, due to their tight spatial confinement and high local intensity, hold great promises in nanofabrication which is beyond the diffraction limit of conventional lithography. Here, we demonstrate theoretically the 2D surface optical lattices based on the surface plasmon polariton interference field, and the potential application to nanometer-scale molecular deposition. We present the different topologies of lattices generated by simple configurations on the substrate. By explicit theoretical derivations, we explain their formation and characteristics including field distribution, periodicity and phase dependence. We conclude that the topologies can not only possess a high stability, but also be dynamically manipulated via changing the polarization of the excitation laser. Nanometer-scale molecular deposition is simulated with these 2D lattices and discussed for improving the deposition resolution. The periodic lattice point with a width resolution of 33.2 nm can be obtained when the fullerene molecular beam is well-collimated. Our study can offer a superior alternative method to fabricate the spatially complicated 2D nanostructures, with the deposition array pitch serving as a reference standard for accurate and traceable metrology of the SI length standard.

An oxygen pressure sensor using surface acoustic wave devices

Science.gov (United States)

Leighty, Bradley D.; Upchurch, Billy T.; Oglesby, Donald M.

1993-01-01

Surface acoustic wave (SAW) piezoelectric devices are finding widespread applications in many arenas, particularly in the area of chemical sensing. We have developed an oxygen pressure sensor based on coating a SAW device with an oxygen binding agent which can be tailored to provide variable sensitivity. The coating is prepared by dissolving an oxygen binding agent in a toluene solution of a copolymer which is then sprayed onto the surface of the SAW device. Experimental data shows the feasibility of tailoring sensors to measure the partial pressure of oxygen from 2.6 to 67 KPa (20 to 500 torr). Potential applications of this technology are discussed.

Lattice dynamics in solid oxygen

International Nuclear Information System (INIS)

Kobashi, K.; Klein, M.L.; Chandrasekharan, V.

1979-01-01

Lattice dynamical calculations for the bulk α, β, and γ phases of solid O 2 and for the monolayer α and β phases have been made in the harmonic approximation. In the α and β phases, atom-atom 6-12 potentials are employed. In the γ phase, effective potentials are used between molecular centers and only the translational lattice vibrations are calculated. It is found that Laufer and Leroi's potential parameters give two k=O frequencies at 42.7 and 43.6 cm -1 in the bulk α-O 2 , and at 40.7 cm -1 for the degenerate k=0 modes in the β phase. The observed Raman lines for α-O 2 at 43 and 79 cm -1 , which are both known to exhibit isotope shifts, are thus tentatively assigned to an accidentally degenerate line and a two-phonon band, respectively, In view of the possible contribution from anharmonic effects, the agreement of the calculation with experiment (48-51 cm -1 ) in β-O 2 may be better than it seems. For the bulk γ-O 2 , a discrepancy is observed between the calculated elastic constants and those derived from Brillouin scattering experiments. This discrepancy may be due to the neglect of translation-rotation coupling. In the monolayer O 2 , Raman active modes at 28.3 and 40.6 cm -1 for the α phase, and 31.9 cm -1 for the β phase are predicted

Influence of oxygen, nitrogen and carbon on the lattice parameter of uranium mono-carbide; Influence de l'oxygene, de l'azote et du carbone sur le parametre reticulaire du monocarbure d'uranium

Energy Technology Data Exchange (ETDEWEB)

Magnier, P [Commissariat a l' Energie Atomique, Saclay (France). Centre d' Etudes Nucleaires

1966-04-15

The author studies the influence of oxygen and nitrogen contents on the lattice parameter of U(C,O,N) solid solutions around UC composition. The whole data conducts to a determination of the solubility of oxygen in UC: a U(C(1-x)O(x)) solid solution exist if x if smaller than 0.37. The author studies also the influence of carbon content on the lattice parameter of U-UC solid solutions around UC. This study conducts to the determination of the solubility of U in UC at the different temperatures. Consequences upon uranium-carbon diagram are envisaged. (author) [French] L'auteur etudie quantitativement l'influence de l'oxygene et de l'azote sur le parametre reticulaire des solutions solides U(C,O,N) proches de UC. Cette etude permet la determination de la solubilite de l'oxygene dans UC: on montre l'existence d'une solution solide U(C(1-x)O(x)) lorsque x est compris entre 0 et 0,37. Par ailleurs l'auteur etudie l'influence de la teneur en carbone sur le parametre des solutions solides U-UC proches de UC. Cette etude permet la determination de la solubilite de l'uranium dans UC aux differentes temperatures. On envisage enfin les modifications apportees par cette etude au diagramme uranium-carbone. (auteur)

Density functional theory study of oxygen and water adsorption on SrTiO3(001)

International Nuclear Information System (INIS)

Guhl, Hannes

2010-01-01

Strontium titanate is an extensively studied material with a wide range of application, for instance in photo-catalysis and most importantly, it is used as a substrate in growth of functional oxides. The surface chemistry is crucial and hence understanding the surface structure on atomic scale is essential for gaining insight into the fundamental processes in the aforementioned applications. Moreover, there exist a lot of evidence that this surface chemistry might be controlled to considerably by extrinsic species, such as residual hydrogen and water. Investigating the properties of water and oxygen on the strontium titanate surface is certainly a natural starting point for a theoretical study based on density functional theory, because these species are practically present on the surface on a wide range of experimental conditions and they are computationally feasible. For the oxygen and water adsorption the binding energy is controlled by long-range surface relaxations leading to an effective repulsion of the adsorbed specimen. The isolated oxygen ad-atom forms a covalently bonded ''quasi-peroxide anion'' in combination with a lattice oxygen atom. Contrariwise, in all investigated configurations containing water molecules and hydroxyl groups, the respective oxygen atoms assumed positions close to the oxygen sites of the continued perovskite lattice of the substrate. Most remarkably, on the strontium oxide termination, the water molecules adsorbs and dissociates effortlessly leading to the formation of a pair of hydroxyl groups. For the titanium dioxide termination, a coverage dependent adsorption mode is observed. Densely packings stabilize water molecules, whereas at lower coverage and finite temperatures the formation of hydroxyl groups is found. The energetics responsible for this behavior is consistent with recent experiments by Iwahori and coworkers. (orig.)

Micropatterning of bacteria on two-dimensional lattice protein surface observed by atomic force microscopy

International Nuclear Information System (INIS)

Oh, Y.J.; Jo, W.; Lim, J.; Park, S.; Kim, Y.S.; Kim, Y.

2008-01-01

In this study, we characterized the two-dimensional lattice of bovine serum albumin (BSA) as a chemical and physical barrier against bacterial adhesion, using fluorescence microscopy and atomic force microscopy (AFM). The lattice of BSA on glass surface was fabricated by micro-contact printing (μCP), which is a useful way to pattern a wide range of molecules into microscale features on different types of substrates. The contact-mode AFM measurements showed that the average height of the printed BSA monolayer was 5-6 nm. Escherichia coli adhered rapidly on bare glass slide, while the bacterial adhesion was minimized on the lattices in the range of 1-3 μm 2 . Especially, the bacterial adhesion was completely inhibited on a 1 μm 2 lattice. The results suggest that the anti-adhesion effects are due by the steric repulsion forces exerted by BSA

Oxygen dosing the surface of SrTiO{sub 3}

Energy Technology Data Exchange (ETDEWEB)

Dudy, L.; Scheiderer, P.; Schuetz, P.; Gabel, J.; Buchwald, M.; Sing, M.; Claessen, R. [Physikalisches Institut, Universitaet Wuerzburg (Germany); Denlinger, J.D. [Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA, 94270 (United States); Schlueter, C.; Lee, T.L. [Diamond Light Source Ltd., Didcot, Oxfordshire (United Kingdom)

2015-07-01

The highly mobile two-dimensional electron system (2DES) on the surface of the insulating SrTiO{sub 3}(STO) offers exciting perspectives for advanced material design. This 2DES resides in a depletion layer caused by oxygen deficiency of the surface. With photoemission spectroscopy, we monitor the appearance of quasi-particle weight (QP) at the Fermi energy and oxygen vacancy induced states in the band gap (IG). Both, QP and IG weight, increase and decrease respectively upon exposure to extreme ultraviolet (XUV) light and in-situ oxygen dosing. By a proper adjustment of oxygen dosing, any intermediate state can be stabilized providing full control over the charge carrier density. From a comparison of the charge carrier concentrations obtained from an analysis of core-level spectra and the Fermi-surface volume, we conclude on a spatially inhomogeneous surface electronic structure with at least two different phases.

A first-principles study of oxygen adsorption on Ir(111) surface

Energy Technology Data Exchange (ETDEWEB)

Gao, Hengjiao, E-mail: gaohengjiao@163.com; Xiong, Yuqing, E-mail: xiongyq@hotmail.com; Liu, Xiaoli, E-mail: shantianzi@126.com; Zhao, Dongcai, E-mail: zhaodongc@163.com; Feng, Yudong, E-mail: yudong_feng@sina.com; Wang, Lanxi, E-mail: wanglanxi@live.com; Wang, Jinxiao, E-mail: coldwind716@gmail.com

2016-12-15

Highlights: • Adsorption of oxygen on Ir(111) surface was studied by density functional theory. • The most stable adsorption site was determined by adsorption energy calculation. • Adsorption of oxygen at bridge and top site on Ir surface was the most stable ones. • Interaction of O 2p and Ir 5d orbits is relatively strong and formed hybridization. - Abstract: In order to understand deposition mechanism of iridium thin film by atomic layer deposition, the adsorption of oxygen on Ir(111) surface was studied by use of density functional theory and a periodical slab model. By calculating the adsorption energy and structure of oxygen at four adsorption sites (top, bridge, fcc-hollow and hcp-hollow) on Ir(111) surface, the most stable adsorption site was determined. On this basis, the banding mechanism of O and Ir atoms was studied by density of states of oxygen and iridium atoms. Oxygen adsorbed at hcp(parallel) site on Ir(111) surface was the most stable one according to the adsorption energy calculation results. Orbital charge analysis indicate that charge transferred from 5p and 5d orbit to 2p orbit of adsorbed O atoms, and 6s orbit of iridium atoms. Meanwhile, density of state study indicated that adsorption of oxygen on Ir(111) surface is mainly due to the interaction between 2p orbit of O atoms and 5d orbit of iridium atoms.

Origami lattices with free-form surface ornaments

NARCIS (Netherlands)

Janbaz, S.; Noordzij, N.; Widyaratih, Dwisetya Safirna; Hagen, C.W.; Fratila-Apachitei, E.L.; Zadpoor, A.A.

2017-01-01

Lattice structures are used in the design of metamaterials to achieve unusual physical, mechanical, or biological properties. The properties of such metamaterials result from the topology of the lattice structures, which are usually three-dimensionally (3D) printed. To incorporate advanced

The surface morphology of retinal breaks and lattice retinal degeneration. A scanning electron microscopic study.

Science.gov (United States)

Robinson, M R; Streeten, B W

1986-02-01

In 14 of 110 eye bank eyes, lesions characteristic of peripheral retinal surface pathology were examined by scanning electron microscopy (SEM). These included operculated and flap tears, trophic round holes, lattice degeneration with holes, and paravascular retinal "pitting" degeneration. By SEM, the edges of the retinal breaks were covered by smooth cellular membranes, merging peripherally with a meshwork of vitreous fibrils. The membrane cells had poorly defined borders, a pitted surface, and variable numbers of microvilli consistent with glia. Lattice surfaces and foci of paravascular retinal degeneration were covered by similar membrane, but showed characteristic differences. It appears that breaks in the internal limiting membrane always stimulate proliferation of preretinal glial membranes. Similar cellular morphology of the membranes associated with breaks is consistent with a common cell of origin. Limited proliferation of these membranes suggests that surface gliosis is normally inhibited when the cells contact either intact basement membrane or vitreous.

Improved thrombogenicity on oxygen etched Ti6Al4V surfaces

International Nuclear Information System (INIS)

Riedel, Nicholas A.; Smith, Barbara S.; Williams, John D.; Popat, Ketul C.

2012-01-01

Thrombus formation on blood contacting biomaterials continues to be a key factor in initiating a critical mode of failure in implantable devices, requiring immediate attention. In the interest of evaluating a solution for one of the most widely used biomaterials, titanium and its alloys, this study focuses on the use of a novel surface oxidation treatment to improve the blood compatibility. This study examines the possibility of using oblique angle ion etching to produce a high quality oxide layer that enhances blood compatibility on medical grade titanium alloy Ti6Al4V. An X-ray photoelectron spectroscopy (XPS) analysis of these oxygen-rich surfaces confirmed the presence of TiO 2 peaks and also indicated increased surface oxidation as well as a reduction in surface defects. After 2 h of contact with whole human plasma, the oxygen etched substrates demonstrated a reduction in both platelet adhesion and activation as compared to bare titanium substrates. The whole blood clotting behavior was evaluated for up to 45 min, showing a significant decrease in clot formation on oxygen etched substrates. Finally, a bicinchoninic acid (BCA) total protein assay and XPS were used to evaluate the degree of key blood serum protein (fibrinogen, albumin, immunoglobulin G) adsorption on the substrates. The results showed similar protein levels for both the oxygen etched and control substrates. These results indicate that oblique angle oxygen etching may be a promising method to increase the thrombogenicity of Ti6Al4V. - Highlights: ►Oblique angle oxygen ion etching creates a high quality, uniform oxide surface. ►Oxygen etched substrates showed fewer adhered platelets. ►Platelet activation was reduced by the improved oxide surface. ►Oxygen etched substrates exhibited increased whole blood clotting times. ►Although clotting reductions were seen, protein adsorption remained similar.

Surface Wettability of Oxygen Plasma Treated Porous Silicon

Directory of Open Access Journals (Sweden)

Lei Jiang

2014-01-01

Full Text Available Oxygen plasma treatment on porous silicon (p-Si surfaces was studied as a practical and effective means to modify wetting properties of as-fabricated p-Si surfaces, that is, contact angles of the p-Si materials. P-Si samples spanning a wide range of surface nanostructures have been fabricated which were subjected to a series of oxygen plasma treatments. Reduction of the p-Si surface contact angles has been systematically observed, and the surface activation rate constant as a function of different pore geometries has been analyzed to achieve an empirical equation. The underlying diffusion mechanisms have been discussed by taking into account of different pore diameters of p-Si samples. It is envisaged that such an approach as well as the corresponding empirical equation may be used to provide relevant process guidance in order to achieve precise control of p-Si contact angles, which is essential for many p-Si applications especially in biosensor areas.

First principles study of dissolved oxygen water adsorption on Fe (001 surfaces

Directory of Open Access Journals (Sweden)

Dong ZHANG

2018-02-01

Full Text Available In order to study the mechanism of dissolved oxygen content on the surface corrosion behavior of Fe-based heat transfer, the first principle is used to study the adsorption of O2 monomolecular, H2O monolayer and dissolved oxygen system on Fe-based heat transfer surface. The GGA/PBE approximation is used to calculate the adsorption energy, state density and population change during the adsorption process. Calculations prove that when the dissolved oxygen is adsorbed on the Fe-based surface, the water molecule tends to adsorb at the top sites, and the oxygen molecule tends to adsorb at Griffiths. When the H2O molecule adsorbs and interacts on the Fe (001 surface, the charge distribution of the interfacial double electric layer changes to cause the Fe atoms to lose electrons, resulting in the change of the surface potential. When the O2 molecule adsorbs on the Fe (001 crystal surfaces, the electrons on the Fe (001 surface are lost and the surface potential increases. O2 molecule and the surface of the Fe atoms are prone to electron transfer, in which O atom's 2p orbit for the adsorption of O2 molecule on Fe (001 crystal surface play a major role. With the increase of the proportion of O2 molecule in the dissolved oxygen water, the absolute value of the adsorption energy increases, and the interaction of the Fe-based heat transfer surface is stronger. This study explores the influence law of different dissolved oxygen on the Fe base heat exchange surface corrosion, and the base metal corrosion mechanism for experimental study provides a theoretical reference.

Surface Characterization and Electrochemical Oxidation of Metal Doped Uranium Dioxide

Energy Technology Data Exchange (ETDEWEB)

Lee, Jeongmook; Kim, Jandee; Youn, Young-Sang; Kim, Jong-Goo; Ha, Yeong-Keong; Kim, Jong-Yun [Korea Atomic Energy Research Institute, Daejeon (Korea, Republic of)

2016-10-15

Trivalent element in UO{sub 2} matrix makes the oxygen vacancy from loss of oxygen for charge compensation. Tetravalent element alters lattice parameter of UO{sub 2} due to diameter difference between the tetravalent element and replaced U. These structural changes have significant effect on not only relevant fuel performance but also the kinetics of fuel oxidation. Park and Olander explained the stabilization of Ln (III)-doped UO{sub 2} against oxidation based on oxygen potential calculations. In this work, we have been investigated the effect of Gd{sup 3+} and Th{sup 4+} doping on the UO{sub 2} structure with Raman spectroscopy and X-ray diffraction to characterize the surface structure of nuclear fuel material. For Gd doped UO{sub 2}, its electrochemical oxidation behaviors are also investigated. The Gd and Th doped uranium dioxide solid solution pellets with various doping level were investigated by XRD, Raman spectroscopy, SEM, electrochemical experiments to investigate surface structure and electro chemical oxidation behaviors. The lattice parameter evaluated from XRD spectra indicated the formation of solid solutions. Raman spectra showed the existence of the oxygen vacancy. SEM images showed the grain structure on the surface of Gd doped uranium dioxide depending on doping level and oxygen-to-metal ratio.

Surface oxygen vacancy and oxygen permeation flux limits of perovskite ion transport membranes

KAUST Repository

Hunt, Anton

2015-09-01

© 2015 Elsevier B.V. The mechanisms and quantitative models for how oxygen is separated from air using ion transport membranes (ITMs) are not well understood, largely due to the experimental complexity for determining surface exchange reactions at extreme temperatures (>800°C). This is especially true when fuels are present at the permeate surface. For both inert and reactive (fuels) operations, solid-state oxygen surface vacancies (δ) are ultimately responsible for driving the oxygen flux, JO2. In the inert case, the value of δ at either surface is a function of the local PO2 and temperature, whilst the magnitude of δ dictates both the JO2 and the inherent stability of the material. In this study values of δ are presented based on experimental measurements under inert (CO2) sweep: using a permeation flux model and local PO2 measurements, collected by means of a local gas-sampling probe in our large-scale reactor, we can determine δ directly. The ITM assessed was La0.9Ca0.1FeO3-δ (LCF); the relative resistances to JO2 were quantified using the pre-defined permeation flux model and local PO2 values. Across a temperature range from 825°C to 1056°C, δ was found to vary from 0.007 to 0.029 (<1%), safely within material stability limits, whilst the permeate surface exchange resistance dominates. An inert JO2 limit was identified owing to a maximum sweep surface δ, δmaxinert. The physical presence of δmaxinert is attributed to a rate limiting step shift from desorption to associative electron transfer steps on the sweep surface as PO2 is reduced. Permeate surface exchange limitations under non-reactive conditions suggest that reactive (fuel) operation is necessary to accelerate surface chemistry for future work, to reduce flux resistance and push δpast δmaxinert in a stable manner.

Synthesis of Graphite Oxide with Different Surface Oxygen Contents Assisted Microwave Radiation

Directory of Open Access Journals (Sweden)

Adriana Ibarra-Hernández

2018-02-01

Full Text Available Graphite oxide is synthesized via oxidation reaction using oxidant compounds that have lattice defects by the incorporation of unlike functional groups. Herein, we report the synthesis of the graphite oxide with diverse surface oxygen content through three (B, C, D different modified versions of the Hummers method assisted microwave radiation compared with the conventional graphite oxide sample obtained by Hummers method (A. These methods allow not only the production of graphite oxide but also reduced graphene oxide, without undergoing chemical, thermal, or mechanical reduction steps. The values obtained of C/O ratio were ~2, 3.4, and ~8.5 for methodologies C, B, and D, respectively, indicating the presence of graphite oxide and reduced graphene oxide, according to X-ray photoelectron spectroscopy. Raman spectroscopy of method D shows the fewest structural defects compared to the other methodologies. The results obtained suggest that the permanganate ion produces reducing species during graphite oxidation. The generation of these species is attributed to a reversible reaction between the permanganate ion with π electrons, ions, and radicals produced after treatment with microwave radiation.

Density functional theory study of oxygen and water adsorption on SrTiO{sub 3}(001)

Energy Technology Data Exchange (ETDEWEB)

Guhl, Hannes

2010-12-03

Strontium titanate is an extensively studied material with a wide range of application, for instance in photo-catalysis and most importantly, it is used as a substrate in growth of functional oxides. The surface chemistry is crucial and hence understanding the surface structure on atomic scale is essential for gaining insight into the fundamental processes in the aforementioned applications. Moreover, there exist a lot of evidence that this surface chemistry might be controlled to considerably by extrinsic species, such as residual hydrogen and water. Investigating the properties of water and oxygen on the strontium titanate surface is certainly a natural starting point for a theoretical study based on density functional theory, because these species are practically present on the surface on a wide range of experimental conditions and they are computationally feasible. For the oxygen and water adsorption the binding energy is controlled by long-range surface relaxations leading to an effective repulsion of the adsorbed specimen. The isolated oxygen ad-atom forms a covalently bonded ''quasi-peroxide anion'' in combination with a lattice oxygen atom. Contrariwise, in all investigated configurations containing water molecules and hydroxyl groups, the respective oxygen atoms assumed positions close to the oxygen sites of the continued perovskite lattice of the substrate. Most remarkably, on the strontium oxide termination, the water molecules adsorbs and dissociates effortlessly leading to the formation of a pair of hydroxyl groups. For the titanium dioxide termination, a coverage dependent adsorption mode is observed. Densely packings stabilize water molecules, whereas at lower coverage and finite temperatures the formation of hydroxyl groups is found. The energetics responsible for this behavior is consistent with recent experiments by Iwahori and coworkers. (orig.)

Generalized isothermic lattices

International Nuclear Information System (INIS)

Doliwa, Adam

2007-01-01

We study multi-dimensional quadrilateral lattices satisfying simultaneously two integrable constraints: a quadratic constraint and the projective Moutard constraint. When the lattice is two dimensional and the quadric under consideration is the Moebius sphere one obtains, after the stereographic projection, the discrete isothermic surfaces defined by Bobenko and Pinkall by an algebraic constraint imposed on the (complex) cross-ratio of the circular lattice. We derive the analogous condition for our generalized isothermic lattices using Steiner's projective structure of conics, and we present basic geometric constructions which encode integrability of the lattice. In particular, we introduce the Darboux transformation of the generalized isothermic lattice and we derive the corresponding Bianchi permutability principle. Finally, we study two-dimensional generalized isothermic lattices, in particular geometry of their initial boundary value problem

Enhanced 29Si spin-lattice relaxation and observation of three-dimensional lattice connectivity in zeolites by two-dimensional 29Si MASS NMR

International Nuclear Information System (INIS)

Sivadinarayana, C.; Choudhary, V.R.; Ganapathy, S.

1994-01-01

It is shown that considerable sensitivity enhancement is achieved in the 29 Si magic angle sample spinning (MASS) NMR spectra of highly siliceous zeolites by pre treating the material with oxygen. The presence of adsorbed molecular oxygen in zeolite channels promotes an efficient 29 Si spin-lattice relaxation via a paramagnetic interaction between the lattice 29 Si T-site and the adsorbed oxygen on zeolite channels. This affords an efficient 2-D data collection and leads to increased sensitivity. The utility of this method is demonstrated in a two-dimensional COSY-45 NMR experiment of a high silica zeolite ZSM-5. (author). 20 refs., 3 figs., 1 tab

Combined measurement of surface, grain boundary and lattice diffusion coefficients on olivine bi-crystals

Science.gov (United States)

Marquardt, Katharina; Dohmen, Ralf; Wagner, Johannes

2014-05-01

Diffusion along interface and grain boundaries provides an efficient pathway and may control chemical transport in rocks as well as their mechanical strength. Besides the significant relevance of these diffusion processes for various geologic processes, experimental data are still very limited (e.g., Dohmen & Milke, 2010). Most of these data were measured using polycrystalline materials and the formalism of LeClaire (1951) to fit integrated concentration depth profiles. To correctly apply this formalism, certain boundary conditions of the diffusion problem need to be fulfilled, e.g., surface diffusion is ignored, and furthermore the lattice diffusion coefficient has to be known from other studies or is an additional fitting parameter, which produces some ambiguity in the derived grain boundary diffusion coefficients. We developed an experimental setup where we can measure the lattice and grain boundary diffusion coefficients simultaneously but independent and demonstrate the relevance of surface diffusion for typical grain boundary diffusion experiments. We performed Mg2SiO4 bicrystal diffusion experiments, where a single grain boundary is covered by a thin-film of pure Ni2SiO4 acting as diffusant source, produced by pulsed laser deposition. The investigated grain boundary is a 60° (011)/[100]. This specific grain boundary configuration was modeled using molecular dynamics for comparison with the experimental observations in the transmission electron microscope (TEM). Both, experiment and model are in good agreement regarding the misorientation, whereas there are still some disagreements regarding the strain fields along the grain boundary that are of outmost importance for the strengths of the material. The subsequent diffusion experiments were carried out in the temperature range between 800° and 1450° C. The inter diffusion profiles were measured using the TEMs energy dispersive x-ray spectrometer standardized using the Cliff-Lorimer equation and EMPA

Nuclear reaction analysis of Ge ion-implanted ZnO bulk single crystals: The evaluation of the displacement in oxygen lattices

Science.gov (United States)

Kamioka, K.; Oga, T.; Izawa, Y.; Kuriyama, K.; Kushida, K.; Kinomura, A.

2014-08-01

The displacement of oxygen lattices in Ge ion-implanted ZnO bulk single crystals is studied by nuclear reaction analysis (NAR), photoluminescence (PL), and Van der Pauw methods. The Ge ion-implantation (net concentration: 2.6 × 1020 cm-3) into ZnO is performed using a multiple-step energy. The high resistivity of ∼103 Ω cm in un-implanted samples remarkably decreased to ∼10-2 Ω cm after implanting Ge-ion and annealing subsequently. NRA measurements of as-implanted and annealed samples suggest the existence of the lattice displacement of O atoms acting as acceptor defects. As O related defects still remain after annealing, these defects are not attributed to the origin of the low resistivity in 800 and 1000 °C annealed ZnO.

Improved thrombogenicity on oxygen etched Ti6Al4V surfaces

Energy Technology Data Exchange (ETDEWEB)

Riedel, Nicholas A. [Department of Mechanical Engineering, Colorado State University, Fort Collins, CO 80523 (United States); Smith, Barbara S. [School of Biomedical Engineering, Colorado State University, Fort Collins, CO 80523 (United States); Williams, John D. [Department of Mechanical Engineering, Colorado State University, Fort Collins, CO 80523 (United States); Popat, Ketul C., E-mail: ketul.popat@colostate.edu [Department of Mechanical Engineering, Colorado State University, Fort Collins, CO 80523 (United States); School of Biomedical Engineering, Colorado State University, Fort Collins, CO 80523 (United States)

2012-07-01

Thrombus formation on blood contacting biomaterials continues to be a key factor in initiating a critical mode of failure in implantable devices, requiring immediate attention. In the interest of evaluating a solution for one of the most widely used biomaterials, titanium and its alloys, this study focuses on the use of a novel surface oxidation treatment to improve the blood compatibility. This study examines the possibility of using oblique angle ion etching to produce a high quality oxide layer that enhances blood compatibility on medical grade titanium alloy Ti6Al4V. An X-ray photoelectron spectroscopy (XPS) analysis of these oxygen-rich surfaces confirmed the presence of TiO{sub 2} peaks and also indicated increased surface oxidation as well as a reduction in surface defects. After 2 h of contact with whole human plasma, the oxygen etched substrates demonstrated a reduction in both platelet adhesion and activation as compared to bare titanium substrates. The whole blood clotting behavior was evaluated for up to 45 min, showing a significant decrease in clot formation on oxygen etched substrates. Finally, a bicinchoninic acid (BCA) total protein assay and XPS were used to evaluate the degree of key blood serum protein (fibrinogen, albumin, immunoglobulin G) adsorption on the substrates. The results showed similar protein levels for both the oxygen etched and control substrates. These results indicate that oblique angle oxygen etching may be a promising method to increase the thrombogenicity of Ti6Al4V. - Highlights: Black-Right-Pointing-Pointer Oblique angle oxygen ion etching creates a high quality, uniform oxide surface. Black-Right-Pointing-Pointer Oxygen etched substrates showed fewer adhered platelets. Black-Right-Pointing-Pointer Platelet activation was reduced by the improved oxide surface. Black-Right-Pointing-Pointer Oxygen etched substrates exhibited increased whole blood clotting times. Black-Right-Pointing-Pointer Although clotting reductions were

Extending the basic function of lattice oxygen in lepidocrocite titanate - The conversion of intercalated fatty acid to liquid hydrocarbon fuels

Science.gov (United States)

Maluangnont, Tosapol; Arsa, Pornanan; Sooknoi, Tawan

2017-12-01

We report herein the basicity of the external and internal lattice oxygen (OL) in lepidocrocite titanates with respect to CO2 and palmitic acid, respectively. Several compositions have been tested with different types of the metal M aliovalently (co)substituted for Ti, K0.8[MyTi2-y]O4 (M = Li, Mg, Fe, Co, Ni, Cu, Zn, Cu/Ni and Cu/Zn). The low CO2 desorption peak temperature (70-100 °C) suggests that the external OL sites are weakly basic similar to TiO2. However, the internal OL sites are sufficiently basic to deprotonate palmitic acid, forming the intercalated potassium palmitate at the interlayer spaces. The latter serves as a two-dimensional (2D) molecular reactor for the production of liquid hydrocarbon fuels via deoxygenation under atmospheric N2. A relationship has been observed between the yield of the liquid products vs the partial charge of the lattice oxygen (δO). Since the deoxygenation pathway is highly dependent on the metal substitution, the redox-active sites might also play some roles. The co-substituted K0.8[Cu0.2Ni0.2]Ti1.6O4 produced 68.0% yield of the liquid products, with 51% saturated and 15% unsaturated C15 hydrocarbons at 350 °C.

Influence of crystal orientation on the formation of femtosecond laser-induced periodic surface structures and lattice defects accumulation

Energy Technology Data Exchange (ETDEWEB)

Sedao, Xxx; Garrelie, Florence, E-mail: florence.garrelie@univ-st-etienne.fr; Colombier, Jean-Philippe; Reynaud, Stéphanie; Pigeon, Florent [Université de Lyon, CNRS, UMR5516, Laboratoire Hubert Curien, Université de Saint Etienne, Jean Monnet, F-42023 Saint-Etienne (France); Maurice, Claire; Quey, Romain [Ecole Nationale Supérieure des Mines de Saint-Etienne, CNRS, UMR5307, Laboratoire Georges Friedel, F-42023 Saint-Etienne (France)

2014-04-28

The influence of crystal orientation on the formation of femtosecond laser-induced periodic surface structures (LIPSS) has been investigated on a polycrystalline nickel sample. Electron Backscatter Diffraction characterization has been exploited to provide structural information within the laser spot on irradiated samples to determine the dependence of LIPSS formation and lattice defects (stacking faults, twins, dislocations) upon the crystal orientation. Significant differences are observed at low-to-medium number of laser pulses, outstandingly for (111)-oriented surface which favors lattice defects formation rather than LIPSS formation.

Kinetics of the high temperature oxygen exchange reaction on 238PuO2 powder

International Nuclear Information System (INIS)

Whiting, Christofer E.; Du, Miting; Felker, L. Kevin; Wham, Robert M.; Barklay, Chadwick D.; Kramer, Daniel P.

2015-01-01

Oxygen exchange reactions performed on PuO 2 suggest the reaction is influenced by at least three mechanisms: an internal chemical reaction, surface mobility of active species/defects, and surface exchange of gaseous oxygen with lattice oxygen. Activation energies for the surface mobility and internal chemical reaction are presented. Determining which mechanism is dominant appears to be a complex function including at least specific surface area and temperature. Thermal exposure may also impact the oxygen exchange reaction by causing reductions in the specific surface area of PuO 2 . Previous CeO 2 surrogate studies exhibit similar behavior, confirming that CeO 2 is a good qualitative surrogate for PuO 2 , in regards to the oxygen exchange reaction. Comparison of results presented here with previous work on the PuO 2 oxygen exchange reaction allows complexities in the previous work to be explained. These explanations allowed new conclusions to be drawn, many of which confirm the conclusions presented here. - Highlights: • PuO 2 Oxygen exchange kinetics can be influenced by at least 3 different mechanisms. • An internal chemical reaction controls the rate at high temperature and large SSA. • Surface mobility and surface exchange influence rate at lower temperatures and SSA. • Exchange temperatures may alter SSA and make data difficult to interpret.

Surface core level shifts of clean and oxygen covered Ir(111)

Energy Technology Data Exchange (ETDEWEB)

Bianchi, M; Cassese, D; Cavallin, A; Comin, R; Orlando, F; Postregna, L [Universita degli Studi di Trieste, Via A Valerio 2, 34127, Trieste (Italy); Golfetto, E; Baraldi, A [Dipartimento di Fisica e CENMAT, Universita degli Studi di Trieste, Via A Valerio 2, 34127, Trieste (Italy); Lizzit, S [Sincrotrone Trieste S.C.p.A., S.S. 14 Km 163.5, 34012 Trieste (Italy)], E-mail: alessandro.baraldi@elettra.trieste.it

2009-06-15

We present the results of high resolution core level photoelectron spectroscopy employed to investigate the electronic structure of clean and oxygen covered Ir(111) surface. Ir 4f{sub 7/2} core level spectra are shown to be very sensitive to the local atomic environment. For the clean surface we detected two distinct components shifted by 550 meV, originated by surface and bulk atoms. The larger Gaussian width of the bulk component is explained as due to experimentally unresolved subsurface components. In order to determine the relevance of the phonon contribution we examined the thermal behaviour of the core level lineshape using the Hedin-Rosengren theory. From the phonon-induced spectral broadening we found the Debye temperature of bulk and surface atoms to be 298 and 181 K, respectively, which confirms the softening of the vibrational modes at the surface. Oxygen adsorption leads to the appearance of new surface core level components at -200 meV and +230 meV, which are interpreted as due to first-layer Ir atoms differently coordinated with oxygen. The coverage dependence of these components demonstrates that the oxygen saturation corresponds to 0.38 ML, in good agreement with recent density functional theory calculations.

Nuclear reaction analysis of Ge ion-implanted ZnO bulk single crystals: The evaluation of the displacement in oxygen lattices

Energy Technology Data Exchange (ETDEWEB)

Kamioka, K.; Oga, T.; Izawa, Y. [College of Engineering and Research Center of Ion Beam Technology, Hosei University, Koganei, Tokyo 184-8584 (Japan); Kuriyama, K., E-mail: kuri@ionbeam.hosei.ac.jp [College of Engineering and Research Center of Ion Beam Technology, Hosei University, Koganei, Tokyo 184-8584 (Japan); Kushida, K. [Department of Arts and Science, Osaka Kyouiku University, Kashiwara, Osaka 582-8582 (Japan); Kinomura, A. [National Institute of Advanced Industrial Science and Technology, Tsukuba, Ibaraki 305-8568 (Japan)

2014-08-01

The displacement of oxygen lattices in Ge ion-implanted ZnO bulk single crystals is studied by nuclear reaction analysis (NAR), photoluminescence (PL), and Van der Pauw methods. The Ge ion-implantation (net concentration: 2.6 × 10{sup 20} cm{sup −3}) into ZnO is performed using a multiple-step energy. The high resistivity of ∼10{sup 3} Ω cm in un-implanted samples remarkably decreased to ∼10{sup −2} Ω cm after implanting Ge-ion and annealing subsequently. NRA measurements of as-implanted and annealed samples suggest the existence of the lattice displacement of O atoms acting as acceptor defects. As O related defects still remain after annealing, these defects are not attributed to the origin of the low resistivity in 800 and 1000 °C annealed ZnO.

Localized versus itinerant states created by multiple oxygen vacancies in SrTiO3

Science.gov (United States)

Jeschke, Harald O.; Shen, Juan; Valentí, Roser

2015-02-01

Oxygen vacancies in strontium titanate surfaces (SrTiO3) have been linked to the presence of a two-dimensional electron gas with unique behavior. We perform a detailed density functional theory study of the lattice and electronic structure of SrTiO3 slabs with multiple oxygen vacancies, with a main focus on two vacancies near a titanium dioxide terminated SrTiO3 surface. We conclude based on total energies that the two vacancies preferably inhabit the first two layers, i.e. they cluster vertically, while in the direction parallel to the surface, the vacancies show a weak tendency towards equal spacing. Analysis of the nonmagnetic electronic structure indicates that oxygen defects in the surface TiO2 layer lead to population of Ti {{t}2g} states and thus itinerancy of the electrons donated by the oxygen vacancy. In contrast, electrons from subsurface oxygen vacancies populate Ti eg states and remain localized on the two Ti ions neighboring the vacancy. We find that both the formation of a bound oxygen-vacancy state composed of hybridized Ti 3eg and 4p states neighboring the oxygen vacancy as well as the elastic deformation after extracting oxygen contribute to the stabilization of the in-gap state.

Strong asymmetry for surface modes in nonlinear lattices with long-range coupling

International Nuclear Information System (INIS)

Martinez, Alejandro J.; Vicencio, Rodrigo A.; Molina, Mario I.

2010-01-01

We analyze the formation of localized surface modes on a nonlinear cubic waveguide array in the presence of exponentially decreasing long-range interactions. We find that the long-range coupling induces a strong asymmetry between the focusing and defocusing cases for the topology of the surface modes and also for the minimum power needed to generate them. In particular, for the defocusing case, there is an upper power threshold for exciting staggered modes, which depends strongly on the long-range coupling strength. The power threshold for dynamical excitation of surface modes increases (decreases) with the strength of long-range coupling for the focusing (defocusing) cases. These effects seem to be generic for discrete lattices with long-range interactions.

Surface oxygen vacancy and oxygen permeation flux limits of perovskite ion transport membranes

KAUST Repository

Hunt, Anton; Dimitrakopoulos, Georgios; Ghoniem, Ahmed F.

2015-01-01

© 2015 Elsevier B.V. The mechanisms and quantitative models for how oxygen is separated from air using ion transport membranes (ITMs) are not well understood, largely due to the experimental complexity for determining surface exchange reactions

Atomic and molecular oxygen adsorbed on (111) transition metal surfaces: Cu and Ni

Energy Technology Data Exchange (ETDEWEB)

López-Moreno, S., E-mail: sinlopez@uacam.mx [Centro de Investigación en Corrosión, Universidad Autónoma de Campeche, Av. Héroe de Nacozari 480, Campeche, Campeche 24029 (Mexico); Romero, A. H. [Physics Department, West Virginia University, Morgantown, West Virginia 26506-6315 (United States)

2015-04-21

Density functional theory is used to investigate the reaction of oxygen with clean copper and nickel [111]-surfaces. We study several alternative adsorption sites for atomic and molecular oxygen on both surfaces. The minimal energy geometries and adsorption energies are in good agreement with previous theoretical studies and experimental data. From all considered adsorption sites, we found a new O{sub 2} molecular precursor with two possible dissociation paths on the Cu(111) surface. Cross barrier energies for the molecular oxygen dissociation have been calculated by using the climbing image nudge elastic band method, and direct comparison with experimental results is performed. Finally, the structural changes and adsorption energies of oxygen adsorbed on surface when there is a vacancy nearby the adsorption site are also considered.

Atomic and molecular oxygen adsorbed on (111) transition metal surfaces: Cu and Ni

Science.gov (United States)

López-Moreno, S.; Romero, A. H.

2015-04-01

Density functional theory is used to investigate the reaction of oxygen with clean copper and nickel [111]-surfaces. We study several alternative adsorption sites for atomic and molecular oxygen on both surfaces. The minimal energy geometries and adsorption energies are in good agreement with previous theoretical studies and experimental data. From all considered adsorption sites, we found a new O2 molecular precursor with two possible dissociation paths on the Cu(111) surface. Cross barrier energies for the molecular oxygen dissociation have been calculated by using the climbing image nudge elastic band method, and direct comparison with experimental results is performed. Finally, the structural changes and adsorption energies of oxygen adsorbed on surface when there is a vacancy nearby the adsorption site are also considered.

Atomic and molecular oxygen adsorbed on (111) transition metal surfaces: Cu and Ni

International Nuclear Information System (INIS)

López-Moreno, S.; Romero, A. H.

2015-01-01

Density functional theory is used to investigate the reaction of oxygen with clean copper and nickel [111]-surfaces. We study several alternative adsorption sites for atomic and molecular oxygen on both surfaces. The minimal energy geometries and adsorption energies are in good agreement with previous theoretical studies and experimental data. From all considered adsorption sites, we found a new O 2 molecular precursor with two possible dissociation paths on the Cu(111) surface. Cross barrier energies for the molecular oxygen dissociation have been calculated by using the climbing image nudge elastic band method, and direct comparison with experimental results is performed. Finally, the structural changes and adsorption energies of oxygen adsorbed on surface when there is a vacancy nearby the adsorption site are also considered

Tantalum surface oxidation: Bond relaxation, energy entrapment, and electron polarization

Energy Technology Data Exchange (ETDEWEB)

Guo, Yongling [Key Laboratory of Low-Dimensional Materials and Application Technologies (Ministry of Education), Hunan Provincial Key Laboratory of Thin Film Materials and Devices, Faculty of Materials Science and Engineering, Xiangtan University, Hunan 411105 (China); Bo, Maolin [Yangtze Normal University, College of Mechanical and Electrical Engineering, Chongqing 408100 (China); Wang, Yan [School of Information and Electronic Engineering, Hunan University of Science and Technology, Hunan 411201 (China); Liu, Yonghui [Key Laboratory of Low-Dimensional Materials and Application Technologies (Ministry of Education), Hunan Provincial Key Laboratory of Thin Film Materials and Devices, Faculty of Materials Science and Engineering, Xiangtan University, Hunan 411105 (China); Sun, Chang Q. [NOVITAS, School of Electrical and Electronic Engineering, Nanyang Technological University, Singapore 639798 (Singapore); Huang, Yongli, E-mail: huangyongli@xtu.edu.cn [Key Laboratory of Low-Dimensional Materials and Application Technologies (Ministry of Education), Hunan Provincial Key Laboratory of Thin Film Materials and Devices, Faculty of Materials Science and Engineering, Xiangtan University, Hunan 411105 (China)

2017-02-28

Graphical abstract: The bond, electron and energy relaxation result in core level energy shift, local densification, quantum entrapment and electron polarization of bonding electrons. - Highlights: • Increasing the oxygen coverage lowers the adsorption energy associated with lattice reconstruction. • Electrons transfer from Ta surface atoms to sp-hydrated oxygen, creating dipole moment that decreases the work function. • Oxygen chemisorption modified valence density-of-state (DOS) for Ta with four excessive DOS features: O−Ta bonding, O{sup 2−} lone pairs, Ta+ electron holes, and the lone-pair polarized Ta dipoles. • The bond, electron and energy relaxation between surface undercoordinated atoms are responsible for core level energy shift, local densification, quantum entrapment and electron polarization of bonding electrons. - Abstract: A combination of photoelectron spectrometric analysis and density functional theory calculations has enabled reconciliation of the bond-energy-electron relaxation for the Ta(100, 110, 111) surfaces chemisorbed with oxygen at different coverages. Results show that increasing oxygen coverage lowers the adsorption energy associated with lattice reconstruction. Valence electrons transfer from Ta surface atoms to oxygen to create four excessive DOS features in terms of O−Ta bonding, lone pairs of oxygen, Ta{sup +} electron holes, and polarized Ta dipoles. Oxidation proceeds in the following dynamics: oxygen gets electrons from two neighboring Ta atoms left behind Ta{sup +}; the sp{sup 3}-orbital hybridization takes place with additional two electron lone pairs, the lone pairs polarize the other two Ta neighbors becoming dipoles. X-ray photoelectron spectral analysis results in the 4f binding energy of an isolated Ta atom and its shift upon bond formation and oxidation. Exercises provide not only a promising numerical approach for the quantitative information about the bond and electronic behavior but also consistent

Tantalum surface oxidation: Bond relaxation, energy entrapment, and electron polarization

International Nuclear Information System (INIS)

Guo, Yongling; Bo, Maolin; Wang, Yan; Liu, Yonghui; Sun, Chang Q.; Huang, Yongli

2017-01-01

Graphical abstract: The bond, electron and energy relaxation result in core level energy shift, local densification, quantum entrapment and electron polarization of bonding electrons. - Highlights: • Increasing the oxygen coverage lowers the adsorption energy associated with lattice reconstruction. • Electrons transfer from Ta surface atoms to sp-hydrated oxygen, creating dipole moment that decreases the work function. • Oxygen chemisorption modified valence density-of-state (DOS) for Ta with four excessive DOS features: O−Ta bonding, O"2"− lone pairs, Ta+ electron holes, and the lone-pair polarized Ta dipoles. • The bond, electron and energy relaxation between surface undercoordinated atoms are responsible for core level energy shift, local densification, quantum entrapment and electron polarization of bonding electrons. - Abstract: A combination of photoelectron spectrometric analysis and density functional theory calculations has enabled reconciliation of the bond-energy-electron relaxation for the Ta(100, 110, 111) surfaces chemisorbed with oxygen at different coverages. Results show that increasing oxygen coverage lowers the adsorption energy associated with lattice reconstruction. Valence electrons transfer from Ta surface atoms to oxygen to create four excessive DOS features in terms of O−Ta bonding, lone pairs of oxygen, Ta"+ electron holes, and polarized Ta dipoles. Oxidation proceeds in the following dynamics: oxygen gets electrons from two neighboring Ta atoms left behind Ta"+; the sp"3-orbital hybridization takes place with additional two electron lone pairs, the lone pairs polarize the other two Ta neighbors becoming dipoles. X-ray photoelectron spectral analysis results in the 4f binding energy of an isolated Ta atom and its shift upon bond formation and oxidation. Exercises provide not only a promising numerical approach for the quantitative information about the bond and electronic behavior but also consistent insight into the

Surface magnetization of the Ising ferromagnet in semi-infinite cubic lattice: renormalization group approach

International Nuclear Information System (INIS)

Chame, A.M.N.; Tsallis, C.

1988-01-01

The behaviour of the spontaneous surface and bulk magnetizations as function of the temperature for the Ising ferromagnet in a semi-infinitre cubic lattice for various ratios JS/JB (JS and JB are the surface and bulk coupling constants, respectively), is studied. The extraordinary transition where the surface maintains its magnetization as the bulk disorders, was study, in particular; a discontinuity on the first derivative of the surface magnetization at the bulk transition temperature was found. The criticality of the system (universality classes, critical exponents and amplitudes) is discussed. An unexpected slight lack of monotonicity of the surface magnetization as a function of JS/JB for JS/JB [pt

The surface oxide as a source of oxygen on Rh(1 1 1)

Energy Technology Data Exchange (ETDEWEB)

Lundgren, E. [Department of Synchrotron Radiation Research, Institute of Physics, Lund University, Box 118, S-221 00 Lund (Sweden)]. E-mail: edvin.lundgren@sljus.lu.se; Gustafson, J. [Department of Synchrotron Radiation Research, Institute of Physics, Lund University, Box 118, S-221 00 Lund (Sweden); Resta, A. [Department of Synchrotron Radiation Research, Institute of Physics, Lund University, Box 118, S-221 00 Lund (Sweden); Weissenrieder, J. [Department of Synchrotron Radiation Research, Institute of Physics, Lund University, Box 118, S-221 00 Lund (Sweden); Mikkelsen, A. [Department of Synchrotron Radiation Research, Institute of Physics, Lund University, Box 118, S-221 00 Lund (Sweden); Andersen, J.N. [Department of Synchrotron Radiation Research, Institute of Physics, Lund University, Box 118, S-221 00 Lund (Sweden); Koehler, L. [Institut fuer Materialphysik and Centre for Computational Materials Science, Universitaet Wien, A-1090 Vienna (Austria); Kresse, G. [Institut fuer Materialphysik and Centre for Computational Materials Science, Universitaet Wien, A-1090 Vienna (Austria); Klikovits, J. [Institut fuer Allgemeine Physik, Technische Universitaet Wien, A-1040 Vienna (Austria); Biederman, A. [Institut fuer Allgemeine Physik, Technische Universitaet Wien, A-1040 Vienna (Austria); Schmid, M. [Institut fuer Allgemeine Physik, Technische Universitaet Wien, A-1040 Vienna (Austria); Varga, P. [Institut fuer Allgemeine Physik, Technische Universitaet Wien, A-1040 Vienna (Austria)

2005-06-15

The reduction of a thin surface oxide on the Rh(1 1 1) surface by CO is studied in situ by photoemission spectroscopy, scanning tunneling microscopy, and density functional theory. CO molecules are found not to adsorb on the surface oxide at a sample temperature of 100 K, in contrast to on the clean and chemisorbed oxygen covered surface. Despite this behavior, the surface oxide may still be reduced by CO, albeit in a significantly different fashion as compared to the reduction of a phase containing only chemisorbed on surface oxygen. The experimental observations combined with theoretical considerations concerning the stability of the surface oxide, result in a model of the reduction process at these pressures suggesting that the surface oxide behaves as a source of oxygen for the CO-oxidation reaction.

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

Kinetics of the high temperature oxygen exchange reaction on {sup 238}PuO{sub 2} powder

Energy Technology Data Exchange (ETDEWEB)

Whiting, Christofer E., E-mail: chris.whiting@udri.udayton.edu [University of Dayton – Research Institute, 300 College Park, Dayton, OH 45469-0172 (United States); Du, Miting; Felker, L. Kevin; Wham, Robert M. [Oak Ridge National Laboratory, P.O. Box 2008, Oak Ridge, TN 37831 (United States); Barklay, Chadwick D.; Kramer, Daniel P. [University of Dayton – Research Institute, 300 College Park, Dayton, OH 45469-0172 (United States)

2015-12-15

Oxygen exchange reactions performed on PuO{sub 2} suggest the reaction is influenced by at least three mechanisms: an internal chemical reaction, surface mobility of active species/defects, and surface exchange of gaseous oxygen with lattice oxygen. Activation energies for the surface mobility and internal chemical reaction are presented. Determining which mechanism is dominant appears to be a complex function including at least specific surface area and temperature. Thermal exposure may also impact the oxygen exchange reaction by causing reductions in the specific surface area of PuO{sub 2}. Previous CeO{sub 2} surrogate studies exhibit similar behavior, confirming that CeO{sub 2} is a good qualitative surrogate for PuO{sub 2}, in regards to the oxygen exchange reaction. Comparison of results presented here with previous work on the PuO{sub 2} oxygen exchange reaction allows complexities in the previous work to be explained. These explanations allowed new conclusions to be drawn, many of which confirm the conclusions presented here. - Highlights: • PuO{sub 2} Oxygen exchange kinetics can be influenced by at least 3 different mechanisms. • An internal chemical reaction controls the rate at high temperature and large SSA. • Surface mobility and surface exchange influence rate at lower temperatures and SSA. • Exchange temperatures may alter SSA and make data difficult to interpret.

Temperature-Independent Fermi Surface in the Kondo Lattice YbRh_{2}Si_{2}

Directory of Open Access Journals (Sweden)

K. Kummer

2015-03-01

Full Text Available Strongly correlated electron systems are one of the central topics in contemporary solid-state physics. Prominent examples for such systems are Kondo lattices, i.e., intermetallic materials in which below a critical temperature, the Kondo temperature T_{K}, the magnetic moments become quenched and the effective masses of the conduction electrons approach the mass of a proton. In Ce- and Yb-based systems, this so-called heavy-fermion behavior is caused by interactions between the strongly localized 4f and itinerant electrons. A major and very controversially discussed issue in this context is how the localized electronic degree of freedom gets involved in the Fermi surface (FS upon increasing the interaction between both kinds of electrons or upon changing the temperature. In this paper, we show that the FS of a prototypic Kondo lattice, YbRh_{2}Si_{2}, does not change its size or shape in a wide temperature range extending from well below to far above the single-ion Kondo temperature T_{K}∼25  K of this system. This experimental observation, obtained by means of angle-resolved photoemission spectroscopy, is in remarkable contrast to the widely believed evolution from a large FS, including the 4f degrees of freedom, to a small FS, without the 4f’s, upon increasing temperature. Our results explicitly demonstrate a need to further advance in theoretical approaches based on the periodic Anderson model in order to elucidate the temperature dependence of Fermi surfaces in Kondo lattices.

The Role of Lattice Vibrations in Adatom Diffusion at Metal Stepped Surfaces

International Nuclear Information System (INIS)

Durakanoglu, S.

2004-01-01

Diffusion of a single atom on metal surfaces remains a subject of continuing interest in the surface science community because of the important role it plays in several technologically important phenomena such as thin-film and eptaxial growth, catalysis and chemical reactions. Except for a few studies, most of theoretical works, ranging from molecular dynamic simulations to first principle electronic structure calculations, are devoted to determination of the characteristics of the diffusion processes and the energy barriers, neglecting the contribution of lattice vibrations in adatom diffusion. However, in a series of theoretical works on self-diffusion on the flat surfaces of Cu(100), Ag(100) and Ni(100), Ulrike et al.[1-3], showed that the vibrational contributions are important and should be included in any complete description of the temperature dependence of the diffusion coefficient. In this work, it is our aim to examine the role of lattice vibrations in adatom diffusion at stepped surfaces of Cu(100) and Ni(100) within the framework of transition state theory. Ehrlich-Shwoebel energy barriers for an adatom diffusing over a step-edge are calculated through the inclusion of vibrational internal energy. Local vibrational density of states, main ingredient to the vibrational thermodynamic functions, are calculated in the harmonic approximation, using real space Green's function method with the force constants derived from interaction potentials based on the embedded atom method. We emphasize the sensitivity of the local vibrational density of states to the local atomic environment. We, furthermore, discuss the contribution of thermodynamic functions calculated from local vibrational density of states to the prefactors in diffusion coefficient

Analysis of heterogeneous oxygen exchange and fuel oxidation on the catalytic surface of perovskite membranes

KAUST Repository

Hong, Jongsup

2013-10-01

The catalytic kinetics of oxygen surface exchange and fuel oxidation for a perovskite membrane is investigated in terms of the thermodynamic state in the immediate vicinity of or on the membrane surface. Perovskite membranes have been shown to exhibit both oxygen perm-selectivity and catalytic activity for hydrocarbon conversion. A fundamental description of their catalytic surface reactions is needed. In this study, we infer the kinetic parameters for heterogeneous oxygen surface exchange and catalytic fuel conversion reactions, based on permeation rate measurements and a spatially resolved physical model that incorporates detailed chemical kinetics and transport in the gas-phase. The conservation equations for surface and bulk species are coupled with those of the gas-phase species through the species production rates from surface reactions. It is shown that oxygen surface exchange is limited by dissociative/associative adsorption/desorption of oxygen molecules onto/from the membrane surface. On the sweep side, while the catalytic conversion of methane to methyl radical governs the overall surface reactions at high temperature, carbon monoxide oxidation on the membrane surface is dominant at low temperature. Given the sweep side conditions considered in ITM reactor experiments, gas-phase reactions also play an important role, indicating the significance of investigating both homogeneous and heterogeneous chemistry and their coupling when examining the results. We show that the local thermodynamic state at the membrane surface should be considered when constructing and examining models of oxygen permeation and heterogeneous chemistry. © 2013 Elsevier B.V.

Analysis of heterogeneous oxygen exchange and fuel oxidation on the catalytic surface of perovskite membranes

KAUST Repository

Hong, Jongsup; Kirchen, Patrick; Ghoniem, Ahmed F.

2013-01-01

The catalytic kinetics of oxygen surface exchange and fuel oxidation for a perovskite membrane is investigated in terms of the thermodynamic state in the immediate vicinity of or on the membrane surface. Perovskite membranes have been shown to exhibit both oxygen perm-selectivity and catalytic activity for hydrocarbon conversion. A fundamental description of their catalytic surface reactions is needed. In this study, we infer the kinetic parameters for heterogeneous oxygen surface exchange and catalytic fuel conversion reactions, based on permeation rate measurements and a spatially resolved physical model that incorporates detailed chemical kinetics and transport in the gas-phase. The conservation equations for surface and bulk species are coupled with those of the gas-phase species through the species production rates from surface reactions. It is shown that oxygen surface exchange is limited by dissociative/associative adsorption/desorption of oxygen molecules onto/from the membrane surface. On the sweep side, while the catalytic conversion of methane to methyl radical governs the overall surface reactions at high temperature, carbon monoxide oxidation on the membrane surface is dominant at low temperature. Given the sweep side conditions considered in ITM reactor experiments, gas-phase reactions also play an important role, indicating the significance of investigating both homogeneous and heterogeneous chemistry and their coupling when examining the results. We show that the local thermodynamic state at the membrane surface should be considered when constructing and examining models of oxygen permeation and heterogeneous chemistry. © 2013 Elsevier B.V.

LATTICE: The Lower ATmosphere-Thermosphere-Ionosphere Coupling Experiment

Science.gov (United States)

Mlynczak, M. G.; Yee, J. H.

2017-12-01

We present the Lower Atmosphere-Thermosphere-Ionosphere Coupling Experiment (LATTICE), which is a candidate mission for proposal to a future NASA Announcement of Opportunity. LATTICE will make the first consistent measurements of global kinetic temperature from the tropopause up to at least 160 km, along with global vector winds from 100 to 160 km at all local times. LATTICE thus provides, for the first time, a consistent picture of the coupling of the terrestrial lower atmosphere to the thermosphere-ionosphere system, which is a major scientific goal outlined in the 2012 Heliophysics Decadal Survey. The core instruments on LATTICE are the Terahertz Limb Sounder (TLS) and the Sounding of the Atmosphere using Broadband Emission Radiometry-II (SABER-II) instrument. The TLS instrument measures the 147 µm (2.04 THz) fine structure line of atomic oxygen. From these measurements TLS will provide kinetic temperature, atomic oxygen density, and vector wind from 100 to at least 160 km altitude. SABER-II is an infrared radiometer and is optically identical to the legacy SABER instrument on the current TIMED satellite. SABER-II is half the mass, half the power, and one-third the volume of the legacy instrument, and expects the same radiometric performance. SABER-II will again measure kinetic temperature from 15 to 110 km and will make measurements of key parameters in the thermosphere-ionosphere system including NO+, the green line and red line emissions, as well as continuing legacy measurements of ozone, water vapor, atomic oxygen, and atomic hydrogen in the mesosphere and lower thermosphere. We will describe the LATTICE mission in detail including other potential instruments for diagnosing thermospheric composition and high latitude energy inputs, and for measuring solar ultraviolet irradiance.

Surface defect chemistry and oxygen exchange kinetics in La2-xCaxNiO4+δ

Science.gov (United States)

Tropin, E. S.; Ananyev, M. V.; Farlenkov, A. S.; Khodimchuk, A. V.; Berenov, A. V.; Fetisov, A. V.; Eremin, V. A.; Kolchugin, A. A.

2018-06-01

Surface oxygen exchange kinetics and diffusion in La2-xCaxNiO4+δ (x = 0; 0.1; 0.3) have been studied by the isotope exchange method with gas phase equilibration in the temperature range of 600-800 °C and oxygen pressure range 0.13-2.5 kPa. Despite an enhanced electrical conductivity of La2-xCaxNiO4+δ theirs oxygen surface exchange (k*) and oxygen tracer diffusion (D*) coefficients were significantly lower in comparison with La2NiO4+δ. The rates of the elementary stages of oxygen exchange have been calculated. Upon Ca doping the change of the rate-determining stage was observed. The surface of the oxides was found to be inhomogeneous towards oxygen exchange process according to the recently developed model. The reasons of such inhomogeneity are discussed as well as Ca influence on the surface defect chemistry and oxygen surface exchange and diffusivity.

A high resolution photoemission study of surface core-level shifts in clean and oxygen-covered Ir(2 1 0) surfaces

Energy Technology Data Exchange (ETDEWEB)

Gladys, M.J.; Ermanoski, I.; Jackson, G.; Quinton, J.S.; Rowe, J.E.; Madey, T.E. E-mail: madey@physics.rutgers.edu

2004-04-01

High resolution soft X-ray photoemission electron spectroscopy (SXPS), using synchrotron radiation, is employed to investigate 4f core-level features of four differently-prepared Ir(2 1 0) surfaces: clean planar, oxygen-covered planar, oxygen-induced faceted, and clean faceted surfaces. Surface and bulk peak identifications are supported by measurements at different photon energies (thus probing different electron escape depths) and variable emission angles. Iridium 4f{sub 7/2} photoemission spectra are fitted with Doniach-Sunjic lineshapes. The surface components are identified with core levels positioned at lower binding energies than the bulk components, in contrast to previous reports of binding energy inversion on Ir(1 0 0) (1x1) and (5x1) surfaces. For clean planar Ir(2 1 0) three surface Ir 4f{sub 7/2} features are observed with core-level shifts of -765, -529, and -281 meV, with respect to the bulk; these are associated with the first, second and third layers of atoms, respectively, for atomically rough Ir(2 1 0). Adsorption of oxygen onto the planar Ir(2 1 0) surface is found to cause a suppression and shift of the surface features to higher binding energies. Annealing at T{>=}600 K in oxygen produces a faceted surface as verified by low energy electron diffraction (LEED). A comparison of planar and faceted oxygen-covered surfaces reveals minor differences in the normal emission SXPS spectra, while grazing emission spectra exhibit differences. The SXPS spectrum of the clean, faceted Ir(2 1 0) exhibits small differences in comparison to the clean planar case, with surface features having binding energy shifts of -710, -450, and -230 meV.

Passivation of CdZnTe surfaces by oxidation in low energy atomic oxygen

International Nuclear Information System (INIS)

Chen, H.; Chattopadhyay, K.; Chen, K.; Burger, A.; George, M.A.; Gregory, J.C.; Nag, P.K.; Weimer, J.J.; James, R.B.

1999-01-01

A method of surface passivation of Cd 1-x Zn x Te (CZT) x-ray and gamma ray detectors has been established by using microwave-assisted atomic oxygen bombardment. Detector performance is significantly enhanced due to the reduction of surface leakage current. CZT samples were exposed to an atomic oxygen environment at the University of Alabama in Huntsville close-quote s Thermal Atomic Oxygen Facility. This system generates neutral atomic oxygen species with kinetic energies of 0.1 - 0.2 eV. The surface chemical composition and its morphology modification due to atomic oxygen exposure were studied by x-ray photoelectron spectroscopy and atomic force microscopy and the results were correlated with current-voltage measurements and with room temperature spectral responses to 133 Ba and 241 Am radiation. A reduction of leakage current by about a factor of 2 is reported, together with significant improvement in the gamma-ray line resolution. copyright 1999 American Vacuum Society

Optical absorption and oxygen passivation of surface states in III-nitride photonic devices

Science.gov (United States)

Rousseau, Ian; Callsen, Gordon; Jacopin, Gwénolé; Carlin, Jean-François; Butté, Raphaël; Grandjean, Nicolas

2018-03-01

III-nitride surface states are expected to impact high surface-to-volume ratio devices, such as nano- and micro-wire light-emitting diodes, transistors, and photonic integrated circuits. In this work, reversible photoinduced oxygen desorption from III-nitride microdisk resonator surfaces is shown to increase optical attenuation of whispering gallery modes by 100 cm-1 at λ = 450 nm. Comparison of photoinduced oxygen desorption in unintentionally and n+-doped microdisks suggests that the spectral changes originate from the unpinning of the surface Fermi level, likely taking place at etched nonpolar III-nitride sidewalls. An oxygen-rich surface prepared by thermal annealing results in a broadband Q improvement to state-of-the-art values exceeding 1 × 104 at 2.6 eV. Such findings emphasize the importance of optically active surface states and their passivation for future nanoscale III-nitride optoelectronic and photonic devices.

Kinetics of diffuesion-controlled oxygen ordering in a lattic-gas model of YBa₂Cu₃O_7-δ

DEFF Research Database (Denmark)

Andersen, Jørgen Vitting; Bohr, Henrik; Mouritsen, Ole G.

1990-01-01

Nonequilibrium properties of oxygen ordering in high-Tc superconductors of the Y-Ba-Cu-O type are studied via computer simulation of an anisotropic two-dimensional lattice-gas model in which the ordering processes are controlled by diffusion across the sample edges. With a view to designing optimal...

The modification of nanocomposite hybrid polymer surfaces by exposure to oxygen containing plasmas

Science.gov (United States)

Figueiredo, Ashley; Zimmermann, Katherine; Augustine, Brian; Hughes, Chris; Chusuei, Charles

2006-11-01

The wetting properties of the surfaces of the nanocomposite hybrid polymer poly[(propylmethacryl-heptaisobutyl- polyhedral oligomeric silsequioxane)-co-(methylmethacrylate)] (POSS-PMMA)has been studied before and after exposure to plasmas containing oxygen. The contact angle of water droplets on the surface showed a substantial decrease after plasma exposure indicating an increase in the hydrophilicity of the surface. A model was developed in which the plasma preferentially removed organic material including both the PMMA backbone and isobutyl groups from the corners of the POSS cages leaving behind a surface characterized by the silicon oxide-like POSS material. Measurements of surface concentrations of oxygen, silicon, and carbon by x-ray photoelectron spectroscopy (XPS) showed an increase in the amount of oxygen and silicon compared to carbon and the appropriate chemical shifts were observed in the XPS data to support the model of Si-O enrichment on the surface. Variable angle spectroscopic ellipsometry (VASE) and atomic force microscopy (AFM) measurements also supported the model and these results will be presented.

REVIEW ARTICLE: Oxygen diffusion and precipitation in Czochralski silicon

Science.gov (United States)

Newman, R. C.

2000-06-01

The objective of this article is to review our understanding of the properties of oxygen impurities in Czochralski silicon that is used to manufacture integrated circuits (ICs). These atoms, present at a concentration of ~1018 cm-3, occupy bond-centred sites (Oi) in as-grown Si and the jump rate between adjacent sites defines `normal' diffusion for the temperature range 1325 - 330 °C. Anneals at high temperatures lead to the formation of amorphous SiO2 precipitates that act as traps for fast diffusing metallic contaminants, such as Fe and Cu, that may be inadvertently introduced at levels as low as 1011 cm-3. Without this `gettering', there may be severe degradation of fabricated ICs. To accommodate the local volume increase during oxygen precipitation, there is parallel generation of self-interstitials that diffuse away and form lattice defects. High temperature (T > 700 °C) anneals are now well understood. Details of lower temperature processes are still a matter of debate: measurements of oxygen diffusion into or out of the Si surface and Oi atom aggregation have implied enhanced diffusion that has variously been attributed to interactions of Oi atoms with lattice vacancies, self-interstitials, metallic elements, carbon, hydrogen impurities etc. There is strong evidence for oxygen-hydrogen interactions at T continue to decrease as the size of future device features decreases below the lower end of the sub-micron range, currently close to 0.18 µm.

Photo-oxidation: Major sink of oxygen in the ocean surface layer

NARCIS (Netherlands)

Gieskes, W.W.C.; Laane, R.W.P.M.; Ruardij, P.

2015-01-01

Evidence is presented that the oxygen demand associated with photochemical processes in the surface layer of oceans and seas worldwide is of the same order of magnitude as the amount of oxygen released by photosynthesis of the world's marine phytoplankton. Both estimates are of necessity quite rough

Photo-oxidation : Major sink of oxygen in the ocean surface layer

NARCIS (Netherlands)

Gieskes, W. W. C.; Laane, R. W. P. M.; Ruardij, P.

2015-01-01

Evidence is presented that the oxygen demand associated with photochemical processes in the surface layer of oceans and seas worldwide is of the same order of magnitude as the amount of oxygen released by photosynthesis of the world's marine phytoplankton. Both estimates are of necessity quite rough

Understanding the influence of surface chemical states on the dielectric tunability of sputtered Ba0.5Sr0.5TiO3 thin films

Science.gov (United States)

Venkata Saravanan, K.; Raju, K. C. James

2014-03-01

The surface chemical states of RF-magnetron sputtered Ba0.5Sr0.5TiO3 (BST5) thin films deposited at different oxygen mixing percentage (OMP) was examined by x-ray photoelectron spectroscopy. The O1s XPS spectra indicate the existence of three kinds of oxygen species (dissociated oxygen ion O2 -, adsorbed oxide ion O- and lattice oxide ion O2-) on the films’ surface, which strongly depends on OMP. The presence of oxygen species other than lattice oxygen ion makes the films’ surface highly reactivity to atmospheric gases, resulting in the formation of undesired surface layers. The XPS results confirm the formation of surface nitrates for the films deposited under oxygen deficient atmosphere (OMP ≦̸ 25%), whereas the films deposited in oxygen rich atmosphere (OMP ≧̸ 75%) show the presence of metal-hydroxide. The influence of a surface dead layer on the tunable dielectric properties of BST5 films have been studied in detail and are reported. Furthermore, our observations indicate that an optimum ratio of Ar:O2 is essential for achieving desired material and dielectric properties in BST5 thin films. The films deposited at 50% OMP have the highest dielectric tunability of ~65% (@280 kV cm-1), with good ɛ r-E curve symmetry of 98% and low tan δ of 0.018. The figure of merit for these films is about 35, which is promising for frequency agile device applications.

Effect of the surface oxygen groups on methane adsorption on coals

Energy Technology Data Exchange (ETDEWEB)

Hao Shixiong [Department of Chemical Engineering, Sichuan University, Chengdu 610065 (China); Department of Chemical Engineering, Sichuan University of Science and Engineering, Zigong 643000 (China); Wen Jie [Department of Chemical Engineering, Sichuan University, Chengdu 610065 (China); Yu Xiaopeng [Department of Chemical Engineering, Sichuan University, Chengdu 610065 (China); Department of Chemical Engineering, Sichuan University of Science and Engineering, Zigong 643000 (China); Chu Wei, E-mail: chuwei1965_scu@yahoo.com [Department of Chemical Engineering, Sichuan University, Chengdu 610065 (China)

2013-01-01

Highlights: Black-Right-Pointing-Pointer We modified one coal with H{sub 2}O{sub 2}, (NH{sub 4}){sub 2}S{sub 2}O{sub 8} and HNO{sub 3} respectively, to prepare coal samples with different surface properties. Black-Right-Pointing-Pointer The oxygen groups on coal surface were characterized by XPS. Black-Right-Pointing-Pointer The textures of the coal samples were investigated by N{sub 2} adsorption at 77 K. Black-Right-Pointing-Pointer The adsorption behaviors were measured by volumetric method. Black-Right-Pointing-Pointer There was a negative correlation between methane saturated adsorption capacity and the O{sub total}/C{sub total}. - Abstract: To investigate the influence of surface oxygen groups on methane adsorption on coals, one bituminous coal was modified with H{sub 2}O{sub 2}, (NH{sub 4}){sub 2}S{sub 2}O{sub 8} and HNO{sub 3} respectively, to prepare coal samples with different surface properties. The oxygen groups on coal surface were characterized by X-ray photoelectron spectroscopy (XPS). The textures of the coal samples were investigated by N{sub 2} adsorption at 77 K. Their surface morphologies were analyzed by scanning electron microscopy (SEM). The methane adsorption behaviors of these coal samples were measured at 303 K in pressure range of 0-5.3 MPa by volumetric method. The adsorption data of methane were fitted to the Langmuir model and Dubinin-Astakhov (D-A) model. The fitting results showed that the D-A model fitted the isotherm data better than the Langmuir model. It was observed that there was, in general, a positive correlation between the methane saturated adsorption capacity and the micropore volume of coals while a negative correlation between methane saturated adsorption capacity and the O{sub total}/C{sub total}. The methane adsorption capacity was determined by the coal surface chemistry when the microporosity parameters of two samples were similar. Coal with a higher amount of oxygen surface groups, and consequently with a less

Role of CO2 in the oxy-dehydrogenation of ethylbenzene to styrene on the CeO2(111) surface

Science.gov (United States)

Fan, Hong-Xia; Feng, Jie; Li, Wen-Ying; Li, Xiao-Hong; Wiltowski, Tomasz; Ge, Qing-Feng

2018-01-01

The role of CO2 in the ethylbenzene oxy-dehydrogenation to styrene on the CeO2(111) surface was thoroughly investigated by the density functional theory (DFT) calculations. Results show that the first Csbnd H bond of ethylbenzene is activated via the oxo-insertion with a barrier of 1.70 eV, resulting in a 2-phenylethyl species and an H atom adsorbed on two-adjacent-lattice oxygen. The H adatom forms a hydroxyl-like species (denoted as O*H). The subsequent dehydrogenation to styrene can be assisted by either the next lattice oxygen (pathway R1) or the O*H species (pathway R2). The two pathways have almost the same activation energy (0.84 eV for R1 and 0.85 eV for R2), forming a new O*H and desorbing a H2O molecule while leaving an oxygen vacancy on the surface, respectively. In the presence of CO2, it will react with O*H through the reverse water gas shift reaction with an activation barrier of 0.98 eV and reaction energy of 0.30 eV. The reverse water gas shift reaction helps to clear the H adatoms from the lattice oxygen, thereby competing with styrene formation via pathway R2. However, the activation energy following the reverse water gas shift mechanism is 0.13 eV higher than that of styrene formation via pathway R2. Therefore, the formation of oxygen vacancy cannot be inhibited, while CO2 can react with the surface oxygen vacancy to produce CO with a high activation energy of 2.10 eV.

Lattice Boltzmann model for thermal free surface flows with liquid-solid phase transition

International Nuclear Information System (INIS)

Attar, Elham; Koerner, Carolin

2011-01-01

Purpose: The main objective of this work is to develop an algorithm to use the Lattice Boltzmann method for solving free surface thermal flow problems with solid/liquid phase changes. Approach: A multi-distribution function model is applied to simulate hydrodynamic flow and the coupled thermal diffusion-convection problem. Findings: The free surface problem, i.e. the reconstruction of the missing distribution functions at the interface, can be solved by applying a physical transparent momentum and heat flux based methodology. The developed method is subsequently applied to some test cases in order to assess its computational potentials. Practical implications: Many industrial processes involve problems where non-isothermal motion and simultaneous solidification of fluids with free surface is important. Examples are all castings processes and especially foaming processes which are characterized by a huge and strongly changing surface. Value: A reconstruction algorithm to treat a thermal hydrodynamic problem with free surfaces is presented which is physically transparent and easy to implement.

Atomic structure of diamond {111} surfaces etched in oxygen water vapor

International Nuclear Information System (INIS)

Theije, F.K. de; Reedijk, M.F.; Arsic, J.; Enckevort, W.J.P. van; Vlieg, E.

2001-01-01

The atomic structure of the {111} diamond face after oxygen-water-vapor etching is determined using x-ray scattering. We find that a single dangling bond diamond {111} surface model, terminated by a full monolayer of -OH fits our data best. To explain the measurements it is necessary to add an ordered water layer on top of the -OH terminated surface. The vertical contraction of the surface cell and the distance between the oxygen atoms are generally in agreement with model calculations and results on similar systems. The OH termination is likely to be present during etching as well. This model experimentally confirms the atomic-scale mechanism we proposed previously for this etching system

Oxygen adsorption on the Al0.25Ga0.75N (0001) surface: A first-principles study

Science.gov (United States)

Fu, Jiaqi; Song, Tielei; Liang, Xixia; Zhao, Guojun

2018-04-01

To understand the interaction mechanism for the oxygen adsorption on AlGaN surface, herein, we built the possible models of oxygen adsorption on Al0.25Ga0.75N (0001) surface. For different oxygen coverage, three kinds of adsorption site are considered. Then the favorable adsorption sites are characterized by first principles calculation for (2 × 2) supercell of Al0.25Ga0.75N (0001) surface. On basis of the optimal adsorption structures, our calculated results show that all the adsorption processes are exothermic, indicating that the (0001) surface orientation is active towards the adsorption of oxygen. The doping of Al is advantage to the adsorption of O atom. Additionally, the adsorption energy decreases with reducing the oxygen coverage, and the relationship between them is approximately linear. Owing to the oxygen adsorption, the surface states in the fundamental band gap are significant reduced with respect to the free Al0.25Ga0.75N (0001) surface. Moreover, the optical properties on different oxygen coverage are also discussed.

Approximate critical surface of the bond-mixed square-lattice Ising model

International Nuclear Information System (INIS)

Levy, S.V.F.; Tsallis, C.; Curado, E.M.F.

1979-09-01

The critical surface of the quenched bond-mixed square-lattice spin-1/2 first-neighbour-interaction ferromagnetic Ising model (with exchange interactions J 1 and J 2 ) has been investigated. Through renormalization group and heuristical procedures, a very accurate (error inferior to 3x10 -4 in the variables t sub(i) = th (J sub(i)/k sub(b)T)) approximate numerical proposal for all points of this surface is presented. This proposal simultaneously satisfies all the available exact results concerning the surface, namely P sub(c) = 1/2, t sub(c) = √2 - 1, both limiting slopes in these points, and t 2 = (1-t 1 )/(1+t 1 ) for p = 1/2. Furthemore an analytic approximation (namely (1 - p) 1n(1 + t 1 ) + p 1n(1 + t 2 ) =(1/2)1n 2) is also proposed. In what concerns the available exact results, it only fails in reproducing one of the two limiting slopes, where there is an error of 1% in the derivative: these facts result in an estimated error less than 10 -3 (in the t-variables) for any points in the surface. (Author) [pt

Relating surface chemistry and oxygen surface exchange in LnBaCo2O(5+δ) air electrodes.

Science.gov (United States)

Téllez, Helena; Druce, John; Kilner, John A; Ishihara, Tatsumi

2015-01-01

The surface and near-surface chemical composition of electroceramic materials often shows significant deviations from that of the bulk. In particular, layered materials, such as cation-ordered LnBaCo2O(5+δ) perovskites (Ln = lanthanide), undergo surface and sub-surface restructuring due to the segregation of the divalent alkaline-earth cation. These processes can take place during synthesis and processing steps (e.g. deposition, sintering or annealing), as well as at temperatures relevant for the operation of these materials as air electrodes in solid oxide fuel cells and electrolysers. Furthermore, the surface segregation in these double perovskites shows fast kinetics, starting at temperatures as low as 400 °C over short periods of time and leading to a decrease in the transition metal surface coverage exposed to the gas phase. In this work, we use a combination of stable isotope tracer labeling and surface-sensitive ion beam techniques to study the oxygen transport properties and their relationship with the surface chemistry in ordered LnBaCo2O(5+δ) perovskites. Time-of-Flight Secondary-Ion Mass Spectrometry (ToF-SIMS) combined with (18)O isotope exchange was used to determine the oxygen tracer diffusion (D*) and surface exchange (k*) coefficients. Furthermore, Low Energy Ion Scattering (LEIS) was used for the analysis of the surface and near surface chemistry as it provides information from the first mono-atomic layer of the materials. In this way, we could relate the compositional modifications (e.g. cation segregation) taking place at the electrochemically-active surface during the exchange at high temperatures and the oxygen transport properties in double perovskite electrode materials to further our understanding of the mechanism of the surface exchange process.

A lattice Boltzmann model for substrates with regularly structured surface roughness

Science.gov (United States)

Yagub, A.; Farhat, H.; Kondaraju, S.; Singh, T.

2015-11-01

Superhydrophobic surface characteristics are important in many industrial applications, ranging from the textile to the military. It was observed that surfaces fabricated with nano/micro roughness can manipulate the droplet contact angle, thus providing an opportunity to control the droplet wetting characteristics. The Shan and Chen (SC) lattice Boltzmann model (LBM) is a good numerical tool, which holds strong potentials to qualify for simulating droplets wettability. This is due to its realistic nature of droplet contact angle (CA) prediction on flat smooth surfaces. But SC-LBM was not able to replicate the CA on rough surfaces because it lacks a real representation of the physics at work under these conditions. By using a correction factor to influence the interfacial tension within the asperities, the physical forces acting on the droplet at its contact lines were mimicked. This approach allowed the model to replicate some experimentally confirmed Wenzel and Cassie wetting cases. Regular roughness structures with different spacing were used to validate the study using the classical Wenzel and Cassie equations. The present work highlights the strength and weakness of the SC model and attempts to qualitatively conform it to the fundamental physics, which causes a change in the droplet apparent contact angle, when placed on nano/micro structured surfaces.

Oxygen adsorption on the Al9Co2(001) surface: first-principles and STM study

International Nuclear Information System (INIS)

Villaseca, S Alarcón; Loli, L N Serkovic; Ledieu, J; Fournée, V; Dubois, J-M; Gaudry, É; Gille, P

2013-01-01

Atomic oxygen adsorption on a pure aluminum terminated Al 9 Co 2 (001) surface is studied by first-principle calculations coupled with STM measurements. Relative adsorption energies of oxygen atoms have been calculated on different surface sites along with the associated STM images. The local electronic structure of the most favourable adsorption site is described. The preferential adsorption site is identified as a ‘bridge’ type site between the cluster entities exposed at the (001) surface termination. The Al–O bonding between the adsorbate and the substrate presents a covalent character, with s–p hybridization occurring between the states of the adsorbed oxygen atom and the aluminum atoms of the surface. The simulated STM image of the preferential adsorption site is in agreement with experimental observations. This work shows that oxygen adsorption generates important atomic relaxations of the topmost surface layer and that sub-surface cobalt atoms strongly influence the values of the adsorption energies. The calculated Al–O distances are in agreement with those reported in Al 2 O and Al 2 O 3 oxides and for oxygen adsorption on Al(111). (paper)

Adsorption of oxygen on low-index surfaces of the TiAl{sub 3} alloy

Energy Technology Data Exchange (ETDEWEB)

Latyshev, A. M.; Bakulin, A. V.; Kulkova, S. E., E-mail: kulkova@ms.tsc.ru [National Research Tomsk State University (Russian Federation); Hu, Q. M.; Yang, R. [Chinese Academy of Sciences, Shenyang National Laboratory for Materials Science, Institute of Metal Research (China)

2016-12-15

Method of the projector augmented waves in the plane-wave basis within the generalized-gradient approximation for the exchange-correlation functional has been used to study oxygen adsorption on (001), (100), and (110) low-index surfaces of the TiAl{sub 3} alloy. It has been established that the sites that are most energetically preferred for the adsorption of oxygen are hollow (H) positions on the (001) surface and bridge (B) positions on the (110) and (100) surfaces. Structural and electronic factors that define their energy preference have been discussed. Changes in the atomic and electronic structure of subsurface layers that occur as the oxygen concentration increases to three monolayers have been analyzed. It has been shown that the formation of chemical bonds of oxygen with both components of the alloy leads to the appearance of states that are split-off from the bottoms of their valence bands, which is accompanied by the formation of a forbidden gap at the Fermi level and by a weakening of the Ti–Al metallic bonds in the alloy. On the Al-terminated (001) and (110) surfaces, the oxidation of aluminum dominates over that of titanium. On the whole, the binding energy of oxygen on the low-index surfaces with a mixed termination is higher than that at the aluminum-terminated surface. The calculation of the diffusion of oxygen in the TiAl{sub 3} alloy has shown that the lowest barriers correspond to the diffusion between tetrahedral positions in the (001) plane; the diffusion of oxygen in the [001] direction occurs through octahedral and tetrahedral positions. An increase in the concentration of aluminum in the alloy favors a reduction in the height of the energy barriers as compared to the corresponding barriers in the γ-TiAl alloy.

The role of oxygen during the catalytic oxidation of ammonia on Co{sub 3}O{sub 4}(1 0 0)

Energy Technology Data Exchange (ETDEWEB)

Shojaee, Kambiz; Haynes, Brian S.; Montoya, Alejandro, E-mail: alejandro.montoya@sydney.edu.au

2014-10-15

Graphical abstract: - Highlights: • Ammonia oxidation on Co{sub 3}O{sub 4}(1 0 0) surface is studied using Density Functional Theory. • The role of lattice O, on-surface O and OH in the dehydrogenation of ammonia is clarified. • NO and H{sub 2}O are the main products of ammonia oxidation on Co{sub 3}O{sub 4}(1 0 0). • The Co{sub 3}O{sub 4} surface is itself capable of oxidising NH{sub 3} to NO using the lattice O, opening the way for a Mars–van Krevelen mechanism of reaction. - Abstract: The adsorption selectivity and dehydrogenation energy barriers of NH{sub 3}, NH{sub 2} and NH on the (1 0 0) surface planes of Co{sub 3}O{sub 4} are determined by means of density functional methods. Stepwise hydrogen abstraction is effected by lattice O{sup 3o} associated with octahedrally coordinated surface Co atoms. The final H-abstraction, from NH, leads directly to the formation of gaseous product NO with the creation of a lattice oxygen vacancy. Reaction of this vacancy with gas-phase O{sub 2} repairs the vacancy and creates surface-adsorbed O{sup *} which is also capable of abstracting H from NH{sub 3}{sup *}, NH{sub 2}{sup *} and NH{sup *}, the final step leading to directly again to NO formation. The mobile surface OH{sup *} formed from the O{sup *}-mediated abstraction steps is also capable of abstracting H from the NH{sub x}{sup *} species, leading ultimately to surface N{sup *} which then easily extracts a lattice O{sup 3o} to form NO and a new vacancy. The overall mechanism to form NO is a complex cycle of lattice- and surface-mediated abstractions. The hydrogen budget in the reaction shows corresponding complexity. Surface H{sup *} (formed when lattice O{sup 3o} abstracts H from NH{sub x}) is stable and immobile but it can be abstracted by surface OH{sup *} to form water. OH{sup *} disproportionation reaction also forms water.

Solid Oxide Fuel Cell Cathodes. Unraveling the Relationship Between Structure, Surface Chemistry and Oxygen Reduction

Energy Technology Data Exchange (ETDEWEB)

Gopalan, Srikanth [Boston Univ., MA (United States)

2013-03-31

In this work we have considered oxygen reduction reaction on LSM and LSCF cathode materials. In particular we have used various spectroscopic techniques to explore the surface composition, transition metal oxidation state, and the bonding environment of oxygen to understand the changes that occur to the surface during the oxygen reduction process. In a parallel study we have employed patterned cathodes of both LSM and LSCF cathodes to extract transport and kinetic parameters associated with the oxygen reduction process.

Late Quaternary changes in surface productivity and oxygen ...

Indian Academy of Sciences (India)

Changes in the abundance of selected planktic foraminiferal species and some sedimentological parameters at ODP site 728A were examined to understand the fluctuations in the surface productivity and deep sea oxygenation in the NW Arabian Sea during last ∼540 kyr. The increased relative abundances of high fertility ...

Electrical property studies of oxygen in Czochralski-grown neutron-transmutation-doped silicon

International Nuclear Information System (INIS)

Cleland, J.W.; Fukuoka, N.

1980-10-01

Electically active oxygen-related donors can be formed in Czochralski (Cz) Si either during crystal growth or during subsequent heat treatment; conventional n- or p-type dopant carrier concentrations are altered if these oxygen donors are present. Neutron transmutation doping (NTD) has been used to introduce a uniform concentration of 31 P in Si. However, oxygen donors can also be formed in NTD Cz Si during the process of annealing to remove NTD radiation damage. In the present experiments, the carrier concentration of Cz and NTD Cz Si samples was determined as a function of the initial dopant, oxygen, and 31 P concentration before and after isothermal or isochronal annealing. It is shown that low temperature (350 to 500 0 C) heat treatment can introduce a significant oxygen donor concentration in Cz Si and in NTD Cz Si that contains radiation-induced lattice defects. Intermediate temperature (550 to 750 0 C) heat treatment, which is intended to remove oxygen donors or lattice defects, can introduce other oxygen donors; annealing above 750 0 C is required to remove any of these oxygen donors. Extended (20 h) high-temperature (1000 to 1200 0 C) annealing can remove oxygen donors and lattice defects, but a significant concentration of oxygen donors can still be introduced by subsequent low temperature heat treatment. These results suggest that oxygen-related donor formation in NTD Cz Si at temperatures below 750 0 C may serve to mask any annealing study of lattice defects. It is concluded that annealing for 30 min at 750 0 C is sufficient to remove radiation damage in NTD Cz Si when the separate effects of oxygen donor formation are included

Elastic lattice in an incommensurate background

International Nuclear Information System (INIS)

Dickman, R.; Chudnovsky, E.M.

1995-01-01

We study a harmonic triangular lattice, which relaxes in the presence of an incommensurate short-wavelength potential. Monte Carlo simulations reveal that the elastic lattice exhibits only short-ranged translational correlations, despite the absence of defects in either lattice. Extended orientational order, however, persists in the presence of the background. Translational correlation lengths exhibit approximate power-law dependence upon cooling rate and background strength. Our results may be relevant to Wigner crystals, atomic monolayers on crystals surfaces, and flux-line and magnetic bubble lattices

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

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

Axisymmetric Lattice Boltzmann Model of Droplet Impact on Solid Surfaces

Science.gov (United States)

Dalgamoni, Hussein; Yong, Xin

2017-11-01

Droplet impact is a ubiquitous fluid phenomena encountered in scientific and engineering applications such as ink-jet printing, coating, electronics manufacturing, and many others. It is of great technological importance to understand the detailed dynamics of drop impact on various surfaces. The lattice Boltzmann method (LBM) emerges as an efficient method for modeling complex fluid systems involving rapidly evolving fluid-fluid and fluid-solid interfaces with complex geometries. In this work, we model droplet impact on flat solid substrates with well-defined wetting behavior using a two-phase axisymmetric LBM with high density and viscosity contrasts. We extend the two-dimensional Lee and Liu model to capture axisymmetric effect in the normal impact. First we compare the 2D axisymmetric results with the 2D and 3D results reported by Lee and Liu to probe the effect of axisymmetric terms. Then, we explore the effects of Weber number, Ohnesorge number, and droplet-surface equilibrium contact angle on the impact. The dynamic contact angle and spreading factor of the droplet during impact are investigated to qualitatively characterize the impact dynamics.

Surface characterization of the chitosan membrane after oxygen plasma treatment and its aging effect

International Nuclear Information System (INIS)

Wang Yingjun; Yin Shiheng; Ren Li; Zhao Lianna

2009-01-01

Chitosan has received considerable attention for biomedical applications in recent years because of its biocompatibility and biodegradability. In this paper, angle-resolved x-ray photoelectron spectroscopy (ARXPS) was carried out to investigate the chemical groups' spatial orientation on the chitosan membrane surface. Oxygen plasma treatment was also employed to improve the surface hydrophilicity of the chitosan membrane. The results of ARXPS revealed the distribution of surface polar groups, such as-OH and O=CNH 2 toward the membrane bulk, which was the origin of the chitosan membrane surface hydrophobicity. The contact angle measurements and XPS results indicated that oxygen plasma treatment can markedly improve the surface hydrophilicity and surface energy of the chitosan membrane by incorporating oxygen-containing polar groups. With the existence of the aging process, the influence of plasma treatment was not permanent, it faded with storage time. The ARXPS result discovered that the reorientation of polar functional groups generated by plasma treatment toward the membrane bulk was primarily responsible for the aging effect.

DFT study of oxygen adsorption on Mo{sub 2}C(001) and (201) surfaces at different conditions

Energy Technology Data Exchange (ETDEWEB)

Cheng, Lihong, E-mail: chenglihong001@126.com [School of Materials and Mechanical & Electrical Engineering, Jiangxi Science and Technology Normal University, Nanchang 330013, Jiangxi (China); Li, Wenkui; Chen, Zhiqin; Ai, Jianping; Zhou, Zehua [School of Materials and Mechanical & Electrical Engineering, Jiangxi Science and Technology Normal University, Nanchang 330013, Jiangxi (China); Liu, Jianwen, E-mail: liujw@nsccsz.gov.cn [National Supercomputing Center in Shenzhen, Shenzhen 518055 (China)

2017-07-31

Highlights: • O adsorption manners on Mo{sub 2}C surfaces were calculated by DFT method. • Stable oxygen adsorption states and coverage were identified at given T and p. • O{sub 2} results in full oxidation while H{sub 2}O and CO{sub 2} cause partial oxidation of Mo{sub 2}C surfaces. • Hydrogen could be used to avoid Mo{sub 2}C surface oxidation. - Abstract: Density functional theory (DFT) calculations were performed to investigate oxygen adsorption on Mo{sub 2}C(001) and (201)surfaces at different coverage. The energies and structures of oxygen from lowest to saturated coverages were clearly identified on each surface. Thermodynamics method was introduced to reveal the roles of temperature, pressure as well as oxygen sources (O{sub 2}, H{sub 2}O and CO{sub 2}) on the surface oxygen coverage, which is related to the surface oxidation. On the basis of phase diagram, we can easily identify the stable oxygen coverage at different defined conditions. In addition, it reveals that O{sub 2} is the strongest oxidant, which results in the full coverage of oxygen on both surfaces in a wide range of temperature and pressure. Then, H{sub 2}O and CO{sub 2} are weaker oxidants, which could only cause partial oxidation of Mo{sub 2}C surfaces. These results indicate the facile oxidation of Mo{sub 2}C catalyst. The possible ways to avoid surface oxidation are keeping higher temperature and H{sub 2} pressure in the gas phase.

Probing adsorption phenomena on a single crystal Pt-alloy surface under oxygen reduction reaction conditions

International Nuclear Information System (INIS)

Bondarenko, Alexander S.; Stephens, Ifan E.L.; Bech, Lone; Chorkendorff, Ib

2012-01-01

Highlights: ► Impedance spectroscopy of Cu/Pt(1 1 1) near-surface alloy and Pt(1 1 1). ► Presence of oxygen changes little the adsorption dynamics. ► Adsorption dynamics similar on alloy and Pt(1 1 1). ► Electrosorption phenomena on alloy shifted in potential, relative to Pt(1 1 1). - Abstract: The adsorption dynamics of *OH and *O species at Pt(1 1 1) and Cu/Pt(1 1 1) near-surface alloy (NSA) surfaces in oxygen-free and O 2 -saturated 0.1 M HClO 4 was investigated. Subsurface Cu modifies the electronic structure at the Pt(1 1 1) surface resulting in weaker bonding to adsorbates like *OH, *H or *O. This provides a basis for the high oxygen reduction activity of the NSA, as predicted by density functional theory calculations. The shift in *OH adsorption of around 0.16 V towards more positive potentials can be clearly monitored in absence of O 2 and under the oxygen reduction reaction (ORR) conditions for the Cu/Pt(1 1 1) NSA. In both cases, for Pt(1 1 1) and NSA, the *OH(*O) adsorption dynamics is very similar in the absence of oxygen and under ORR conditions. Therefore, theoretical assumptions about the coverage of adsorbates in the absence of oxygen can be reasonably extrapolated to the situation when oxygen reduction takes place at the surface. A ∼5-fold improvement in the ORR activity over the Pt(1 1 1) at 0.9 V (RHE) was measured for the Cu/Pt(1 1 1) near-surface alloy.

Understanding the influence of surface chemical states on the dielectric tunability of sputtered Ba0.5Sr0.5TiO3 thin films

International Nuclear Information System (INIS)

Venkata Saravanan, K; James Raju, K C

2014-01-01

The surface chemical states of RF-magnetron sputtered Ba 0.5 Sr 0.5 TiO 3 (BST5) thin films deposited at different oxygen mixing percentage (OMP) was examined by x-ray photoelectron spectroscopy. The O1s XPS spectra indicate the existence of three kinds of oxygen species (dissociated oxygen ion O 2 − , adsorbed oxide ion O − and lattice oxide ion O 2− ) on the films’ surface, which strongly depends on OMP. The presence of oxygen species other than lattice oxygen ion makes the films’ surface highly reactivity to atmospheric gases, resulting in the formation of undesired surface layers. The XPS results confirm the formation of surface nitrates for the films deposited under oxygen deficient atmosphere (OMP not ≦ 25%), whereas the films deposited in oxygen rich atmosphere (OMP not ≧ 75%) show the presence of metal-hydroxide. The influence of a surface dead layer on the tunable dielectric properties of BST5 films have been studied in detail and are reported. Furthermore, our observations indicate that an optimum ratio of Ar:O 2 is essential for achieving desired material and dielectric properties in BST5 thin films. The films deposited at 50% OMP have the highest dielectric tunability of ∼65% (@280 kV cm −1 ), with good ϵ r -E curve symmetry of 98% and low tan δ of 0.018. The figure of merit for these films is about 35, which is promising for frequency agile device applications. (papers)

Chemistry of SOFC Cathode Surfaces: Fundamental Investigation and Tailoring of Electronic Behavior

Energy Technology Data Exchange (ETDEWEB)

Yildiz, Bilge; Heski, Clemens

2013-08-31

1) Electron tunneling characteristics on La0.7Sr0.3MnO3 (LSM) thin-film surfaces were studied up to 580oC in 10-3mbar oxygen pressure, using scanning tunneling microscopy/ spectroscopy (STM/STS). A threshold-like drop in the tunneling current was observed at positive bias in STS, which is interpreted as a unique indicator for the activation polarization in cation oxygen bonding on LSM cathodes. Sr-enrichment was found on the surface at high temperature using Auger electron spectroscopy, and was accompanied by a decrease in tunneling conductance in STS. This suggests that Sr-terminated surfaces are less active for electron transfer in oxygen reduction compared to Mn-terminated surfaces on LSM. 2) Effects of strain on the surface cation chemistry and the electronic structure are important to understand and control for attaining fast oxygen reduction kinetics on transition metal oxides. Here, we demonstrate and mechanistically interpret the strain coupling to Sr segregation, oxygen vacancy formation, and electronic structure on the surface of La0.7Sr0.3MnO3 (LSM) thin films as a model system. Our experimental results from x-ray photoelectron spectroscopy and scanning tunneling spectroscopy are discussed in light of our first principles-based calculations. A stronger Sr enrichment tendency and a more facile oxygen vacancy formation prevail for the tensile strained LSM surface. The electronic structure of the tensile strained LSM surface exhibits a larger band gap at room temperature, however, a higher tunneling conductance near the Fermi level than the compressively strained LSM at elevated temperatures in oxygen. Our findings suggest lattice strain as a key parameter to tune the reactivity of perovskite transition metal oxides with oxygen in solid oxide fuel cell cathodes. 3) Cation segregation on perovskite oxide surfaces affects vastly the oxygen reduction activity and stability of solid oxide fuel cell (SOFC) cathodes. A unified theory that explains the physical

Crystal structure and surface characteristics of Sr-doped GdBaCo2O6−δ double perovskites: oxygen evolution reaction and conductivity

KAUST Repository

Pramana, Stevin S.

2017-12-04

A cheap and direct solution towards engineering better catalysts through identification of novel materials is required for a sustainable energy system. Perovskite oxides have emerged as potential candidates to replace the less economically attractive Pt and IrO2 water splitting catalysts. In this work, excellent electrical conductivity (980 S cm−1) was found for the double perovskite of composition GdBa0.6Sr0.4Co2O6−δ which is consistent with a better oxygen evolution reaction activity with the onset polarisation of 1.51 V with respect to a reversible hydrogen electrode (RHE). GdBa1−xSrxCo2O6−δ with increasing Sr content was found to crystallise in the higher symmetry tetragonal P4/mmm space group in comparison with the undoped GdBaCo2O6−δ which is orthorhombic (Pmmm), and yields higher oxygen uptake, accompanied by higher Co oxidation states. This outstanding electrochemical performance is explained by the wider carrier bandwidth, which is a function of Co–O–Co buckling angles and Co–O bond lengths. Furthermore the higher oxygen evolution activity was observed despite the formation of non-lattice oxides (mainly hydroxide species) and enrichment of alkaline earth ions on the surface.

Crystal structure and surface characteristics of Sr-doped GdBaCo2O6−δ double perovskites: oxygen evolution reaction and conductivity

KAUST Repository

Pramana, Stevin S.; Cavallaro, Andrea; Li, Cheng; Handoko, Albertus D.; Chan, Kuang Wen; Walker, Robert J.; Regoutz, Anna; Herrin, Jason S.; Yeo, Boon Siang; Payne, David J.; Kilner, John A.; Ryan, Mary P.; Skinner, Stephen J.

2017-01-01

A cheap and direct solution towards engineering better catalysts through identification of novel materials is required for a sustainable energy system. Perovskite oxides have emerged as potential candidates to replace the less economically attractive Pt and IrO2 water splitting catalysts. In this work, excellent electrical conductivity (980 S cm−1) was found for the double perovskite of composition GdBa0.6Sr0.4Co2O6−δ which is consistent with a better oxygen evolution reaction activity with the onset polarisation of 1.51 V with respect to a reversible hydrogen electrode (RHE). GdBa1−xSrxCo2O6−δ with increasing Sr content was found to crystallise in the higher symmetry tetragonal P4/mmm space group in comparison with the undoped GdBaCo2O6−δ which is orthorhombic (Pmmm), and yields higher oxygen uptake, accompanied by higher Co oxidation states. This outstanding electrochemical performance is explained by the wider carrier bandwidth, which is a function of Co–O–Co buckling angles and Co–O bond lengths. Furthermore the higher oxygen evolution activity was observed despite the formation of non-lattice oxides (mainly hydroxide species) and enrichment of alkaline earth ions on the surface.

Surface and Core Electronic Structure of Oxidized Silicon Nanocrystals

Directory of Open Access Journals (Sweden)

Noor A. Nama

2010-01-01

Full Text Available Ab initio restricted Hartree-Fock method within the framework of large unit cell formalism is used to simulate silicon nanocrystals between 216 and 1000 atoms (1.6–2.65 nm in diameter that include Bravais and primitive cell multiples. The investigated properties include core and oxidized surface properties. Results revealed that electronic properties converge to some limit as the size of the nanocrystal increases. Increasing the size of the core of a nanocrystal resulted in an increase of the energy gap, valence band width, and cohesive energy. The lattice constant of the core and oxidized surface parts shows a decreasing trend as the nanocrystal increases in a size that converges to 5.28 Ǻ in a good agreement with the experiment. Surface and core convergence to the same lattice constant reflects good adherence of oxide layer at the surface. The core density of states shows highly degenerate states that split at the oxygenated (001-(1×1 surface due to symmetry breaking. The nanocrystal surface shows smaller gap and higher valence and conduction bands when compared to the core part, due to oxygen surface atoms and reduced structural symmetry. The smaller surface energy gap shows that energy gap of the nanocrystal is controlled by the surface part. Unlike the core part, the surface part shows a descending energy gap that proves its obedience to quantum confinement effects. Nanocrystal geometry proved to have some influence on all electronic properties including the energy gap.

Effective Wettability of Heterogenous Fracture Surfaces Using the Lattice-Boltzmann Method

Science.gov (United States)

E Santos, J.; Prodanovic, M.; Landry, C. J.

2017-12-01

Fracture walls in the subsurface are often structured by minerals of different composition (potentially further altered in contact with fluids during hydrocarbon extraction or CO2 sequestration), this yields in a heterogeneous wettability of the surface in contact with the fluids. The focus of our work is to study how surfaces presenting different mineralogy and roughness affect multiphase flow in fractures. Using the Shan-Chen model of the lattice-Boltzmann method (LBM) we define fluid interaction and surface attraction parameters to simulate a system of a wetting and a non-wetting fluid. In this work, we use synthetically created fractures presenting different arrangements of wetting and non-wetting patches, and with or without roughness; representative of different mineralogy, similar workflow can be applied to fractures extracted from X-ray microtomography images of fractures porous media. The results from the LBM simulations provide an insight on how the distribution of mineralogy and surface roughness are related with the observed macroscopic contact angle. We present a comparison between the published analytical models, and our results based on surface areas, spatial distribution and local fracture aperture. The understanding of the variables that affect the contact angle is useful for the comprehension of multiphase processes in naturally fractured reservoirs like primary oil production, enhanced oil recovery and CO2 sequestration. The macroscopic contact angle analytical equations for heterogeneous surfaces with variable roughness are no longer valid in highly heterogeneous systems; we quantify the difference thus offering an alternative to analytical models.

First Principles Calculations of Oxygen Adsorption on the UN(001) Surface

International Nuclear Information System (INIS)

Zhukovskii, Yuri F.; Bocharov, Dmitry; Kotomin, Eugene Alexej; Evarestov, Robert; Bandura, A.V.

2009-01-01

Fabrication, handling and disposal of nuclear fuel materials require comprehensive knowledge of their surface morphology and reactivity. Due to unavoidable contact with air components (even at low partial pressures), UN samples contain considerable amount of oxygen impurities affecting fuel properties. In this study we focus on reactivity of the energetically most stable (001) substrate of uranium nitride towards the atomic oxygen as one of initial stages for further UN oxidation. The basic properties of O atoms adsorbed on the UN(001) surface are simulated here combining the two first principles calculation methods based on the plane wave basis set and that of the localized orbitals.

Charge-lattice interplay in layered cobaltates RBaCo2O5+x

Science.gov (United States)

Lavrov, A. N.; Kameneva, M. Yu.; Kozeeva, L. P.; Zhdanov, K. R.

2017-10-01

X-ray diffraction, electrical resistivity and thermal expansion measurements are used to study the interrelation between the structural, magnetic and electron-transport peculiarities in RBaCo2O5+x (R=Y, Gd) over a wide range of oxygen contents. We find that the anisotropic lattice strain caused by the oxygen chain ordering in these compounds favors the metallic state and is a necessary condition for the coupled insulator-to-metal and spin-state phase transitions to occur. The obtained data point to the key role of the crystal lattice in selecting the preferred spin and orbital states of cobalt ions.

The effect of plutonium dioxide water surface coverage on the generation of hydrogen and oxygen

Energy Technology Data Exchange (ETDEWEB)

Veirs, Douglas K. [Los Alamos National Laboratory; Berg, John M. [Los Alamos National Laboratory; Crowder, Mark L. [Savannah River National Laboratory

2012-06-20

The conditions for the production of oxygen during radiolysis of water adsorbed onto plutonium dioxide powder are discussed. Studies in the literature investigating the radiolysis of water show that both oxygen and hydrogen can be generated from water adsorbed on high-purity plutonium dioxide powder. These studies indicate that there is a threshold in the amount of water below which oxygen is not generated. The threshold is associated with the number of monolayers of adsorbed water and is shown to occur at approximately two monolayers of molecularly adsorbed water. Material in equilibrium with 50% relative humidity (RH) will be at the threshold for oxygen generation. Using two monolayers of molecularly adsorbed water as the threshold for oxygen production, the total pressure under various conditions is calculated assuming stoichiometric production of hydrogen and oxygen. The specific surface area of the oxide has a strong effect on the final partial pressure. The specific surface areas resulting in the highest pressures within a 3013 container are evaluated. The potential for oxygen generation is mitigated by reduced relative humidity, and hence moisture adsorption, at the oxide surface which occurs if the oxide is warmer than the ambient air. The potential for oxygen generation approaches zero as the temperature difference between the ambient air and the material approaches 6 C.

Surface activation of cyclo olefin polymer by oxygen plasma discharge: a molecular dynamics study

International Nuclear Information System (INIS)

Soberon, Felipe

2014-01-01

Thermoplastic substrates made of cyclo olefin polymer (COP) are treated with oxygen plasma discharges to introduce polar groups at the surface. This is the first step in the process of surface functionalization of COP substrates used in biosensor devices. A molecular dynamics model of basic COP structure is implemented using the second-generation reactive empirical bond order (REBO) potentials for hydrocarbon–oxygen interactions. The model includes covalent bond and Van der Waals interactions. The bombardment of a COP surface with mono-energetic atomic oxygen ions, energy in the range 1-35 eV, is simulated and reported here. The dynamics of the substrate modification reveals that the substrate top layer is de-hydrogenated and subsequently builds up an oxygen–carbon matrix layer, ∼10 Å thick. Analysis of the modified substrates indicates that surface yield is predominantly peroxide groups. (paper)

Surface modification of argon/oxygen plasma treated vulcanized ethylene propylene diene polymethylene surfaces for improved adhesion with natural rubber

International Nuclear Information System (INIS)

Basak, Ganesh C.; Bandyopadhyay, Abhijit; Neogi, Sudarsan; Bhowmick, Anil K.

2011-01-01

Vulcanized ethylene propylene diene polymethylene (EPDM) rubber surface was treated in a radio frequency capacitatively coupled low pressure argon/oxygen plasma to improve adhesion with compounded natural rubber (NR) during co-vulcanization. The plasma modified surfaces were analyzed by means of contact angle measurement, surface energy, attenuated total reflection-infrared spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy, energy dispersive X-ray sulfur mapping and atomic force microscopy. Several experimental variables such as plasma power, length of exposure time and composition of the argon-oxygen gas mixture were considered. It was delineated that plasma treatment changed both surface composition and roughness, and consequently increased peel strength. The change in surface composition was mainly ascribed to the formation of C-O and -C=O functional groups on the vulcanized surfaces. A maximum of 98% improvement in peel strength was observed after plasma treatment.

Surface modification of argon/oxygen plasma treated vulcanized ethylene propylene diene polymethylene surfaces for improved adhesion with natural rubber

Energy Technology Data Exchange (ETDEWEB)

Basak, Ganesh C. [Rubber Technology Centre, Indian Institute of Technology, Kharagpur 721302 (India); Bandyopadhyay, Abhijit [Department of Polymer Science and Technology, University of Calcutta, Calcutta 700 009 (India); Neogi, Sudarsan [Department of Chemical Engineering, Indian Institute of Technology, Kharagpur 721302 (India); Bhowmick, Anil K., E-mail: anilkb@rtc.iitkgp.ernet.in [Rubber Technology Centre, Indian Institute of Technology, Kharagpur 721302 (India)

2011-01-15

Vulcanized ethylene propylene diene polymethylene (EPDM) rubber surface was treated in a radio frequency capacitatively coupled low pressure argon/oxygen plasma to improve adhesion with compounded natural rubber (NR) during co-vulcanization. The plasma modified surfaces were analyzed by means of contact angle measurement, surface energy, attenuated total reflection-infrared spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy, energy dispersive X-ray sulfur mapping and atomic force microscopy. Several experimental variables such as plasma power, length of exposure time and composition of the argon-oxygen gas mixture were considered. It was delineated that plasma treatment changed both surface composition and roughness, and consequently increased peel strength. The change in surface composition was mainly ascribed to the formation of C-O and -C=O functional groups on the vulcanized surfaces. A maximum of 98% improvement in peel strength was observed after plasma treatment.

[Distribution and sources of oxygen and sulfur heterocyclic aromatic compounds in surface soil of Beijing, China].

Science.gov (United States)

He, Guang-Xiu; Zhang, Zhi-Huan; Peng, Xu-Yang; Zhu, Lei; Lu, Ling

2011-11-01

62 surface soil samples were collected from different environmental function zones in Beijing. Sulfur and oxygen heterocyclic aromatic compounds were detected by GC/MS. The objectives of this study were to identify the composition and distribution of these compounds, and discuss their sources. The results showed that the oxygen and sulfur heterocyclic aromatic compounds in the surface soils mainly contained dibenzofuran, methyl- and C2-dibenzofuran series, dibenzothiophene, methyl-, C2- and C3-dibenzothiophene series and benzonaphthothiophene series. The composition and distribution of the oxygen and sulfur heterocyclic aromatic compounds in the surface soil samples varied in the different environmental function zones, of which some factories and the urban area received oxygen and sulfur heterocyclic aromatic compounds most seriously. In Beijing, the degree of contamination by oxygen and sulfur heterocyclic aromatic compounds in the north surface soil was higher than that in the south. There were preferable linear correlations between the concentration of dibenzofuran series and fluorene series, as well as the concentration of dibenzothiophene series and dibenzofuran series. The oxygen and sulfur heterocyclic aromatic compounds in the surface soil were mainly derived from combustion products of oil and coal and direct input of mineral oil, etc. There were some variations in pollution sources of different environmental function zones.

Probing adsorption phenomena on a single crystal Pt-alloy surface under oxygen reduction reaction conditions

DEFF Research Database (Denmark)

Bondarenko, Alexander S.; Stephens, Ifan E.L.; Bech, Lone

2012-01-01

The adsorption dynamics of *OH and *O species at Pt(111) and Cu/Pt(111) near-surface alloy (NSA) surfaces in oxygen-free and O2-saturated 0.1M HClO4 was investigated. Subsurface Cu modifies the electronic structure at the Pt(111) surface resulting in weaker bonding to adsorbates like *OH, *H or *O....... This provides a basis for the high oxygen reduction activity of the NSA, as predicted by density functional theory calculations. The shift in *OH adsorption of around 0.16V towards more positive potentials can be clearly monitored in absence of O2 and under the oxygen reduction reaction (ORR) conditions...... for the Cu/Pt(111) NSA. In both cases, for Pt(111) and NSA, the *OH(*O) adsorption dynamics is very similar in the absence of oxygen and under ORR conditions. Therefore, theoretical assumptions about the coverage of adsorbates in the absence of oxygen can be reasonably extrapolated to the situation when...

SPE (tm) regenerative hydrogen/oxygen fuel cells for extraterrestrial surface and microgravity applications

Science.gov (United States)

Mcelroy, J. F.

1990-01-01

Viewgraphs on SPE regenerative hydrogen/oxygen fuel cells for extraterrestrial surface and microgravity applications are presented. Topics covered include: hydrogen-oxygen regenerative fuel cell energy storage system; electrochemical cell reactions; SPE cell voltage stability; passive water removal SPE fuel cell; fuel cell performance; SPE water electrolyzers; hydrophobic oxygen phase separator; hydrophilic/electrochemical hydrogen phase separator; and unitized regenerative fuel cell.

Plasma-polymerized SiOx deposition on polymer film surfaces for preparation of oxygen gas barrier polymeric films

International Nuclear Information System (INIS)

Inagaki, N.

2003-01-01

SiOx films were deposited on surfaces of three polymeric films, PET, PP, and Nylon; and their oxygen gas barrier properties were evaluated. To mitigate discrepancies between the deposited SiOx and polymer film, surface modification of polymer films was done, and how the surface modification could contribute to was discussed from the viewpoint of apparent activation energy for the permeation process. The SiOx deposition on the polymer film surfaces led to a large decrease in the oxygen permeation rate. Modification of polymer film surfaces by mans of the TMOS or Si-COOH coupling treatment in prior to the SiOx deposition was effective in decreasing the oxygen permeation rate. The cavity model is proposed as an oxygen permeation process through the SiOx-deposited Nylon film. From the proposed model, controlling the interface between the deposited SiOx film and the polymer film is emphasized to be a key factor to prepare SiOx-deposited polymer films with good oxygen gas barrier properties. (author)

Synthesis of surface oxygen-deficient BiPO{sub 4} nanocubes with enhanced visible light induced photocatalytic activity

Energy Technology Data Exchange (ETDEWEB)

Shi, Bingtao; Yin, Haoyong; Li, Tao; Gong, Jianying; Lv, Shumei; Nie, Qiulin, E-mail: yhy@hdu.edu.cn [College of Materials & Environmental Engineering, Hangzhou Dianzi University, Hangzhou (China)

2017-05-15

The visible light driven BiPO{sub 4} nanocubes with sufficient surface oxygen deficiency were fabricated by a hydrothermal process and subsequently ultrasonic assistant Fe reduction process. The products were characterized by XRD, DRS, XPS, SEM and TEM which showed that the BiPO{sub 4} had cuboid-like shape with a smooth surface and clear edges and the oxygen vacancies were successfully introduced on the surface of the BiPO{sub 4} nanocubes. The as prepared oxygen-deficient BiPO{sub 4} nanocubes showed greatly enhanced visible light induced photocatalytic activity in degradation of Rhodamine B. The enhanced photocatalytic performance and expanded visible light response of BiPO{sub 4} may be due to the introduction of surface oxygen vacancies which can generate the oxygen vacancies mid-gap states lower to the conduction band of BiPO{sub 4}. (author)

Oxygen Evolution at Hematite Surfaces: The Impact of Structure and Oxygen Vacancies on Lowering the Overpotential

NARCIS (Netherlands)

Zhang, X.; Klaver, P.; van Santen, R.; van de Sanden, M. C. M.; Bieberle, A.

2016-01-01

Simulations of the oxygen evolution reaction (OER) are essential for understanding the limitations of water splitting. Most research has focused so far on the OER at flat metal oxide surfaces. The structure sensitivity of the OER has, however, recently been highlighted as a promising research

Oxygen Modulates Human Decidual Natural Killer Cell Surface Receptor Expression and Interactions with Trophoblasts1

Science.gov (United States)

Wallace, Alison E.; Goulwara, Sonu S.; Whitley, Guy S.; Cartwright, Judith E.

2014-01-01

Decidual natural killer (dNK) cells have been shown to both promote and inhibit trophoblast behavior important for decidual remodeling in pregnancy and have a distinct phenotype compared to peripheral blood NK cells. We investigated whether different levels of oxygen tension, mimicking the physiological conditions of the decidua in early pregnancy, altered cell surface receptor expression and activity of dNK cells and their interactions with trophoblast. dNK cells were isolated from terminated first-trimester pregnancies and cultured in oxygen tensions of 3%, 10%, and 21% for 24 h. Cell surface receptor expression was examined by flow cytometry, and the effects of secreted factors in conditioned medium (CM) on the trophoblast cell line SGHPL-4 were assessed in vitro. SGHPL-4 cells treated with dNK cell CM incubated in oxygen tensions of 10% were significantly more invasive (P cells treated with dNK cell CM incubated in oxygen tensions of 3% or 21%. After 24 h, a lower percentage of dNK cells expressed CD56 at 21% oxygen (P cells expressed NKG2D at 10% oxygen (P oxygen tensions, with large patient variation. This study demonstrates dNK cell phenotype and secreted factors are modulated by oxygen tension, which induces changes in trophoblast invasion and endovascular-like differentiation. Alterations in dNK cell surface receptor expression and secreted factors at different oxygen tensions may represent regulation of function within the decidua during the first trimester of pregnancy. PMID:25232021

Modeling the thermostability of surface functionalisation by oxygen, hydroxyl, and water on nanodiamonds.

Science.gov (United States)

Lai, Lin; Barnard, Amanda S

2011-06-01

Understanding nanodiamond functionalisation is of great importance for biological and medical applications. Here we examine the stabilities of oxygen, hydroxyl, and water functionalisation of the nanodiamonds using the self-consistent charge density functional tight-binding simulations. We find that the oxygen and hydroxyl termination are thermodynamically favourable and form strong C–O covalent bonds on the nanodiamond surface in an O2 and H2 gas reservoir, which confirms previous experiments. Yet, the thermodynamic stabilities of oxygen and hydroxyl functionalisation decrease dramatically in a water vapour reservoir. In contrast, H2O molecules are found to be physically adsorbed on the nanodiamond surface, and forced chemical adsorption results in decomposition of H2O. Moreover, the functionalisation efficiency is found to be facet dependent. The oxygen functionalisation prefers the {100} facets as opposed to alternative facets in an O2 and H2 gas reservoir. The hydroxyl functionalisation favors the {111} surfaces in an O2 and H2 reservoir and the {100} facets in a water vapour reservoir, respectively. This facet selectivity is found to be largely dependent upon the environmental temperature, chemical reservoir, and morphology of the nanodiamonds.

Ultrafast electron, lattice and spin dynamics on rare earth metal surfaces. Investigated with linear and nonlinear optical techniques

Energy Technology Data Exchange (ETDEWEB)

Radu, I.E.

2006-03-15

This thesis presents the femtosecond laser-induced electron, lattice and spin dynamics on two representative rare-earth systems: The ferromagnetic gadolinium Gd(0001) and the paramagnetic yttrium Y(0001) metals. The employed investigation tools are the time-resolved linear reflectivity and second-harmonic generation, which provide complementary information about the bulk and surface/interface dynamics, respectively. The femtosecond laser excitation of the exchange-split surface state of Gd(0001) triggers simultaneously the coherent vibrational dynamics of the lattice and spin subsystems in the surface region at a frequency of 3 THz. The coherent optical phonon corresponds to the vibration of the topmost atomic layer against the underlying bulk along the normal direction to the surface. The coupling mechanism between phonons and magnons is attributed to the modulation of the exchange interaction J between neighbour atoms due to the coherent lattice vibration. This leads to an oscillatory motion of the magnetic moments having the same frequency as the lattice vibration. Thus these results reveal a new type of phonon-magnon coupling mediated by the modulation of the exchange interaction and not by the conventional spin-orbit interaction. Moreover, we show that coherent spin dynamics in the THz frequency domain is achievable, which is at least one order of magnitude faster than previously reported. The laser-induced (de)magnetization dynamics of the ferromagnetic Gd(0001) thin films have been studied. Upon photo-excitation, the nonlinear magneto-optics measurements performed in this work show a sudden drop in the spin polarization of the surface state by more than 50% in a <100 fs time interval. Under comparable experimental conditions, the time-resolved photoemission studies reveal a constant exchange splitting of the surface state. The ultrafast decrease of spin polarization can be explained by the quasi-elastic spin-flip scattering of the hot electrons among spin

Diffraction experiments of argon or helium on polluted surfaces

International Nuclear Information System (INIS)

Berthier, J.P.; Constans, A.; Daury, G.; Lostis, P.

1975-01-01

Scattering patterns of molecular beams of argon or helium from metal surfaces (bulk metal or thin films) are reported. The pressure in the scattering chamber is about 10 -6 torr. So, the surfaces are polluted. Diffraction peaks are observed which can be interpreted very well by assuming that nitrogen, oxygen or carbon atoms are adsorbed of the surface. On the other hand, diffraction peaks from a silicon crystal have been observed which can be reproduced very well by using silicon crystal lattice. These experiments are not interpreted accurately, but show that molecular reflection can be used for some surface studies [fr

Enhancing oxygen transport through Mixed-Ionic-and-Electronic-Conducting ceramic membranes

Science.gov (United States)

Yu, Anthony S.

Ceramic membranes based on Mixed-Ionic-and-Electronic-Conducting (MIEC) oxides are capable of separating oxygen from air in the presence of an oxygen partial-pressure gradient. These MIEC membranes show great promise for oxygen consuming industrial processes, such as the production of syngas from steam reforming of natural gas (SRM), as well as for electricity generation in Solid Oxide Fuel Cells (SOFC). For both applications, the overall performance is dictated by the rate of oxygen transport across the membrane. Oxygen transport across MIEC membranes is composed of a bulk oxygen-ion diffusion process and surface processes, such as surface reactions and adsorption/desorption of gaseous reactants/products. The main goal of this thesis was to determine which process is rate-limiting in order to significantly enhance the overall rate of oxygen transport in MIEC membrane systems. The rate-limiting step was determined by evaluating the total resistance to oxygen transfer, Rtot. Rtot is the sum of a bulk diffusion resistance in the membrane itself, Rb, and interfacial loss components, Rs. Rb is a function of the membrane's ionic conductivity and thickness, while Rs arises primarily from slow surface-exchange kinetics that cause the P(O2) at the surfaces of the membrane to differ from the P(O 2) in the adjacent gas phases. Rtot can be calculated from the Nernst potential across the membrane and the measured oxygen flux. The rate-limiting process can be determined by evaluating the relative contributions of the various losses, Rs and Rb, to Rtot. Using this method, this thesis demonstrates that for most membrane systems, Rs is the dominating factor. In the development of membrane systems with high oxygen transport rates, thin membranes with high ionic conductivities are required to achieve fast bulk oxygen-ion diffusion. However, as membrane thickness is decreased, surface reaction kinetics become more important in determining the overall transport rate. The two

Determination of Oxygen in Zircaloy Surfaces by Means of Charged Particle Activation Analysis

Energy Technology Data Exchange (ETDEWEB)

Lorenzen, J; Brune, D

1973-01-15

Oxygen in zircaloy surfaces has been determined by means of charged particle activation analysis employing the following two reactions I. 16O (d, n) 17F ->(beta+decay) 17O Q = - 1.63 MeV; II. 16O (d, pgamma) 17O Q = + 1.05 MeV. The detection limits for oxygen in such surfaces has been investigated by measuring the promptly emitted 0.87 MeV gamma rays (reaction II) and also the 511 keV annihilation radiation which arises from beta-decay of 17F (reaction I). The correlation between the detection limit for oxygen in zircaloy, the particle energy and the surface thickness analyzed has been evaluated. At a deuteron energy of 3 MeV a detection limit of 0.7 x 10-7 g/cm2 was obtained from the measurement of the prompt gamma radiation arising from the second of these reactions. The analysis carried out by means of this technique is characterized by a high rapidity

A miniaturized oxygen sensor integrated on fiber surface based on evanescent-wave induced fluorescence quenching

Energy Technology Data Exchange (ETDEWEB)

Xiong, Yan [School of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500 (China); Oil and Gas Field Applied Chemistry Key Laboratory of Sichuan Province, Southwest Petroleum University, Chengdu, 610500 (China); Tan, Jun; Wang, Chengjie; Zhu, Ying [School of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500 (China); Fang, Shenwen [School of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500 (China); Oil and Gas Field Applied Chemistry Key Laboratory of Sichuan Province, Southwest Petroleum University, Chengdu, 610500 (China); Wu, Jiayi; Wang, Qing [School of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500 (China); Duan, Ming, E-mail: swpua124@126.com [State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu 610500 (China); School of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500 (China); Oil and Gas Field Applied Chemistry Key Laboratory of Sichuan Province, Southwest Petroleum University, Chengdu, 610500 (China)

2016-11-15

In this work, a miniaturized sensor was integrated on fiber surface and developed for oxygen determination through evanescent-wave induced fluorescence quenching. The sensor was designed by using light emitting diode (LED) as light source and optical fiber as light transmission element. Tris(2,2′-bipyridyl) ruthenium ([Ru(bpy){sub 3}]{sup 2+}) fluorophore was immobilized in the organically modified silicates (ORMOSILs) film and coated onto the fiber surface. When light propagated by total internal reflection (TIR) in the fiber core, evanescent wave could be produced on the fiber surface and excite [Ru(bpy){sub 3}]{sup 2+} fluorophore to produce fluorescence emission. Then oxygen could be determinated by its quenching effect on the fluorescence and its concentration could be evaluated according to Stern–Volumer model. Through integrating evanescent wave excitation and fluorescence quenching on fiber surface, the sensor was successfully miniaturized and exhibit improved performances of high sensitivity (1.4), excellent repeatability (1.2%) and fast analysis (12 s) for oxygen determination. The sensor provided a newly portable method for in-situ and real-time measurement of oxygen and showed potential for practical oxygen analysis in different application fields. Furthermore, the fabrication of this sensor provides a miniaturized and portable detection platform for species monitoring by simple modular design. - Highlights: • ORMOSILs sensing film immobilized with [Ru(bpy){sub 3}]{sup 2+} fluorophore was coated on fiber surface. • Evanescent wave on the fiber surface was utilized as excitation source to produce fluorescence. • Oxygen was measured based on its quenching effect on evanescent wave-induce fluorescence. • Sensor fabrication was miniaturized by integrating detection and sensing elements on the fiber. • The modular design sensor provides a detection platform for other species monitoring.

Surface modification effects of fluorine-doped tin dioxide by oxygen plasma ion implantation

Science.gov (United States)

Tang, Peng; Liu, Cai; Zhang, Jingquan; Wu, Lili; Li, Wei; Feng, Lianghuan; Zeng, Guanggen; Wang, Wenwu

2018-04-01

SnO2:F (FTO), as a kind of transparent conductive oxide (TCO), exhibits excellent transmittance and conductivity and is widely used as transparency electrodes in solar cells. It's very important to modifying the surface of FTO for it plays a critical role in CdTe solar cells. In this study, modifying effects of oxygen plasma on FTO was investigated systematically. Oxygen plasma treatment on FTO surface with ion accelerating voltage ranged from 0.4 kV to 1.6 kV has been processed. The O proportion of surface was increased after ion implantation. The Fermi level of surface measurement by XPS valance band spectra was lowered as the ion accelerating voltage increased to 1.2 kV and then raised as accelerating voltage was elevated to 1.6 kV. The work function measured by Kelvin probe force microscopy increased after ion implanting, and it was consistent with the variation of Fermi level. The change of energy band structure of FTO surface mainly originated from the surface composition variation. As FTO conduction was primarily due to oxyanion hole, the carrier was electron and its concentration was reduced while O proportion was elevated at the surface of FTO, as a result, the Fermi level lowered and the work function was enlarged. It was proved that oxygen plasma treatment is an effective method to modulate the energy band structure of the surface as well as other properties of FTO, which provides much more space for interface and surface modification and then photoelectric device performance promotion.

A theoretical study of stability and vacancy replenishing of MoO{sub 3}(0 1 0) surfaces in oxygen atmosphere

Energy Technology Data Exchange (ETDEWEB)

Lei, Yan-Hua; Chen, Zhao-Xu, E-mail: zxchen@nju.edu.cn

2016-01-15

Graphical abstract: - Highlights: • Under normal experimental conditions perfect surface of MoO{sub 3}(0 1 0) is favorable. • Line defects along asymmetric oxygen direction in lean oxygen condition are favored. • Vacancy replenishing occurs on vacancies formed by terminal and asymmetrical oxygen. - Abstract: Oxygen vacancies on transition metal oxide surfaces are catalytically very important. The stability, shape and replenishing process of the vacancies are critical to understanding reactions happening on the surfaces. In this paper we investigate the stability of various defective MoO{sub 3}(0 1 0) surfaces and examine the influence of environmental oxygen on the stability as well as the active sites for the replenishing process. Our calculations reveal that the line oxygen defect along a (asymmetric oxygen) direction is thermodynamically most favorable at higher defect concentration whereas point defect surfaces are unfavorable. Under normal experimental conditions the perfect surface dominates the MoO{sub 3}(0 1 0). We show that for stoichiometric surfaces of any oxides (A{sub x}O{sub y}) the formation energy per vacancy controls the favorable defect shape (line or point defects). Calculations indicate that O{sub 2} can dissociate readily on the surfaces that double vacancies share one Mo atom. The replenishing process of the oxygen vacancies through O{sub 2} dissociation most likely occurs on the double-vacancy containing one terminal and one asymmetrical oxygen vacancies.

Emission of positive oxygen ions from ion bombardment of adsorbate-covered metal surfaces

International Nuclear Information System (INIS)

Kaurin, M.G.

1989-01-01

During ion bombardment of metal surfaces, collision cascades can result in the emission of sputtered secondary ions. Recent experiments, however, have suggested that the emission of positive ions of electronegative adsorbates can result from electronic processes rather than from processes involving elastic collisions. This dissertation presents the results of experiments studying the emission of positive oxygen ions from oxygen- and carbon-monoxide-covered transition metal surfaces during bombardment by 25-250 keV ions of neon, argon, and krypton. The systems studied may be grouped into four categories. For a nickel substrate with adsorbed oxygen, the emission of positive oxygen ions proceeds through collision cascades. For titanium and niobium with adsorbed oxygen, the emission of positive oxygen ions is proportional to the primary ion velocity, consistent with emission from electronic processes; for a given primary ion velocity, the oxygen ion yield is independent of primary ion species. For substrates of molybdenum and tungsten, the oxygen yield is proportional to primary ion velocity, but the yield also depends on the primary ion species for a given primary ion velocity in a manner that is consistent with emission resulting from electronic processes. For these two groups, except for titanium, the yields during neon ion bombardment do not extrapolate (assuming linearity with primary ion velocity) to a nonzero value at zero beam velocity. The magnitude of the oxygen ion yields from these targets is not consistent with that expected if the emission were induced by secondary electrons emitted during the ion bombardment

Is the surface oxygen exchange rate linked to bulk ion diffusivity in mixed conducting Ruddlesden-Popper phases?

Science.gov (United States)

Tomkiewicz, Alex C; Tamimi, Mazin A; Huq, Ashfia; McIntosh, Steven

2015-01-01

The possible link between oxygen surface exchange rate and bulk oxygen anion diffusivity in mixed ionic and electronic conducting oxides is a topic of great interest and debate. While a large body of experimental evidence and theoretical analyses support a link, observed differences between bulk and surface composition of these materials are hard to reconcile with this observation. This is further compounded by potential problems with simultaneous measurement of both parameters. Here we utilize separate techniques, in situ neutron diffraction and pulsed isotopic surface exchange, to examine bulk ion mobility and surface oxygen exchange rates of three Ruddlesden-Popper phases, general form A(n-1)A(2)'B(n)O(3n+1), A(n-1)A(2)'B(n)X(3n+1); LaSrCo(0.5)Fe(0.5)O(4-δ) (n = 1), La(0.3)Sr(2.7)CoFeO(7-δ) (n = 2) and LaSr3Co(1.5)Fe(1.5)O(10-δ) (n = 3). These measurements are complemented by surface composition determination via high sensitivity-low energy ion scattering. We observe a correlation between bulk ion mobility and surface exchange rate between materials. The surface exchange rates vary by more than one order of magnitude with high anion mobility in the bulk of an oxygen vacancy-rich n = 2 Ruddlesden-Popper material correlating with rapid oxygen exchange. This is in contrast with the similar surface exchange rates which we may expect due to similar surface compositions across all three samples. We conclude that experimental limitations lead to inherent convolution of surface and bulk rates, and that surface exchange steps are not likely to be rate limiting in oxygen incorporation.

Adsorption of atomic oxygen on PdAg/Pd(111) surface alloys and coadsorption of CO

Energy Technology Data Exchange (ETDEWEB)

Farkas, Arnold P. [Institute of Surface Chemistry and Catalysis, Ulm University, D-89069 Ulm (Germany); Reaction Kinetics Research Group, University of Szeged, Chemical Research Center of the Hungarian Academy of Sciences, H-6720 Szeged (Hungary); Bansmann, Joachim; Diemant, Thomas; Behm, R. Juergen [Institute of Surface Chemistry and Catalysis, Ulm University, D-89069 Ulm (Germany)

2011-07-01

The interaction of dissociated oxygen with structurally well-defined PdAg/Pd(111) surface alloys and the coadsorption of CO was studied by high resolution electron energy loss spectroscopy (HREELS) and temperature-programmed desorption (TPD). After oxygen saturation of the non-modified Pd(111) surface at RT, we observed the formation of a prominent peak in the HREEL spectra at 60 meV corresponding to the perpendicular vibration of oxygen atoms adsorbed in threefold hollow sites. Deposition of small Ag amounts does not change the signal intensity of this peak; it decreases only above 20% Ag. Beyond this Ag content, the peak intensity steeply declines and disappears at around 55-60% Ag. CO coadsorption on the oxygen pre-covered surfaces at 120 K leads to the formation of additional features in HREELS. For a surface alloy with 29% Ag, three loss features due to CO adsorption in on-top, bridge, and threefold-hollow sites can be discriminated already after the lowest CO exposure. Annealing of the co-adsorbed layer to 200 K triggers a decrease of the oxygen concentration due to CO{sub 2} formation. These findings are corroborated by TPD spectra of the CO desorption and CO{sub 2} production.

Study of the influence of surface anisotropy and lattice structure on the behaviour of a small magnetic cluster

International Nuclear Information System (INIS)

Hernandez, Laura; Pinettes, Claire

2005-01-01

We have studied by Monte Carlo simulations the thermal behaviour of a small (N=13 particles) cluster described by a Heisenberg model, including nearest-neighbour ferromagnetic interactions and radial surface anisotropy, in an applied magnetic field. We have studied three different lattice structures: hexagonal close packed, face centered cubic and icosahedral. We show that the zero-field thermal behaviour depends not only on the value of the anisotropy constant but also on the lattice structure. The behaviour in an applied field, additionally depends, on the different orientations of the field with respect to the crystal axes. According to these relative orientations, hysteresis cycles show different step-like characteristics

Study of the influence of surface anisotropy and lattice structure on the behaviour of a small magnetic cluster

Energy Technology Data Exchange (ETDEWEB)

Hernandez, Laura [Laboratoire de Physique Theorique et Modelisation, CNRS-UMR 8089, Universite de Cergy-Pontoise, 5 mail Gay Lussac, Neuville-sur-Oise, 95031 Cergy-Pontoise, Cedex (France)]. E-mail: Laura.Hernandez@ptm.u-cergy.fr; Pinettes, Claire [Laboratoire de Physique Theorique et Modelisation, CNRS-UMR 8089, Universite de Cergy-Pontoise, 5 mail Gay Lussac, Neuville-sur-Oise, 95031 Cergy-Pontoise, Cedex (France)

2005-08-15

We have studied by Monte Carlo simulations the thermal behaviour of a small (N=13 particles) cluster described by a Heisenberg model, including nearest-neighbour ferromagnetic interactions and radial surface anisotropy, in an applied magnetic field. We have studied three different lattice structures: hexagonal close packed, face centered cubic and icosahedral. We show that the zero-field thermal behaviour depends not only on the value of the anisotropy constant but also on the lattice structure. The behaviour in an applied field, additionally depends, on the different orientations of the field with respect to the crystal axes. According to these relative orientations, hysteresis cycles show different step-like characteristics.

Water Induced Surface Reconstruction of the Oxygen (2x1) covered Ru(0001)

Energy Technology Data Exchange (ETDEWEB)

Maier, Sabine; Cabrera-Sanfelix, Pepa; Stass, Ingeborg; Sanchez-Portal, Daniel; Arnau, Andres; Salmeron, Miquel

2010-08-06

Low temperature scanning tunneling microscopy (STM) and density functional theory (DFT) were used to study the adsorption of water on a Ru(0001) surface covered with half monolayer of oxygen. The oxygen atoms occupy hcp sites in an ordered structure with (2x1) periodicity. DFT predicts that water is weakly bound to the unmodified surface, 86 meV compared to the ~;;200 meV water-water H-bond. Instead, we found that water adsorption causes a shift of half of the oxygen atoms from hcp sites to fcc sites, creating a honeycomb structure where water molecules bind strongly to the exposed Ru atoms. The energy cost of reconstructing the oxygen overlayer, around 230 meV per displaced oxygen atom, is more than compensated by the larger adsorption energy of water on the newly exposed Ru atoms. Water forms hydrogen bonds with the fcc O atoms in a (4x2) superstructure due to alternating orientations of the molecules. Heating to 185 K results in the complete desorption of the water layer, leaving behind the oxygen honeycomb structure, which is metastable relative to the original (2x1). This stable structure is not recovered until after heating to temperatures close to 260K.

Dimers and the Critical Ising Model on lattices of genus >1

International Nuclear Information System (INIS)

Costa-Santos, Ruben; McCoy, B.M.

2002-01-01

We study the partition function of both Close-Packed Dimers and the Critical Ising Model on a square lattice embedded on a genus two surface. Using numerical and analytical methods we show that the determinants of the Kasteleyn adjacency matrices have a dependence on the boundary conditions that, for large lattice size, can be expressed in terms of genus two theta functions. The period matrix characterizing the continuum limit of the lattice is computed using a discrete holomorphic structure. These results relate in a direct way the lattice combinatorics with conformal field theory, providing new insight to the lattice regularization of conformal field theories on higher genus Riemann surfaces

Comparing the results of lattice and off-lattice simulations for the melt of nonconcatenated rings

International Nuclear Information System (INIS)

Halverson, Jonathan D; Kremer, Kurt; Grosberg, Alexander Y

2013-01-01

To study the conformational properties of unknotted and nonconcatenated ring polymers in the melt, we present a detailed qualitative and quantitative comparison of simulation data obtained by molecular dynamics simulation using an off-lattice bead-spring model and by Monte Carlo simulation using a lattice model. We observe excellent, and sometimes even unexpectedly good, agreement between the off-lattice and lattice results for many quantities measured including the gyration radii of the ring polymers, gyration radii of their subchains, contact probabilities, surface characteristics, number of contacts between subchains, and the static structure factors of the rings and their subchains. These results are, in part, put in contrast to Moore curves, and the open, linear polymer counterparts. While our analysis is extensive, our understanding of the ring melt conformations is still rather preliminary. (paper)

Simulation of surface profile formation in oxygen laser cutting of mild steel due to combustion cycles

Energy Technology Data Exchange (ETDEWEB)

Ermolaev, G V; Kovalev, O B [Khristianovich Institute of Theoretical and Applied Mechanics, Siberian Branch of Russian Academy of Sciences, Institutskaya Str 4/1, Novosibirsk, 630090 (Russian Federation)

2009-09-21

A physicomathematical model of cyclic iron combustion in an oxygen flow during oxygen laser cutting of metal sheets is developed. The combustion front is set into motion by focused laser radiation and a heterogeneous oxidation reaction in oxygen. The burning rate is limited by oxygen supply from the gas phase towards the metal surface, and the interface motion depends on the local temperature. A 3D numerical simulation predicts wavy structures on the metal surface; their linear sizes depend on the scanning speed of the laser beam, the thickness of the produced liquid oxide film and the parameters of the oxygen jet flow. Simulation results help in understanding the mechanism of striation formation during oxygen gas-laser cutting of mild steel and are in qualitative agreement with experimental findings.

Optical lattice on an atom chip

DEFF Research Database (Denmark)

Gallego, D.; Hofferberth, S.; Schumm, Thorsten

2009-01-01

Optical dipole traps and atom chips are two very powerful tools for the quantum manipulation of neutral atoms. We demonstrate that both methods can be combined by creating an optical lattice potential on an atom chip. A red-detuned laser beam is retroreflected using the atom chip surface as a high......-quality mirror, generating a vertical array of purely optical oblate traps. We transfer thermal atoms from the chip into the lattice and observe cooling into the two-dimensional regime. Using a chip-generated Bose-Einstein condensate, we demonstrate coherent Bloch oscillations in the lattice....

Interaction of ammonia with semiconducting oxide surfaces

Science.gov (United States)

Nigam, Sandeep; Sahoo, Suman Kalyan; Majumder, Chiranjib

2018-04-01

Using density functional theory (DFT) we have investigated the adsorption of NH3 molecule on the rutile SnO2(110) and mixed Sn0.5Ti0.5O2(110) surfaces. NH3 molecule gets absorbed on the 5-coordinated Sn atom (Sn5c) of the surface in tilted mode having an additional hydrogen bond with nearby surface bridged oxygen (Obr) atom. After adsorption, 3a1 molecular orbital of ammonia undergo significant dispersal as it donates its electron to surface atoms. The adsorption energy is found to be 1.4-1.6eV. Inclusion of Ti atoms in the SnO2 lattice leads to decrease in the adsorption energy value.

Lattice Boltzmann Study of Bubbles on a Patterned Superhydrophobic Surface under Shear Flow

Science.gov (United States)

Chen, Wei; Wang, Kai; Hou, Guoxiang; Leng, Wenjun

2018-01-01

This paper studies shear flow over a 2D patterned superhydrophobic surface using lattice Boltzmann method (LBM). Single component Shan-Chen multiphase model and Carnahan-Starling EOS are adopted to handle the liquid-gas flow on superhydrophobic surface with entrapped micro-bubbles. The shape of bubble interface and its influence on slip length under different shear rates are investigated. With increasing shear rate, the bubble interface deforms. Then the contact lines are depinned from the slot edges and move downstream. When the shear rate is high enough, a continuous gas layer forms. If the protrusion angle is small, the gas layer forms and collapse periodically, and accordingly the slip length changes periodically. While if the protrusion angle is large, the gas layer is steady and separates the solid wall from liquid, resulting in a very large slip length.

Distribution of local magnetic field of vortex lattice near anisotropic superconductor surface in inclined external fields

International Nuclear Information System (INIS)

Efremova, S.A.; Tsarevskij, S.L.

1997-01-01

Magnetic field distribution in a unit cell of the Abrikosov vortex lattice near the surface of monoaxial anisotropic type-ii superconductors in inclined external magnetic field has been found in the framework of London model for the cases when the symmetry axis is perpendicular and parallel to the superconductor surface interface. Distribution of local magnetic field as a function of the distance from the superconductor interface surface and external field inclination angle has been obtained. Using high-Tc superconductor Y-Ba-Cu-O by way of examples, it has been shown that the study of local magnetic field distribution function, depending on external magnetic field inclination angle towards the superconductor symmetry axis and towards the superconductor surface, can provide important data on anisotropic properties of the superconductor [ru

Effects of Nanofiber Architecture and Antimony Doping on the Performance of Lithium-Rich Layered Oxides: Enhancing Lithium Diffusivity and Lattice Oxygen Stability.

Science.gov (United States)

Yu, Ruizhi; Zhang, Zhijuan; Jamil, Sidra; Chen, Jiancheng; Zhang, Xiaohui; Wang, Xianyou; Yang, Zhenhua; Shu, Hongbo; Yang, Xiukang

2018-05-07

Li-rich layered oxides (LLOs) with high specific capacities are favorable cathode materials with high-energy density. Unfortunately, the drawbacks of LLOs such as oxygen release, low conductivity, and depressed kinetics for lithium ion transport during cycling can affect the safety and rate capability. Moreover, they suffer severe capacity and voltage fading, which are major challenges for the commercializing development. To cure these issues, herein, the synthesis of high-performance antimony-doped LLO nanofibers by an electrospinning process is put forward. On the basis of the combination of theoretical analyses and experimental approaches, it can be found that the one-dimensional porous micro-/nanomorphology is in favor of lithium-ion diffusion, and the antimony doping can expand the layered phase lattice and further improve the lithium ion diffusion coefficient. Moreover, the antimony doping can decrease the band gap and contribute extra electrons to O within the Li 2 MnO 3 phase, thereby enhancing electronic conductivity and stabilizing lattice oxygen. Benefitting from the unique architecture, reformative electronic structure, and enhanced kinetics, the antimony-doped LLO nanofibers possess a high reversible capacity (272.8 mA h g -1 ) and initial coulombic efficiency (87.8%) at 0.1 C. Moreover, the antimony-doped LLO nanofibers show excellent cycling performance, rate capability, and suppressed voltage fading. The capacity retention can reach 86.9% after 200 cycles at 1 C, and even cycling at a high rate of 10 C, a capacity of 172.3 mA h g -1 can still be obtained. The favorable results can assist in developing the LLO material with outstanding electrochemical properties.

SrRuO3 thin films grown on MgO substrates at different oxygen partial pressures

KAUST Repository

Zou, Bin

2013-01-08

A comprehensive study of SrRuO3 thin films growth on (001) MgO substrates by pulsed laser deposition in a wide oxygen pressure range from 10 to 300 mTorr was carried out. The experimental results showed a correlation between the lattice constants, resistivity, and oxygen partial pressures used. Ru deficiency detected only in films deposited at lower oxygen pressures (<50 mTorr), resulted in an elongation of the in-plane and out-of-plane lattice constants and an increase in the film resistivity. When deposited with oxygen partial pressure of 50 mTorr, SrRuO3 films had lattice parameters matching those of bulk SrRuO3 material and exhibited room temperature resistivity of 320 μΩ·cm. The resistivity of SrRuO 3/MgO films decreased with increasing oxygen partial pressure. Copyright © 2013 Materials Research Society.

Modelling and investigation of partial wetting surfaces for drop dynamics using lattice Boltzmann method

Science.gov (United States)

Pravinraj, T.; Patrikar, Rajendra

2017-07-01

Partial wetting surfaces and its influence on the droplet movement of micro and nano scale being contemplated for many useful applications. The dynamics of the droplet usually analyzed with a multiphase lattice Boltzmann method (LBM). In this paper, the influence of partial wetting surface on the dynamics of droplet is systematically analyzed for various cases. Splitting of droplets due to chemical gradient of the surface is studied and analyses of splitting time for various widths of the strips for different Weber numbers are computed. With the proposed model one can tune the splitting volume and time by carefully choosing a strip width and droplet position. The droplet spreading on chemically heterogeneous surfaces shows that the spreading can be controlled not only by parameters of Weber number but also by tuning strip width ratio. The transportation of the droplet from hydrophobic surface to hydrophilic surface due to chemical gradient is simulated and analyzed using our hybrid thermodynamic-image processing technique. The results prove that with the progress of time the surface free energy decreases with increase in spreading area. Finally, the transportation of a droplet on microstructure gradient is demonstrated. The model explains the temporal behaviour of droplet during the spreading, recoiling and translation along with tracking of contact angle hysteresis phenomenon.

Simulation of the catalyst layer in PEMFC based on a novel two-phase lattice model

Energy Technology Data Exchange (ETDEWEB)

Zhang Jiejing; Yang Wei; Xu Li [School of Chemical Engineering and Technology, State Key Laboratory of Chemical Engineering, Tianjin Key Laboratory of Membrane Science and Desalination Technology, Tianjin University, Tianjin 300072 (China); Wang Yuxin, E-mail: yxwang@tju.edu.cn [School of Chemical Engineering and Technology, State Key Laboratory of Chemical Engineering, Tianjin Key Laboratory of Membrane Science and Desalination Technology, Tianjin University, Tianjin 300072 (China)

2011-08-01

Highlights: > We propose a novel two phase lattice model of catalyst layer in PEMFC. > The model features a catalyst phase and a mixed ionomer and pores phase. > Transport and electrochemical reaction in the lattice are simulated. > The model enables more accurate results than pore-solid two phase model. > Profiles of oxygen level and reaction rate across catalyst layer vary with cell current. - Abstract: A lattice model of catalyst layer in proton exchange membrane fuel cells (PEMFCs), consisting of randomly distributed catalyst phase (C phase) and mixed ionomer-pore phase (IP phase), was established by means of Monte Carlo method. Transport and electrochemical reactions in the model catalyst layer were calculated. The newly proposed C-IP model was compared with previously established pore-solid two phase model. The variation of oxygen level and reaction rate along the thickness of catalyst layer with cell current was discussed. The effect of ionomer distribution across catalyst layer was studied by comparing profiles of oxygen level, reaction rate and overpotential, as well as corresponding polarization curves.

Hydrogen and oxygen isotope exchange reactions over illuminated and nonilluminated TiO2

International Nuclear Information System (INIS)

Sato, S.

1987-01-01

Hydrogen isotope exchange between H 2 , gaseous H 2 O, and the surface hydroxyls of TiO 2 , and oxygen isotope exchange between O 2 , CO 2 , CO, H 2 O vapor, and the hydroxyls over TiO 3 were studied at room temperature in the dark and under illumination. Hydrogen isotope exchange between H 2 O and the hydroxyls occurred rapidly in the dark, but the exchange involving H 2 did not occur at all even under illumination. Oxygen isotope exchange among H 2 O vapor, CO 2 , and the hydroxyls easily took place in the dark, but the exchange involving O 2 required band-gap illumination. Dioxygen isotope equilibration was much faster than the other photoexchange reactions. Although the oxygen exchange between O 2 and illuminated TiO 2 has been considered to involve lattice-oxygen exchange, the present experiments revealed that the hydroxyls of TiO 2 mainly participate in the exchange reaction. The oxygen exchange between O 2 and H 2 O vapor was strongly inhibited by H 2 O vapor itself probably because oxygen adsorption was retarded by adsorbed water. Oxygen in CO was not exchanged with the other substrates under any conditions tested

Evolution of Oxygen Deficiency Center on Fused Silica Surface Irradiated by Ultraviolet Laser and Posttreatment

Directory of Open Access Journals (Sweden)

Hai-Bing Lü

2014-01-01

Full Text Available Evolution of oxygen deficiency centers (ODCs on a fused silica surface irradiated using a 355 nm ultraviolet (UV laser beam in both vacuum and atmospheric conditions was quantitatively studied using photoluminescence and X-ray photoelectron spectroscopy. When the fusedsilica surface was exposed to the UV laser in vacuum, the laser damage threshold was decreased whereas the concentration of the ODCs was increased. For the fuse silica operated under the high power lasers, creation of ODCs on their surface resulted from the UV laser irradiation, and this is more severe in a high vacuum. The laser fluence and/or laser intensity have significant effects on the increase of the ODCs concentration. The ODCs can be effectively repaired using postoxygen plasma treatment and UV laser irradiation in an excessive oxygen environment. Results also demonstrated that the “gain” and “loss” of oxygen at the silica surface is a reversible and dynamic process.

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

Investigation of the generation of singlet oxygen in ensembles of photoexcited silicon nanocrystals by electron paramagnetic resonance spectroscopy

International Nuclear Information System (INIS)

Konstantinova, E. A.; Demin, V. A.; Timoshenko, V. Yu.

2008-01-01

The generation of singlet oxygen is investigated and its concentration upon photoexcitation of silicon nanocrystals in porous silicon layers is determined using electron paramagnetic resonance spectroscopy. The relaxation times of spin centers, i.e., silicon dangling bonds, in vacuum and in an oxygen atmosphere in the dark and under illumination of the samples are measured for the first time. It is revealed that the spin-lattice relaxation in porous silicon is retarded as compared to that in a single-crystal substrate. From analyzing experimental data, a microscopic model is proposed for interaction of oxygen molecules in the triplet state and spin centers at the surface of silicon nanocrystals. The results obtained have demonstrated that porous silicon holds promise for the use as a photosensitizer of molecular oxygen in biomedical applications

Crystalline and lattice matched Ba0.7Si0.3O layers on plane and vicinal Si(001) surfaces

International Nuclear Information System (INIS)

Zachariae, J.

2006-01-01

In this work the low temperature growth conditions of epitaxial and lattice-matched Ba 0.7 Sr 0.3 O layers on Si(100) were investigated using the combination of low energy electron diffraction (LEED), x-ray photoemission (XPS) and electron energy loss spectroscopy (EELS). With these methods crystallinity, stoichiometry and electronic structure of both occupied and unoccupied levels were studied as a function of layer thickness. Oxide layers were generated by evaporating the metals in oxygen ambient pressure with the sample at room temperature. Perfect crystallinity and lattice matching was only obtained starting with a preadsorbed monolayer (ML) of Sr or Ba at a concentration close to one monolayer. The XPS analysis shows that Ba 0.7 Sr 0.3 O as a high-K gate dielectric offers an adequate band gap, an appropriate band alignment and a atomically sharp interface to the Si(001) substrate. No silicide and silicate species, or SiO 2 formation at the interface after oxidation were found. To show that Ba 0.7 Sr 0.3 O is really appropriate to replace SiO 2 as a gate dielectric, first C-V and I-V curves of MOS-diodes with SrO, BaO and Ba 0.7 Sr 0.3 O as gateoxide were measured under ambient conditions. Besides other results, it turns out that the measured dielectric constant of Ba 0.7 Sr 0.3 O conforms with the expected value of ε ∼ 25 - 30. Exploring ways for self-organized structuring of insulating films, the possibility to produce replicas of step trains, given by a vicinal Si(001)-4 [110] surface, in layers of crystalline and perfectly lattice matched Ba 0.7 Sr 0.3 O were investigated. For this purpose high-resolution spot profile analyses in low-energy electron diffraction (SPA-LEED) both on flat Si(001) and on vicinal Si(001)-4 [110] were carried out. The G(S) analysis of these mixed oxide layers reveals a strong influence of local compositional fluctuations of Sr and Ba ions and their respective scattering phases, which appears as an unphysically large variation

Effect of annealing ambience on the formation of surface/bulk oxygen vacancies in TiO2 for photocatalytic hydrogen evolution

Science.gov (United States)

Hou, Lili; Zhang, Min; Guan, Zhongjie; Li, Qiuye; Yang, Jianjun

2018-01-01

The surface and bulk oxygen vacancy have a prominent effect on the photocatalytic performance of TiO2. In this study, TiO2 possessing different types and concentration of oxygen vacancies were prepared by annealing nanotube titanic acid (NTA) at various temperatures in air or vacuum atmosphere. TiO2 with the unitary bulk single-electron-trapped oxygen vacancies (SETOVs) formed when NTA were calcined in air. Whereas, TiO2 with both bulk and surface oxygen vacancies were obtained when NTA were annealed in vacuum. The series of TiO2 with different oxygen vacancies were systematically characterized by TEM, XRD, PL, XPS, ESR, and TGA. The PL and ESR analysis verified that surface oxygen vacancies and more bulk oxygen vacancies could form in vacuum atmosphere. Surface oxygen vacancies can trap electron and hinder the recombination of photo-generated charges, while bulk SETOVs act as the recombination center. The surface or bulk oxygen vacancies attributed different roles on the photo-absorbance and activity, leading that the sample of NTA-A400 displayed higher hydrogen evolution rate under UV light, whereas NTA-V400 displayed higher hydrogen evolution rate under visible light because bulk SETOVs can improve visible light absorption because sub-band formed by bulk SETOVs prompted the secondary transition of electron excited.

Control of magnetic properties and band gap by Co/Mn ordering and oxygen distributions of La{sub 2}CoMnO{sub 6}

Energy Technology Data Exchange (ETDEWEB)

Liu, Fang; Gao, Yu; Chang, Hong, E-mail: changhong@imu.edu.cn; Liu, Yifan; Yun, Yuehou

2017-08-01

Highlights: • The stretching vibration of the ordered Co-O-Mn bond is observed in IR-FT curve. • The surface absorbed oxygen transforms to the lattice oxygen is observed at 905 °C. - Abstract: La{sub 2}CoMnO{sub 6} are synthesized at different annealing temperature ranging from 600 °C to 1300 °C, marked as S600, S800, S1000 and S1300. S600 has the R-3c and the rest have the Pnma structure. The DTA curve exhibits two exothermic peaks, at 553 °C for the phase formation and 905 °C for the oxygen redistribution into the lattice. Deduced from xps, S1000 has the highest lattice oxygen. S1300 has one extra xps peak due to the oxygen deficient regions. Even though the xrd refinements are not reliable at telling whether Co/Mn ions are ordered or not, IR-FT, magnetic measurements and energy band gaps indicate that S1000 has the best Co/Mn ordering, and S600 has the worst. A stretching vibration at about 580–595 cm{sup −1} in the IR-FT spectra is attributed to the ordered Co–O–Mn bond. A homogenous atomic distribution in S600, S800 and S1000 leads to one magnetic phase configuration, and the agglomeration of the FM ordered Co/Mn and the AFM disordered regions in S1300 induces the multi magnetic phases. From the aspects of band gap and energy level, S600 is a good candidate for light harvesting.

Multi-functional magnesium alloys containing interstitial oxygen atoms.

Science.gov (United States)

Kang, H; Choi, H J; Kang, S W; Shin, S E; Choi, G S; Bae, D H

2016-03-15

A new class of magnesium alloys has been developed by dissolving large amounts of oxygen atoms into a magnesium lattice (Mg-O alloys). The oxygen atoms are supplied by decomposing titanium dioxide nanoparticles in a magnesium melt at 720 °C; the titanium is then completely separated out from the magnesium melt after solidification. The dissolved oxygen atoms are located at the octahedral sites of magnesium, which expand the magnesium lattice. These alloys possess ionic and metallic bonding characteristics, providing outstanding mechanical and functional properties. A Mg-O-Al casting alloy made in this fashion shows superior mechanical performance, chemical resistance to corrosion, and thermal conductivity. Furthermore, a similar Mg-O-Zn wrought alloy shows high elongation to failure (>50%) at room temperature, because the alloy plastically deforms with only multiple slips in the sub-micrometer grains (alloys are expected to open a new paradigm in commercial alloy design.

Off-lattice self-learning kinetic Monte Carlo: application to 2D cluster diffusion on the fcc(111) surface

International Nuclear Information System (INIS)

Kara, Abdelkader; Yildirim, Handan; Rahman, Talat S; Trushin, Oleg

2009-01-01

We report developments of the kinetic Monte Carlo (KMC) method with improved accuracy and increased versatility for the description of atomic diffusivity on metal surfaces. The on-lattice constraint built into our recently proposed self-learning KMC (SLKMC) (Trushin et al 2005 Phys. Rev. B 72 115401) is released, leaving atoms free to occupy 'off-lattice' positions to accommodate several processes responsible for small-cluster diffusion, periphery atom motion and heteroepitaxial growth. This technique combines the ideas embedded in the SLKMC method with a new pattern-recognition scheme fitted to an off-lattice model in which relative atomic positions are used to characterize and store configurations. Application of a combination of the 'drag' and the repulsive bias potential (RBP) methods for saddle point searches allows the treatment of concerted cluster, and multiple- and single-atom, motions on an equal footing. This tandem approach has helped reveal several new atomic mechanisms which contribute to cluster migration. We present applications of this off-lattice SLKMC to the diffusion of 2D islands of Cu (containing 2-30 atoms) on Cu and Ag(111), using the interatomic potential from the embedded-atom method. For the hetero-system Cu/Ag(111), this technique has uncovered mechanisms involving concerted motions such as shear, breathing and commensurate-incommensurate occupancies. Although the technique introduces complexities in storage and retrieval, it does not introduce noticeable extra computational cost.

3D Metallic Lattices for Accelerator Applications

CERN Document Server

Shapiro, Michael A; Sirigiri, Jagadishwar R; Temkin, Richard J

2005-01-01

We present the results of research on 3D metallic lattices operating at microwave frequencies for application in (1) accelerator structures with higher order mode suppression, (2) Smith-Purcell radiation beam diagnostics, and (3) polaritonic materials for laser acceleration. Electromagnetic waves in a 3D simple cubic lattice formed by metal wires are calculated using HFSS. The bulk modes in the lattice are determined using single cell calculations with different phase advances in all three directions. The Brillouin diagram for the bulk modes is presented and indicates the absence of band gaps in simple lattices except the band below the cutoff. Lattices with thin wires as well as with thick wires have been analyzed. The Brillouin diagram also indicates the presence of low frequency 3D plasmon mode as well as the two degenerate photon modes analogous to those in a 2D lattice. Surface modes for a semi-infinite cubic lattice are modeled as a stack of cells with different phase advances in the two directions alon...

Theoretical Studies of the Structure and the Dynamics on Clean and Chemisorbed Metal Surfaces

Science.gov (United States)

Yang, Liqiu

Molecular dynamics (MD) and lattice dynamics (LD) techniques are employed to investigate several phenomena related to the structure and vibrations at metal surfaces. The MD simulations are performed with the many-body interaction potentials obtained using the Embedded-Atom Method (EAM). As specific examples, we present the results for Ag(100) at 300 K and Cu(100) at 150 K, 300 K, and 600 K. The calculated frequencies and polarizations of all surface modes and resonances at the high-symmetry points in the two-dimensional Brillouin zone are in good agreement with available data, as well as, existing lattice dynamics results with force constants obtained from first-principles calculations. Our calculated surface relaxation is also in reasonable agreement with the data. We also test a much simpler lattice dynamics model with nearest neighbor central force interactions, and conclude that it can reproduce the main features of the phonon modes, but only when adjustable surface parameters are used. Additionally, the temperature dependent studies of the phonon line-widths and the mean-square displacement (MSD) of surface atoms are indicative of enhanced surface anharmonicity. On several chemisorbed metal surfaces, for which force constants are not available from first-principles calculations or the EAM, we perform lattice dynamics studies of phonon dispersion curves using simple force-constant models. These studies provide reliable mean-square displacement of surface atoms and can distinguish between possible reconstruction patterns, the results being insensitive to the exact values of the surface parameters. On c(2 times 2)S-Ni(100), it is found that the parallel component of the mean-square displacement for sulfur is around 50% larger than the vertical component, but for the mean-square displacement of oxygen atoms in the system c(2 times 2)O-Ni(100), the opposite is the case. As regards surface reconstruction, for both p(2 times 1)O-Ag(110) and p(2 times 1)O-Ni(110

First-principles studies on vacancy-modified interstitial diffusion mechanism of oxygen in nickel, associated with large-scale atomic simulation techniques

International Nuclear Information System (INIS)

Fang, H. Z.; Shang, S. L.; Wang, Y.; Liu, Z. K.; Alfonso, D.; Alman, D. E.; Shin, Y. K.; Zou, C. Y.; Duin, A. C. T. van; Lei, Y. K.; Wang, G. F.

2014-01-01

This paper is concerned with the prediction of oxygen diffusivities in fcc nickel from first-principles calculations and large-scale atomic simulations. Considering only the interstitial octahedral to tetrahedral to octahedral minimum energy pathway for oxygen diffusion in fcc lattice, greatly underestimates the migration barrier and overestimates the diffusivities by several orders of magnitude. The results indicate that vacancies in the Ni-lattice significantly impact the migration barrier of oxygen in nickel. Incorporation of the effect of vacancies results in predicted diffusivities consistent with available experimental data. First-principles calculations show that at high temperatures the vacancy concentration is comparable to the oxygen solubility, and there is a strong binding energy and a redistribution of charge density between the oxygen atom and vacancy. Consequently, there is a strong attraction between the oxygen and vacancy in the Ni lattice, which impacts diffusion

Ordering phenomena and non-equilibrium properties of lattice gas models

International Nuclear Information System (INIS)

Fiig, T.

1994-03-01

This report falls within the general field of ordering processes and non-equilibrium properties of lattice gas models. The theory of diffuse scattering of lattice gas models originating from a random distribution of clusters is considered. We obtain relations between the diffuse part of the structure factor S dif (q), the correlation function C(r), and the size distribution of clusters D(n). For a number of distributions we calculate S dif (q) exactly in one dimension, and discuss the possibility for a Lorentzian and a Lorentzian square lineshape to arise. We discuss the two- and three-dimensional oxygen ordering processes in the high T c superconductor YBa 2 Cu 3 O 6+x based on a simple anisotropic lattice gas model. We calculate the structural phase diagram by Monte Carlo simulation and compared the results with experimental data. The structure factor of the oxygen ordering properties has been calculated in both two and three dimensions by Monte Carlo simulation. We report on results obtained from large scale computations on the Connection Machine, which are in excellent agreement with recent neutron diffraction data. In addition we consider the effect of the diffusive motion of metal-ion dopants on the oxygen ordering properties on YBa 2 Cu 3 O 6+x . The stationary properties of metastability in long-range interaction models are studied by application of a constrained transfer matrix (CTM) formalism. The model considered, which exhibits several metastable states, is an extension of the Blume Capel model to include weak long-range interactions. We show, that the decay rate of the metastable states is closely related to the imaginary part of the equilibrium free-energy density obtained from the CTM formalism. We discuss a class of lattice gas model for dissipative transport in the framework of a Langevin description, which is capable of producing power law spectra for the density fluctuations. We compare with numerical results obtained from simulations of a

Unraveling the oxygen vacancy structures at the reduced Ce O2(111 ) surface

Science.gov (United States)

Han, Zhong-Kang; Yang, Yi-Zhou; Zhu, Beien; Ganduglia-Pirovano, M. Verónica; Gao, Yi

2018-03-01

Oxygen vacancies at ceria (Ce O2 ) surfaces play an essential role in catalytic applications. However, during the past decade, the near-surface vacancy structures at Ce O2(111 ) have been questioned due to the contradictory results from experiments and theoretical simulations. Whether surface vacancies agglomerate, and which is the most stable vacancy structure for varying vacancy concentration and temperature, are being heatedly debated. By combining density functional theory calculations and Monte Carlo simulations, we proposed a unified model to explain all conflicting experimental observations and theoretical results. We find a novel trimeric vacancy structure which is more stable than any other one previously reported, which perfectly reproduces the characteristics of the double linear surface oxygen vacancy clusters observed by STM. Monte Carlo simulations show that at low temperature and low vacancy concentrations, vacancies prefer subsurface sites with a local (2 × 2) ordering, whereas mostly linear surface vacancy clusters do form with increased temperature and degree of reduction. These results well explain the disputes about the stable vacancy structure and surface vacancy clustering at Ce O2(111 ) , and provide a foundation for the understanding of the redox and catalytic chemistry of metal oxides.

Feasibility Analysis of Liquefying Oxygen Generated from Water Electrolysis Units on Lunar Surface

Science.gov (United States)

Jeng, Frank F.

2009-01-01

Concepts for liquefying oxygen (O2) generated from water electrolysis subsystems on the Lunar surface were explored. Concepts for O2 liquefaction units capable of generating 1.38 lb/hr (0.63 kg/hr) liquid oxygen (LOX) were developed. Heat and mass balance calculations for the liquefaction concepts were conducted. Stream properties, duties of radiators, heat exchangers and compressors for the selected concepts were calculated and compared.

Chiral symmetry on the lattice

International Nuclear Information System (INIS)

Creutz, M.

1994-11-01

The author reviews some of the difficulties associated with chiral symmetry in the context of a lattice regulator. The author discusses the structure of Wilson Fermions when the hopping parameter is in the vicinity of its critical value. Here one flavor contrasts sharply with the case of more, where a residual chiral symmetry survives anomalies. The author briefly discusses the surface mode approach, the use of mirror Fermions to cancel anomalies, and finally speculates on the problems with lattice versions of the standard model

Simultaneous modulation of surface composition, oxygen vacancies and assembly in hierarchical Co3O4 mesoporous nanostructures for lithium storage and electrocatalytic oxygen evolution

DEFF Research Database (Denmark)

Sun, Hongyu; Zhao, Yanyan; Mølhave, Kristian

2017-01-01

in superior electrochemical properties when used as the anode materials for lithium-ion batteries and as an electrocatalyst for the oxygen evolution reaction. The excellent electrochemical performance is attributed to the synergistic effects of novel hierarchical morphology, crystal structure of the active...... materials, the improvement of intrinsic conductivity and inner surface area induced by the oxygen vacancies. The present strategy not only provides a facile method to assemble novel hierarchical architectures, but also paves a way to control surface structures (chemical composition and crystal defects...

A lattice Boltzmann simulation of coalescence-induced droplet jumping on superhydrophobic surfaces with randomly distributed structures

Science.gov (United States)

Zhang, Li-Zhi; Yuan, Wu-Zhi

2018-04-01

The motion of coalescence-induced condensate droplets on superhydrophobic surface (SHS) has attracted increasing attention in energy-related applications. Previous researches were focused on regularly rough surfaces. Here a new approach, a mesoscale lattice Boltzmann method (LBM), is proposed and used to model the dynamic behavior of coalescence-induced droplet jumping on SHS with randomly distributed rough structures. A Fast Fourier Transformation (FFT) method is used to generate non-Gaussian randomly distributed rough surfaces with the skewness (Sk), kurtosis (K) and root mean square (Rq) obtained from real surfaces. Three typical spreading states of coalesced droplets are observed through LBM modeling on various rough surfaces, which are found to significantly influence the jumping ability of coalesced droplet. The coalesced droplets spreading in Cassie state or in composite state will jump off the rough surfaces, while the ones spreading in Wenzel state would eventually remain on the rough surfaces. It is demonstrated that the rough surfaces with smaller Sks, larger Rqs and a K at 3.0 are beneficial to coalescence-induced droplet jumping. The new approach gives more detailed insights into the design of SHS.

Dynamics and Thermochemistry of Oxygen Uptake by a Mixed Ce-Pr Oxide

Science.gov (United States)

Sinev, M. Yu.; Fattakhova, Z. T.; Bychkov, V. Yu.; Lomonosov, V. I.; Gordienko, Yu. A.

2018-03-01

The dynamics of oxygen uptake by mixed Ce0.55Pr0.45O2-x oxide is studied in a pulsed oxygen supply mode using in situ high-temperature heat flow differential scanning calorimetry. It is stated that the oxidation proceeds in two regimes: a fast one at the beginning of the oxidation process, and a slow one, which is controlled by the diffusion of oxygen through the bulk of the solid at the later stages of the process. Analysis of the shape of calorimetric profiles reveals some processes, accompanied by heat release, that occur in the sample in the absence of oxygen in the gas phase. These could be due to both the redistribution of consumed oxygen in the oxide lattice and the lattice relaxation associated with the transformation of phases with different arrangements of oxygen vacancies in them. The heat effect (which diminishes from 60 to 40 kJ/mol in the course of oxygen uptake) associated with the oxidation of the reduced form of mixed Ce-Pr oxide, corresponds to the oxidation of praseodymium ions from (3+) to (4+).

Universality in Oxygen Evolution Electrocatalysis on Oxide Surfaces

DEFF Research Database (Denmark)

Man, Isabela Costinela; Su, Hai-Yan; Vallejo, Federico Calle

2011-01-01

with the computational standard hydrogen electrode (SHE) model. We showed that by the discovery of a universal scaling relation between the adsorption energies of HOO* vs HO*, it is possible to analyze the reaction free energy diagrams of all the oxides in a general way. This gave rise to an activity volcano......Trends in electrocatalytic activity of the oxygen evolution reaction (OER) are investigated on the basis of a large database of HO* and HOO* adsorption energies on oxide surfaces. The theoretical overpotential was calculated by applying standard density functional theory in combination...

Oxygen termination of homoepitaxial diamond surface by ozone and chemical methods: An experimental and theoretical perspective

Science.gov (United States)

Navas, Javier; Araujo, Daniel; Piñero, José Carlos; Sánchez-Coronilla, Antonio; Blanco, Eduardo; Villar, Pilar; Alcántara, Rodrigo; Montserrat, Josep; Florentin, Matthieu; Eon, David; Pernot, Julien

2018-03-01

Phenomena related with the diamond surface of both power electronic and biosensor devices govern their global behaviour. In particular H- or O-terminations lead to wide variations in their characteristics. To study the origins of such aspects in greater depth, different methods to achieve oxygen terminated diamond were investigated following a multi-technique approach. DFT calculations were then performed to understand the different configurations between the C and O atoms. Three methods for O-terminating the diamond surface were performed: two physical methods with ozone at different pressures, and an acid chemical treatment. X-ray photoelectron spectroscopy, spectroscopic ellipsometry, HRTEM, and EELS were used to characterize the oxygenated surface. Periodic-DFT calculations were undertaken to understand the effect of the different ways in which the oxygen atoms are bonded to carbon atoms on the diamond surface. XPS results showed the presence of hydroxyl or ether groups, composed of simple Csbnd O bonds, and the acid treatment resulted in the highest amount of O on the diamond surface. In turn, ellipsometry showed that the different treatments led to the surface having different optical properties, such as a greater refraction index and extinction coefficient in the case of the sample subjected to acid treatment. TEM analysis showed that applying temperature treatment improved the distribution of the oxygen atoms at the interface and that this generates a thinner amount of oxygen at each position and higher interfacial coverage. Finally, DFT calculations showed both an increase in the number of preferential electron transport pathways when π bonds and ether groups appear in the system, and also the presence of states in the middle of the band gap when there are π bonds, Cdbnd C or Cdbnd O.

Systematic spatial and stoichiometric screening towards understanding the surface of ultrasmall oxygenated silicon nanocrystal

Energy Technology Data Exchange (ETDEWEB)

Niaz, Shanawer, E-mail: shanawersi@gmail.com [Department of Physics, Bilkent University, Ankara 06800 (Turkey); Molecular Engineering Laboratory, at the Department of Physics, University of Patras, Patras, GR-26500 (Greece); Zdetsis, Aristides D.; Koukaras, Emmanuel N. [Molecular Engineering Laboratory, at the Department of Physics, University of Patras, Patras, GR-26500 (Greece); Gülseren, Oǧuz [Department of Physics, Bilkent University, Ankara 06800 (Turkey); Sadiq, Imran [Centre of Excellence in Solid State Physics, University of the Punjab, Lahore (Pakistan)

2016-11-30

Highlights: • Understanding surface science of oxygenated silicon nanocrystals by means of their composition, stoichiometry and spatial distribution. • Drastic change observed in binding energy, localization of frontier orbitals and HOMO-LUMO gap up to 1.48 eV. • Might be a safe alternative of size dependent bandgap tunability. - Abstract: In most of the realistic ab initio and model calculations which have appeared on the emission of light from silicon nanocrystals, the role of surface oxygen has been usually ignored, underestimated or completely ruled out. We investigate theoretically, by density functional theory (DFT/B3LYP) possible modes of oxygen bonding in hydrogen terminated silicon quantum dots using as a representative case of the Si{sub 29} nanocrystal. We have considered Bridge-bonded oxygen (BBO), Doubly-bonded oxygen (DBO), hydroxyl (OH) and Mix of these oxidizing agents. Due to stoichiometry, all comparisons performed are unbiased with respect to composition whereas spatial distribution of oxygen species pointed out drastic change in electronic and cohesive characteristics of nanocrytals. From an overall perspective of this study, it is shown that bridge bonded oxygenated Si nanocrystals accompanied by Mix have higher binding energies and large electronic gap compared to nanocrystals with doubly bonded oxygen atoms. In addition, it is observed that the presence of OH along with BBO, DBO and mixed configurations further lowers electronic gaps and binding energies but trends in same fashion. It is also demonstrated that within same composition, oxidizing constituent, along with their spatial distribution substantially alters binding energy, highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) gap (up to 1.48 eV) and localization of frontier orbitals.

Systematic spatial and stoichiometric screening towards understanding the surface of ultrasmall oxygenated silicon nanocrystal

International Nuclear Information System (INIS)

Niaz, Shanawer; Zdetsis, Aristides D.; Koukaras, Emmanuel N.; Gülseren, Oǧuz; Sadiq, Imran

2016-01-01

Highlights: • Understanding surface science of oxygenated silicon nanocrystals by means of their composition, stoichiometry and spatial distribution. • Drastic change observed in binding energy, localization of frontier orbitals and HOMO-LUMO gap up to 1.48 eV. • Might be a safe alternative of size dependent bandgap tunability. - Abstract: In most of the realistic ab initio and model calculations which have appeared on the emission of light from silicon nanocrystals, the role of surface oxygen has been usually ignored, underestimated or completely ruled out. We investigate theoretically, by density functional theory (DFT/B3LYP) possible modes of oxygen bonding in hydrogen terminated silicon quantum dots using as a representative case of the Si 29 nanocrystal. We have considered Bridge-bonded oxygen (BBO), Doubly-bonded oxygen (DBO), hydroxyl (OH) and Mix of these oxidizing agents. Due to stoichiometry, all comparisons performed are unbiased with respect to composition whereas spatial distribution of oxygen species pointed out drastic change in electronic and cohesive characteristics of nanocrytals. From an overall perspective of this study, it is shown that bridge bonded oxygenated Si nanocrystals accompanied by Mix have higher binding energies and large electronic gap compared to nanocrystals with doubly bonded oxygen atoms. In addition, it is observed that the presence of OH along with BBO, DBO and mixed configurations further lowers electronic gaps and binding energies but trends in same fashion. It is also demonstrated that within same composition, oxidizing constituent, along with their spatial distribution substantially alters binding energy, highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) gap (up to 1.48 eV) and localization of frontier orbitals.

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...

Phenol by direct hydroxylation of benzene with nitrous oxide - role of surface oxygen species in the reaction pathways

Energy Technology Data Exchange (ETDEWEB)

Reitzmann, A.; Klemm, E.; Emig, G. [Erlangen-Nuernberg Univ., Erlangen (Germany). Lehrstuhl fuer Technische Chemie 1; Buchholz, S.A.; Zanthoff, H.W. [Bochum Univ. (Germany). Inst. of Technical Chemistry

1998-12-31

Transient experiments in a Temporal Analysis of Products (TAP) Reactor were performed to elucidate the role of surface oyxgen species in the oxidation of benzene to phenol on ZSM-5 type zeolites with nitrous oxide as a selective oxidant. It was shown by puls experiments with nitrous oxide that the mean lifetime of the generated surface oxygen species is between 0.2s at 500 C and about 4.2 s at 400 C. Afterwards the surface oxygen species desorb as molecular oxygen into the gas phase where total oxidation will take place if hydrocarbons are present. Dual puls experiments consisting of a nitrous oxide puls followed by a benzene puls allowed studying the reactivity of the surface oxygen species formed during the first puls. The observation of the phenol formation was impeded due to the strong sorption of phenol. Multipulse experiments were necessary to reach a pseudo steady state phenol yield. (orig.)

The surface structure of SrTiO3 at high temperatures under influence of oxygen

International Nuclear Information System (INIS)

Hesselberth, M. B. S.; Molen, S. J. van der; Aarts, J.

2014-01-01

We use low energy electron microscopy to investigate the structure of the SrTiO 3 (001) surface at elevated temperatures and different oxygen pressures. Upon varying the temperature between 500 °C and 900 °C in oxygen pressures ranging from 10 −9 millibar to 10 −4 millibar, two surface transitions are found to be present. The lower temperature (1 × 1) → (2 × 1) transition that is known to occur in ultrahigh vacuum can be reversed by increasing the oxygen pressure. At higher temperatures, we observe a (2 × 1) → disordered (1 × 1) transition which is irreversible in the experimental parameter range. The observations are expected to have a strong bearing on the growth of interface structures

Effects of reduced surface tension on two-phase diversion cross-flow between subchannels simplifying triangle tight lattice rod bundle

International Nuclear Information System (INIS)

Kawahara, Akimaro; Sadatomi, Michio; Higuchi, Tatsuya

2009-01-01

Two-phase diversion cross-flow between tight lattice subchannels has been investigated experimentally and analytically. For hydraulically non-equilibrium flows with the pressure difference between the subchannels, experiments were conducted using a vertical multiple-channel with two subchannels simplifying a triangle tight lattice rod bundle. To know the effects of the reduced surface tension on the diversion cross-flow, water and water with a surfactant were used as the test liquids. Data were obtained on the axial variations in the pressure difference between the subchannels, gas and liquid flow rates and void fraction in each subchannel for slug-churn and annular flows. In the analysis, flow redistribution processes due to the diversion cross-flow have been calculated by our subchannel analysis code based on a two-fluid model. From a comparison between the experiment and the code calculation, the code was found to be valid against the present data if the improved constitutive equations of wall and interfacial friction reported in our previous paper were incorporated to account for the reduced surface tension effects. (author)

Lattice Transparency of Graphene.

Science.gov (United States)

Chae, Sieun; Jang, Seunghun; Choi, Won Jin; Kim, Youn Sang; Chang, Hyunju; Lee, Tae Il; Lee, Jeong-O

2017-03-08

Here, we demonstrated the transparency of graphene to the atomic arrangement of a substrate surface, i.e., the "lattice transparency" of graphene, by using hydrothermally grown ZnO nanorods as a model system. The growth behaviors of ZnO nanocrystals on graphene-coated and uncoated substrates with various crystal structures were investigated. The atomic arrangements of the nucleating ZnO nanocrystals exhibited a close match with those of the respective substrates despite the substrates being bound to the other side of the graphene. By using first-principles calculations based on density functional theory, we confirmed the energetic favorability of the nucleating phase following the atomic arrangement of the substrate even with the graphene layer present in between. In addition to transmitting information about the atomic lattice of the substrate, graphene also protected its surface. This dual role enabled the hydrothermal growth of ZnO nanorods on a Cu substrate, which otherwise dissolved in the reaction conditions when graphene was absent.

Evaluation of hydrogen and oxygen impurity levels on silicon surfaces

Energy Technology Data Exchange (ETDEWEB)

Kenny, M.J.; Wielunski, L.S.; Netterfield, R.P.; Martin, P.J.; Leistner, A. [Commonwealth Scientific and Industrial Research Organisation (CSIRO), Lindfield, NSW (Australia). Div. of Applied Physics

1996-12-31

This paper reports on surface analytical techniques used to quantify surface concentrations of impurities such as oxygen and hydrogen. The following analytical techniques were used: Rutherford and Backscattering, elastic recoil detection, time-of-flight SIMS, spectroscopic ellipsometry, x-ray photoelectron spectroscopy. The results have shown a spread in thickness of oxide layer, ranging from unmeasurable to 1.6 nm. The data must be considered as preliminary at this stage, but give some insight into the suitability of the techniques and a general idea of the significance of impurities at the monolayer level. These measurements have been carried out on a small number of silicon surfaces both semiconductor grade <111> crystalline material and silicon which has been used in sphere fabrication. 5 refs., 1 fig.

Evaluation of hydrogen and oxygen impurity levels on silicon surfaces

Energy Technology Data Exchange (ETDEWEB)

Kenny, M J; Wielunski, L S; Netterfield, R P; Martin, P J; Leistner, A [Commonwealth Scientific and Industrial Research Organisation (CSIRO), Lindfield, NSW (Australia). Div. of Applied Physics

1997-12-31

This paper reports on surface analytical techniques used to quantify surface concentrations of impurities such as oxygen and hydrogen. The following analytical techniques were used: Rutherford and Backscattering, elastic recoil detection, time-of-flight SIMS, spectroscopic ellipsometry, x-ray photoelectron spectroscopy. The results have shown a spread in thickness of oxide layer, ranging from unmeasurable to 1.6 nm. The data must be considered as preliminary at this stage, but give some insight into the suitability of the techniques and a general idea of the significance of impurities at the monolayer level. These measurements have been carried out on a small number of silicon surfaces both semiconductor grade <111> crystalline material and silicon which has been used in sphere fabrication. 5 refs., 1 fig.

Comparison of oxygen liquefaction methods for use on the Martian surface

Science.gov (United States)

Johnson, W. L.; Hauser, D. M.; Plachta, D. W.; Wang, X.-Y. J.; Banker, B. F.; Desai, P. S.; Stephens, J. R.; Swanger, A. M.

2018-03-01

In order to use oxygen that is produced on the surface of Mars from In-Situ production processes in a chemical propulsion system, the oxygen must first be converted from vapor phase to liquid phase and then stored within the propellant tanks of the propulsions system. There are multiple ways that this can be accomplished, from simply attaching a liquefaction system onto the propellant tanks to carrying separate tanks for liquefaction and storage of the propellant and loading just prior to launch (the way that traditional rocket launches occur on Earth). A study was done into these various methods by which the oxygen (and methane) could be liquefied and stored on the Martian surface. Five different architectures or cycles were considered: Tube-on-Tank (also known as Broad Area Cooling or Distributed Refrigeration), Tube-in-Tank (also known as Integrated Refrigeration and Storage), a modified Linde open liquefaction/refrigeration cycle, the direct mounting of a pulse tube cryocooler onto the tank, and an in-line liquefier at ambient pressure. Models of each architecture were developed to give insight into the performance and losses of each of the options. The results were then compared across eight categories: Mass, Power (both input and heat rejection), Operability, Cost, Manufacturability, Reliability, Volume-ility, and Scalability. The result was that Tube-on-Tank and Tube-in-Tank architectures were the most attractive solutions, with NASA's engineering management choosing to pursue tube on tank development rather than further differentiate the two. As a result NASA is focusing its Martian surface liquefaction activities and technology development on Tube-on-Tank liquefaction cycles.

Untangling surface oxygen exchange effects in YBa2Cu3O6+x thin films by electrical conductivity relaxation.

Science.gov (United States)

Cayado, P; Sánchez-Valdés, C F; Stangl, A; Coll, M; Roura, P; Palau, A; Puig, T; Obradors, X

2017-05-31

The kinetics of oxygen incorporation (in-diffusion process) and excorporation (out-diffusion process), in YBa 2 Cu 3 O 6+x (YBCO) epitaxial thin films prepared using the chemical solution deposition (CSD) methodology by the trifluoroacetate route, was investigated by electrical conductivity relaxation measurements. We show that the oxygenation kinetics of YBCO films is limited by the surface exchange process of oxygen molecules prior to bulk diffusion into the films. The analysis of the temperature and oxygen partial pressure influence on the oxygenation kinetics has drawn a consistent picture of the oxygen surface exchange process enabling us to define the most likely rate determining step. We have also established a strategy to accelerate the oxygenation kinetics at low temperatures based on the catalytic influence of Ag coatings thus allowing us to decrease the oxygenation temperature in the YBCO thin films.

Surface coverage of Pt atoms on PtCo nanoparticles and catalytic kinetics for oxygen reduction

Energy Technology Data Exchange (ETDEWEB)

Jiang Rongzhong, E-mail: rongzhong.jiang@us.army.mi [Sensors and Electron Devices Directorate, U.S. Army Research Laboratory, 2800 Powder Mill Road, Adelphi, MD 20783-1197 (United States); Rong, Charles; Chu, Deryn [Sensors and Electron Devices Directorate, U.S. Army Research Laboratory, 2800 Powder Mill Road, Adelphi, MD 20783-1197 (United States)

2011-02-01

The surface coverage of Pt atoms on PtCo nanoparticles and its effect on catalytic kinetics for oxygen reduction were investigated. The PtCo nanoparticles with different surface coverage of Pt atoms were synthesized with various methods, including normal chemical method, microemulsion synthesis, and ultrasound-assisted microemulsion. A model of Pt atoms filling into a spherical nanoparticle was proposed to explain the relationship of surface metal atoms and nanoparticle size. The catalytic activity of the PtCo nano-particles is highly dependent on the synthetic methods, even if they have the same chemical composition. The PtCo nano-particles synthesized with ultrasound-assisted microemulsion showed the highest activity, which is attributed to an increase of active surface coverage of Pt atoms on the metal nanoparticles. The rate of oxygen reduction at 0.5 V (vs. SCE) catalyzed by the PtCo synthesized with ultrasound-assisted micro-emulsion was about four times higher than that of the PtCo synthesized with normal chemical method. As demonstrated with rotating-ring disk electrode measurement, the PtCo nano-particles can catalyze oxygen 4-electron reduction to water without intermediate H{sub 2}O{sub 2} detected.

Oxidative Corrosion of the UO ₂ (001) Surface by Nonclassical Diffusion

Energy Technology Data Exchange (ETDEWEB)

Stubbs, Joanne E.; Biwer, Craig A.; Chaka, Anne M. [Pacific Northwest; Ilton, Eugene S. [Pacific Northwest; Du, Yingge [Pacific Northwest; Bargar, John R. [Stanford Synchrotron; Eng, Peter J.

2017-11-07

Uranium oxide is central to every stage of the nuclear fuel cycle, from mining through fuel fabrication and use, to waste disposal and environmental cleanup. Its chemical and mechanical stability are intricately linked to the concentration of interstitial O atoms within the structure and the oxidation state of U. We have previously shown that during corrosion of the UO2 (111) surface under either 1 atm O2 gas or oxygenated water at room temperature, oxygen interstitials diffuse into the substrate to form a superlattice with three-layer periodicity. In the current study, we present results from surface x-ray scattering that reveal the structure of the oxygen diffusion profile beneath the (001) surface. The first few layers below the surface oscillate strongly in their surface-normal lattice parameters, suggesting preferential interstitial occupation of every other layer below the surface, which is geometrically consistent with the interstitial network that forms below the oxidized (111) surface. Deeper layers are heavily contracted and indicate that the oxidation front penetrates ~52 Å below the (001) surface after 21 days of dry O2 gas exposure at ambient pressure and temperature. X-ray photoelectron spectroscopy indicates U is present as U(IV), U(V), and U(VI).

On Traveling Waves in Lattices: The Case of Riccati Lattices

Science.gov (United States)

Dimitrova, Zlatinka

2012-09-01

The method of simplest equation is applied for analysis of a class of lattices described by differential-difference equations that admit traveling-wave solutions constructed on the basis of the solution of the Riccati equation. We denote such lattices as Riccati lattices. We search for Riccati lattices within two classes of lattices: generalized Lotka-Volterra lattices and generalized Holling lattices. We show that from the class of generalized Lotka-Volterra lattices only the Wadati lattice belongs to the class of Riccati lattices. Opposite to this many lattices from the Holling class are Riccati lattices. We construct exact traveling wave solutions on the basis of the solution of Riccati equation for three members of the class of generalized Holling lattices.

[Study on Square Super-Lattice Pattern with Surface Discharge in Dielectric Barrier Discharge by Optical Emission Spectra].

Science.gov (United States)

Niu, Xue-jiao; Dong, Li-fang; Liu, Ying; Wang, Qian; Feng, Jian-yu

2016-02-01

Square super-lattice pattern with surface discharge consisting of central spots and dim spots is firstly observed in the mixture of argon and air by using a dielectric barrier discharge device with water electrodes. By observing the image, it is found that the central spot is located at the centriod of its surrounding four dim spots. The short-exposure image recorded by a high speed video camera shows that the dim spot results from the surface discharges (SDs). The brightness of the central spot and is quite different from that of the dim spot, which indicates that the plasma states of the central spot and the dim spot may be differentiated. The optical emission spectrum method is used to further study the several plasma parameters of the central spot and the dim spot in different argon content. The emission spectra of the N₂ second positive band (C³IIu --> B³ IIg) are measured, from which the molecule vibration temperatures of the central spot and the dim spot are calculated respectively. The broadening of spectral line 696.57 nm (2P₂-->1S₅) is used to study the electron densities of the central spot and the dim spot. It is found that the molecule vibration temperature and electron density of the dim spot are higher than those of the central spot in the same argon content The molecule vibration temperature and electron density of the central spot and the dim spot increase with the argon content increasing from 90% to 99.9%. The surface discharge induced by the volume discharge (VD) has the determinative effect on the formation of the dim spot The experimental results above play an important role in studying the formation mechanism of surface discharg&of square super-lattice pattern with surface discharge. In addition, the studies exert an influence on the application of surface discharge and volume discharge in different fields.

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.

2018-06-01

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 and 100 K. After dosing the reactants on to 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.

LATTICE: an interactive lattice computer code

International Nuclear Information System (INIS)

Staples, J.

1976-10-01

LATTICE is a computer code which enables an interactive user to calculate the functions of a synchrotron lattice. This program satisfies the requirements at LBL for a simple interactive lattice program by borrowing ideas from both TRANSPORT and SYNCH. A fitting routine is included

Super-oxidation of silicon nanoclusters: magnetism and reactive oxygen species at the surface

Energy Technology Data Exchange (ETDEWEB)

Lepeshkin, Sergey; Baturin, Vladimir; Tikhonov, Evgeny; Matsko, Nikita; Uspenskii, Yurii; Naumova, Anastasia; Feya, Oleg; Schoonen, Martin A.; Oganov, Artem R.

2016-01-01

Oxidation of silicon nanoclusters depending on the temperature and oxygen pressure is explored from first principles using the evolutionary algorithm, and structural and thermodynamic analysis. From our calculations of 90 SinOm clusters we found that under normal conditions oxidation does not stop at the stoichiometric SiO2 composition, as it does in bulk silicon, but goes further placing extra oxygen atoms on the cluster surface. These extra atoms are responsible for light emission, relevant to reactive oxygen species and many of them are magnetic. We argue that the super-oxidation effect is size-independent and discuss its relevance to nanotechnology and miscellaneous applications, including biomedical ones.

Adsorption of atomic oxygen (N2O) on a clean Ge(001) surface

NARCIS (Netherlands)

Zandvliet, Henricus J.W.; Keim, Enrico G.; van Silfhout, Arend

1990-01-01

We present the results of a study concerning the interaction of atomic oxygen (as released by decomposition of N2O ) with the clean Ge(001)2×1 surface at 300 K. Ellipsometry in the photon energy range of 1.5–4 eV, surface conductance measurements and Auger electron spectroscopy(AES) have been used

Understanding lattice defects to influence ferromagnetic order of ZnO nanoparticles by Ni, Cu, Ce ions

Energy Technology Data Exchange (ETDEWEB)

Verma, Kuldeep Chand, E-mail: dkuldeep.physics@gmail.com [Department of Physics, Panjab University, Chandigarh 160014 (India); Kotnala, R.K., E-mail: rkkotnala@gmail.com [CSIR-National Physical Laboratory, New Delhi 110012 (India)

2017-02-15

Future spintronics technologies based on diluted magnetic semiconductors (DMS) will rely heavily on a sound understanding of the microscopic origins of ferromagnetism in such materials. It remains unclear, however, whether the ferromagnetism in DMS is intrinsic - a precondition for spintronics - or due to dopant clustering. For this, we include a simultaneous doping from transition metal (Ni, Cu) and rare earth (Ce) ions in ZnO nanoparticles that increase the antiferromagnetic ordering to achieve high-T{sub c} ferromagnetism. Rietveld refinement of XRD patterns indicate that the dopant ions in ZnO had a wurtzite structure and the dopants, Ni{sup 2+}, Cu{sup 2+}, Ce{sup 3+} ions, are highly influenced the lattice constants to induce lattice defects. The Ni, Cu, Ce ions in ZnO have nanoparticles formation than nanorods was observed in pure sample. FTIR involve some organic groups to induce lattice defects and the metal-oxygen bonding of Zn, Ni, Cu, Ce and O atoms to confirm wurtzite structure. Raman analysis evaluates the crystalline quality, structural disorder and defects in ZnO lattice with doping. Photoluminescence spectra have strong near-band-edge emission and visible emission bands responsible for defects due to oxygen vacancies. The energy band gap is calculated using Tauc relation. Room temperature ferromagnetism has been described due to bound magnetic polarons formation with Ni{sup 2+}, Cu{sup 2+}, Ce{sup 3+} ions in ZnO via oxygen vacancies. The zero field and field cooling SQUID measurement confirm the strength of antiferromagnetism in ZnO. The field cooling magnetization is studied by Curie-Weiss law that include antiferromagnetic interactions up to low temperature. The XPS spectra have involve +3/+4 oxidation states of Ce ions to influence the observed ferromagnetism. - Graphical abstract: The lattice defects/vacancies attributed by Ni and Ce ions in the wurtzite ZnO structure are responsible in high T{sub c} -ferromagnetism due to long-range magnetic

Lattice Waves, Spin Waves, and Neutron Scattering

Science.gov (United States)

Brockhouse, Bertram N.

1962-03-01

Use of neutron inelastic scattering to study the forces between atoms in solids is treated. One-phonon processes and lattice vibrations are discussed, and experiments that verified the existence of the quantum of lattice vibrations, the phonon, are reviewed. Dispersion curves, phonon frequencies and absorption, and models for dispersion calculations are discussed. Experiments on the crystal dynamics of metals are examined. Dispersion curves are presented and analyzed; theory of lattice dynamics is considered; effects of Fermi surfaces on dispersion curves; electron-phonon interactions, electronic structure influence on lattice vibrations, and phonon lifetimes are explored. The dispersion relation of spin waves in crystals and experiments in which dispersion curves for spin waves in Co-Fe alloy and magnons in magnetite were obtained and the reality of the magnon was demonstrated are discussed. (D.C.W)

Hydrogen, oxygen and hydroxyl on porous silicon surface: A joint density-functional perturbation theory and infrared spectroscopy approach

International Nuclear Information System (INIS)

Alfaro, Pedro; Palavicini, Alessio; Wang, Chumin

2014-01-01

Based on the density functional perturbation theory (DFPT), infrared absorption spectra of porous silicon are calculated by using an ordered pore model, in which columns of silicon atoms are removed along the [001] direction and dangling bonds are initially saturated with hydrogen atoms. When these atoms on the pore surface are gradually replaced by oxygen ones, the ab-initio infrared absorption spectra reveal oxygen, hydroxyl, and coupled hydrogen–oxygen vibrational modes. In a parallel way, freestanding porous silicon samples were prepared by using electrochemical etching and they were further thermally oxidized in a dry oxygen ambient. Fourier transform infrared spectroscopy was used to investigate the surface modifications caused by oxygen adsorption. In particular, the predicted hydroxyl and oxygen bound to the silicon pore surface are confirmed. Finally, a global analysis of measured transmittance spectra has been performed by means of a combined DFPT and thin-film optics approach. - Highlights: • The density functional perturbation theory is used to study infrared absorption. • An ordered pore model is used to investigate the oxidation in porous silicon (PSi). • Infrared transmittance spectra of oxidized PSi freestanding samples are measured

Modifying TiO{sub 2} surface architecture by oxygen plasma to increase dye sensitized solar cell efficiency

Energy Technology Data Exchange (ETDEWEB)

Rajmohan, Gayathri Devi [Institute for Frontier Materials, Deakin University, Geelong Waurn Ponds, Victoria 3216 (Australia); Dai, Xiujuan J., E-mail: jane.dai@deakin.edu.au [Institute for Frontier Materials, Deakin University, Geelong Waurn Ponds, Victoria 3216 (Australia); Tsuzuki, Takuya; Lamb, Peter R. [Institute for Frontier Materials, Deakin University, Geelong Waurn Ponds, Victoria 3216 (Australia); Plessis, Johan du [School of Applied Sciences, RMIT University, GPO Box 2476 V, Melbourne, Victoria 3001 (Australia); Huang, Fuzhi; Cheng, Yi-Bing [Department of Materials Engineering, Monash University, Melbourne, Victoria 3800 (Australia)

2013-10-31

Oxygen plasma treatment of TiO{sub 2} films has been used to improve the efficiency of dye sensitized solar cells. Both a commercial TiO{sub 2} sample and a TiO{sub 2} thin film synthesized by a sol-gel technique were treated using a custom built inductively coupled plasma apparatus. X-ray photoelectron spectroscopy revealed that oxygen-plasma treatment increased the number of oxygen functional groups (hydroxyl groups) and introduced some Ti{sup 3+} species on the surface of TiO{sub 2}. A sample solar cell with plasma treated TiO{sub 2} showed an overall solar-to-electricity conversion efficiency of 4.3%, about a 13% increase over untreated TiO{sub 2}. The photon conversion efficiency for the plasma treated TiO{sub 2} was 34% higher than untreated TiO{sub 2}. This enhanced cell-performance is partly due to increased dye adsorption from an increase in surface oxygen functional groups and also may be partly due to Ti{sup 3+} states on the surface of TiO{sub 2}. - Highlights: • Oxygen plasma is used to generate hydroxyl groups on the surface of TiO{sub 2} • Parallel study was conducted using a spin coated TiO{sub 2} and a Commercial TiO{sub 2} film. • The plasma functionalization caused increased dye uptake. • Some species in Ti{sup 3+} state are also generated after oxygen plasma. • Dye sensitised solar cell with functionalised electrode showed improved efficiency.

Fast MAS ¹H NMR Study of Water Adsorption and Dissociation on the (100) Surface of Ceria Nanocubes: A Fully Hydroxylated, Hydrophobic Ceria Surface

Energy Technology Data Exchange (ETDEWEB)

Gill, Lance [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Beste, Ariana [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Joint Institute for Computational Sciences (JIBS); Univ. of Tennessee, Knoxville, TN (United States); Chen, Banghao [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Li, Meijun [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Mann, Amanda K. P. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Overbury, Steven H. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Hagaman, Edward W. [Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division

2017-03-22

¹H nuclear magnetic resonance (NMR) spectroscopy was used to study hydroxylic surface species on ceria nanocubes, a crystalline, high-surface-area CeO₂ that presents mostly (100) facets. Water adsorption and desorption experiments in combination with fast magic angle spinning (MAS, 20–40 kHz) 1H NMR provide high-resolution ¹H spectra that allow the observation of ten resonance bands (water or hydroxyl) on or under the (100) surface. Assignments were made using a combination of adsorption and temperature-programmed desorption, quantitative spin counting, deuterium exchange, spin–lattice (T₁) and spin–spin (T₂) relaxation, and DFT calculations. In air, the (100) surface exists as a fully hydroxylated surface. Water adsorption and dissociation on dry ceria surfaces occur first at oxygen vacancies, but Ce³⁺ centers are not required since water dissociation is barrier-less on the fully oxidized surface. Surface $-$OH functionality occurs in two resolved bands representing isolated $-$OH (1 ppm) and hydrogen-bonded $-$OH (9 ppm), the latter being dominant. Deuterium exchange of surface hydroxyls with D₂O does not occur under mild or forcing conditions. Despite large differences in the T₁ of surface hydroxyls and physisorbed water, surface hydroxyl T₁ values are independent of the presence or absence of physisorbed water, demonstrating that the protons within these two functional group pools are not in intimate contact. These observations show that, once hydroxylated, the surface $-$OH functionality preferentially forms hydrogen bonds with surface lattice oxygen, i.e., the hydroxylated (100) surface of ceria is hydrophobic. Near this surface it is energetically more favorable for physisorbed water to hydrogen bond to itself rather than to the surface. DFT calculations support this notion. Impurity Na⁺ remaining in incompletely washed ceria nanocubes

Vortex solitons at the interface separating square and hexagonal lattices

Energy Technology Data Exchange (ETDEWEB)

Jović Savić, Dragana, E-mail: jovic@ipb.ac.rs; Piper, Aleksandra; Žikić, Radomir; Timotijević, Dejan

2015-06-19

Vortex solitons at the interface separating two different photonic lattices – square and hexagonal – are demonstrated numerically. We consider the conditions for the existence of discrete vortex states at such interfaces and develop a concise picture of different scenarios of the vortex solutions behavior. Various vortices with different size and topological charges are considered, as well as various lattice interfaces. A novel type of discrete vortex surface solitons in a form of five-lobe solution is observed. Besides stable three-lobe and six-lobe discrete surface modes propagating for long distances, we observe various oscillatory vortex surface solitons, as well as dynamical instabilities of different kinds of solutions and study their angular momentum. Dynamical instabilities occur for higher values of the propagation constant, or at higher beam powers. - Highlights: • We demonstrate vortex solitons at the square–hexagonal photonic lattice interface. • A novel type of five-lobe surface vortex solitons is observed. • Different phase structures of surface solutions are studied. • Orbital angular momentum transfer of such solutions is investigated.

Modulating Protein Adsorption on Oxygen Plasma Modified Polysiloxane Surfaces

International Nuclear Information System (INIS)

Marletta, G.

2006-01-01

In the present paper we report the study on the adsorption behaviour of three model globular proteins, Human Serum Albumin, Lactoferrin and Egg Chicken Lysozyme onto both unmodified surfaces of a silicon-based polymer and the corresponding plasma treated surfaces. In particular, thin films of hydrophobic polysiloxane (about 90 degree of static water contact angle, WCA) were converted by oxygen plasma treatment at reduced pressure into very hydrophilic phases of SiOx (WCA less than 5 degree). The kinetics of protein adsorption processes were investigated by QCM-D technique, while the chemical structure and topography of the protein adlayer have been studied by Angular resolved-XPS and AFM respectively. It turned out that Albumin and Lysozyme exhibited the opposite preferential adsorption respectively onto the hydrophobic and hydrophilic surfaces, while Lactoferrin did not exhibit significant differences. The observed protein behaviour are discussed both in terms of surface-dependent parameters, including surface free energy and chemical structure, and in terms of protein-dependent parameters, including charge as well as the average molecular orientation in the adlayers. Finally, some examples of differential adsorption behaviour of the investigated proteins are reported onto nanopatterned polysiloxane surfaces consisting of hydrophobic nanopores surrounded by hydrophilic (plasma-treated) matrix and the reverse

The effect of annealing ambient on surface segregation in indium implanted sapphire

International Nuclear Information System (INIS)

Sood, D.K.; Victoria University of Technology, Melbourne; Zhou, W.; Victoria University of Technology, Melbourne; Academia Sinica, Shanghai Institute of Metallurgy; Cao, D.X.; Victoria University of Technology, Melbourne; Academia Sinica, Shanghai, SH

1991-01-01

A systematic study of the effect of annealing ambient on both indium surface segregation and lattice damage recovery of single crystal Al 2 O 3 has been done by performing 1 hour anneals at 800 deg C for the samples identically implanted with indium ions at 100keV energy to a high dose of 5x10 16 ions/cm 2 . Following solid phase epitaxial re-crystallization of amorphous layer, the indium dopant shows rapid thermal migration. The indium redistribution consists of 2 parts: 1. appreciable broadening corresponding to diffusion within the amorphous layer, and 2. indium segregation to the free surface to form In 2 O 3 , or escape out of the surface to sublime into the surrounding ambient. Lattice damage recovery depends on indium concentration profile in amorphous layer of Al 2 O 3 which is directly influenced by the annealing ambient. It is confirmed that the presence of moisture or oxygen in annealing ambient results in In 2 O 3 formation on the surface. (author). 6 refs.; 3 figs.; 1 tab

Surface deformation caused by the Abrikosov vortex lattice

Czech Academy of Sciences Publication Activity Database

Lipavský, Pavel; Morawetz, K.; Koláček, Jan; Brandt, E. H.

2008-01-01

Roč. 77, č. 18 (2008), 184509/1-184509/7 ISSN 1098-0121 R&D Projects: GA ČR GA202/08/0326; GA AV ČR IAA100100712 Grant - others:GA ČR(CZ) GA202/07/0597 Institutional research plan: CEZ:AV0Z10100521 Keywords : superconductivity * magneto-elastic effect * vortex lattice Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 3.322, year: 2008

Surface modification of electrospun fibre meshes by oxygen plasma for bone regeneration

International Nuclear Information System (INIS)

Nandakumar, A; Tahmasebi Birgani, Z; Santos, D; Mentink, A; Auffermann, N; Moroni, L; Van Blitterswijk, C; Habibovic, P; Van der Werf, K; Bennink, M

2013-01-01

Plasma treatment is a method to modify the physicochemical properties of biomaterials, which consequently may affect interactions with cells. Based on the rationale that physical cues on the surface of culture substrates and implants, such as surface roughness, have proven to alter cell behaviour, we used electrospinning to fabricate fibrous three-dimensional scaffolds made of a poly (ethylene oxide terephthalate)/poly (butylene terephthalate) copolymer to mimic the physical microenvironment of extracellular matrix and applied radio-frequency oxygen plasma treatment to create nanoscale roughness. Scanning electron microscopy (SEM) analysis revealed a fibre diameter of 5.49 ± 0.96 µm for as-spun meshes. Atomic force microscopy (AFM) measurements determined an exponential increase of surface roughness with plasma treatment time. An increase in hydrophilicity after plasma treatment was observed, which was associated with higher oxygen content in plasma treated scaffolds compared to untreated ones. A more pronounced adsorption of bovine serum albumin occurred on scaffolds treated with plasma for 15 and 30 min compared to untreated fibres. Clinically relevant human mesenchymal stromal cells (hMSCs) were cultured on untreated, 15 and 30 min treated scaffolds. SEM analysis confirmed cell attachment and a pronounced spindle-like morphology on all scaffolds. No significant differences were observed between different scaffolds regarding the amount of DNA, metabolic activity and alkaline phosphatase (ALP) activity after 7 days of culture. The amount of ALP positive cells increased between 7 and 21 days of culture on both untreated and 30 min treated meshes. In addition, ALP staining of cells on plasma treated meshes appeared more pronounced than on untreated meshes after 21 days of culture. Quantitative polymerase chain reaction showed significant upregulation of bone sialoprotein and osteonectin expression on oxygen plasma treated fibres compared to untreated fibres in

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.

Strontium-free rare earth perovskite ferrites with fast oxygen exchange kinetics: Experiment and theory

Science.gov (United States)

Berger, Christian; Bucher, Edith; Windischbacher, Andreas; Boese, A. Daniel; Sitte, Werner

2018-03-01

The Sr-free mixed ionic electronic conducting perovskites La0.8Ca0.2FeO3-δ (LCF82) and Pr0.8Ca0.2FeO3-δ (PCF82) were synthesized via a glycine-nitrate process. Crystal structure, phase purity, and lattice constants were determined by XRD and Rietveld analysis. The oxygen exchange kinetics and the electronic conductivity were obtained from in-situ dc-conductivity relaxation experiments at 600-800 °C and 1×10-3≤pO2/bar≤0.1. Both LCF82 and PCF82 show exceptionally fast chemical surface exchange coefficients and chemical diffusion coefficients of oxygen. The oxygen nonstochiometry of LCF82 and PCF82 was determined by precision thermogravimetry. A point defect model was used to calculate the thermodynamic factors of oxygen and to estimate self-diffusion coefficients and ionic conductivities. Density Functional Theory (DFT) calculations on the crystal structure, oxygen vacancy formation as well as oxygen migration energies are in excellent agreement with the experimental values. Due to their favourable properties both LCF82 and PCF82 are of interest for applications in solid oxide fuel cell cathodes, solid oxide electrolyser cell anodes, oxygen separation membranes, catalysts, or electrochemical sensors.

The dynamics of ultraviolet-induced oxygen vacancy at the surface of insulating SrTiO_3(0 0 1)

International Nuclear Information System (INIS)

Suwanwong, S.; Eknapakul, T.; Rattanachai, Y.; Masingboon, C.; Rattanasuporn, S.; Phatthanakun, R.; Nakajima, H.; King, P.D.C.; Hodak, S.K.; Meevasana, W.

2015-01-01

Highlights: • The dynamics of UV-induced oxygen vacancy is studied from the change of surface resistance. • The formation of 2DEG at the insulating surface of SrTiO_3 is confirmed by ARPES. • The UV-induced change in resistance responds differently to oxygen/gas exposure. • The behavior of resistance recovery suggests an alternative method of low-pressure sensing. - Abstract: The effect of ultra-violet (UV) irradiation on the electronic structure and the surface resistance of an insulating SrTiO_3(0 0 1) crystal is studied in this work. Upon UV irradiation, we show that the two-dimensional electron gas (2DEG) emerges at the insulating SrTiO_3 surface and there is a pronounced change in the surface resistance. By combining the observations of the change in valance band and the resistance change under different environments of gas pressure and gas species, we find that UV-induced oxygen vacancies at the surface plays a major role in the resistance change. The dynamic of the resistance change at different oxygen pressures also suggests an alternative method of low-pressure sensing.

Improvement of Surface Wettability and Hydrophilization of Poly-paraphenylene benzobisoxazole Fiber with Fibrillation Combined Oxygen Plasma Treatment

Directory of Open Access Journals (Sweden)

Xiwen Wang

2012-01-01

Full Text Available A new surface modification method fibrillation combined with oxygen plasma treatment to improve the wettability and hydrophily of PBO fiber was studied in this paper. The surface chemical structure and morphology of PBO fiber were characterized by the methods of FTIR, XPS and SEM. The wettability and hydrophlic characters changes on the surface were evaluated by the dynamic contact angle system and image analysis. The results show that the increase surface roughness by fibrillation could improve the wettability. Fibrillation combined oxygen plasma treatment has a better effect than oxygen plasma treatment to improve the wettability and hdyrophlization of PBO fiber. The specific area of PBO fiber increased to 10.7 m2/g from 0.7 m2/g, contact angle decreased to 43.2° from 84.4° and WRV increased to 208.4% from 13.7%. The modified fibers have a good dispersion in water for hydrophilization improvement.

Molecular simulation insights on the in vacuo adsorption of amino acids on graphene oxide surfaces with varying surface oxygen densities

Energy Technology Data Exchange (ETDEWEB)

Rahmani, Farzin; Nouranian, Sasan, E-mail: sasan@olemiss.edu; Mahdavi, Mina [University of Mississippi, Department of Chemical Engineering (United States); Al-Ostaz, Ahmed [University of Mississippi, Department of Civil Engineering (United States)

2016-11-15

In this fundamental study, a series of molecular dynamics simulations were performed in vacuo to investigate the energetics and select geometries of 20 standard amino acids (AAs) on pristine graphene (PG) and graphene oxide (GO) surfaces as a function of graphene surface oxygen density. These interactions are of key interest to graphene/biomolecular systems. Our results indicate that aromatic AAs exhibit the strongest total interactions with the PG surfaces due to π-π stacking. Tryptophan (Trp) has the highest aromaticity due to its indole side chain and, hence, has the strongest interaction among all AAs (−16.66 kcal/mol). Aliphatic, polar, and charged AAs show various levels of affinity to the PG sheets depending on the strength of their side chain hydrophobic interactions. For example, arginine (Arg) with its guanidinium side chain exhibits the strongest interaction with the PG sheets (−13.81 kcal/mol) following aromatic AAs. Also, glycine (Gly; a polar AA) has the weakest interaction with the PG sheets (−7.29 kcal/mol). When oxygen-containing functional groups are added to the graphene sheets, the π-π stacking in aromatic AAs becomes disrupted and perfect parallelism of the aromatic rings is lost. Moreover, hydrogen bonding and/or electrostatic interactions become more pronounced. Charged AAs exhibit the strongest interactions with the GO surfaces. In general, the AA-GO interactions increase with increasing surface oxygen density, and the effect is more pronounced at higher O/C ratios. This study provides a quantitative measure of AA-graphene interactions for the design and tuning of biomolecular systems suitable for biosensing, drug delivery, and gene delivery applications.

TPD and XPS study on thermal behavior of absorbed oxygen in La sub(1-x)Sr sub(x)CoO/sub 3/

Energy Technology Data Exchange (ETDEWEB)

Yamazoe, N; Teraoka, Y; Seiyama, T [Kyushu Univ., Fukuoka (Japan). Faculty of Engineering

1981-12-01

Two types of oxygen desorption from La sub(1-x)Sr sub(x)CoO/sub 3/ were revealed by the appearance of a broad desorption peak (..cap alpha..) below ca. 800/sup 0/C and a sharp one (..beta..) around 820/sup 0/C. The binding energy of O is level for absorbed oxygen was clearly different from that for lattice oxygen. Close examination shows that ..cap alpha.. is ascribable to the desorption of the absorbed oxygen while ..beta.. may be the desorption of a part of lattice oxygen.

Lattice Gas Model Based Optimization of Plasma-Surface Processes for GaN-Based Compound Growth

Science.gov (United States)

Nonokawa, Kiyohide; Suzuki, Takuma; Kitamori, Kazutaka; Sawada, Takayuki

2001-10-01

Progress of the epitaxial growth technique for GaN-based compounds makes these materials attractive for applications in high temperature/high-power electronic devices as well as in short-wavelength optoelectronic devices. For MBE growth of GaN epilayer, atomic nitrogen is usually supplied from ECR-plasma while atomic Ga is supplied from conventional K-cell. To grow high-quality epilayer, fundamental knowledge of the detailed atomic process, such as adsorption, surface migration, incorporation, desorption and so forth, is required. We have studied the influence of growth conditions on the flatness of the growth front surface and the growth rate using Monte Carlo simulation based on the lattice gas model. Under the fixed Ga flux condition, the lower the nitrogen flux and/or the higher the growth temperature, the better the flatness of the front surface at the sacrifice of the growth rate of the epilayer. When the nitrogen flux is increased, the growth rate reaches saturation value determined from the Ga flux. At a fixed growth temperature, increasing of nitrogen to Ga flux ratio results in rough surface owing to 3-dimensional island formation. Other characteristics of MBE-GaN growth using ECR-plasma can be well reproduced.

On techniques of ATR lattice computation

International Nuclear Information System (INIS)

1997-08-01

Lattice computation is to compute the average nuclear constants of unit fuel lattice which are required for computing core nuclear characteristics such as core power distribution and reactivity characteristics. The main nuclear constants are infinite multiplying rate, neutron movement area, cross section for diffusion computation, local power distribution and isotope composition. As for the lattice computation code, WIMS-ATR is used, which is based on the WIMS-D code developed in U.K., and for the purpose of heightening the accuracy of analysis, which was improved by adding heavy water scattering cross section considering the temperature dependence by Honeck model. For the computation of the neutron absorption by control rods, LOIEL BLUE code is used. The extrapolation distance of neutron flux on control rod surfaces is computed by using THERMOS and DTF codes, and the lattice constants of adjoining lattices are computed by using the WIMS-ATR code. As for the WIMS-ATR code, the computation flow and nuclear data library, and as for the LOIEL BLUE code, the computation flow are explained. The local power distribution in fuel assemblies determined by the WIMS-ATR code was verified with the measured data, and the results are reported. (K.I.)

Chemisorption of oxygen and subsequent reactions on low index surfaces of β-Mo₂C

DEFF Research Database (Denmark)

Shi, Xue Rong; Wang, Shengguang; Wang, Jianguo

2016-01-01

to the carbon vacancy were identified. We examined the effect of oxygen coverage on the morphology of β-Mo2C by plotting the equilibrium crystal shape. Thermodynamic effect of temperature and reactant or product pressure on the CO/CO2 desorption were investigated. The CO/CO2 desorption is more favorable...... at the saturated oxygen coverage than the low oxygen coverage thermodynamically. The subsequent oxygen diffusion to the carbon vacancy after CO/CO2 desorption may happen depending on the surfaces and oxygen coverage....

Three-dimensional CaP/gelatin lattice scaffolds with integrated osteoinductive surface topographies for bone tissue engineering

International Nuclear Information System (INIS)

Nadeem, Danish; Su, Bo; Smith, Carol-Anne; Dalby, Matthew J; Dominic Meek, R M; Lin, Sien; Li, Gang

2015-01-01

Surface topography is known to influence stem cells and has been widely used as physical stimuli to modulate cellular behaviour including adhesion, proliferation and differentiation on 2D surfaces. Integration of well-defined surface topography into three-dimensional (3D) scaffolds for tissue engineering would be useful to direct the cell fate for intended applications. Technical challenges are remaining as how to fabricate such 3D scaffolds with controlled surface topography from a range of biodegradable and biocompatible materials. In this paper, a novel fabrication process using computer numerically controlled machining and lamination is reported to make 3D calcium phosphate/gelatin composite scaffolds with integrated surface micropatterns that are introduced by embossing prior to machining. Geometric analysis shows that this method is versatile and can be used to make a wide range of lattices with porosities that meet the basic requirements for bone tissue engineering. Both in vitro and in vivo studies show that micropatterned composite scaffolds with surfaces comprising 40 μm pits and 50 μm grooves were optimal for improved osteogenesis. The results have demonstrated the potential of a novel fabrication process for producing cell-instructive scaffolds with designed surface topographies to induce specific tissue regeneration. (paper)

Lateral ordering of PTCDA on the clean and the oxygen pre-covered Cu(100) surface investigated by scanning tunneling microscopy and low energy electron diffraction.

Science.gov (United States)

Gärtner, Stefan; Fiedler, Benjamin; Bauer, Oliver; Marele, Antonela; Sokolowski, Moritz M

2014-01-01

We have investigated the adsorption of perylene-3,4,9,10-tetracarboxylic acid dianhydride (PTCDA) on the clean and on the oxygen pre-covered Cu(100) surface [referred to as (√2 × 2√2)R45° - 2O/Cu(100)] by scanning tunneling microscopy (STM) and low energy electron diffraction (LEED). Our results confirm the (4√2 × 5√2)R45° superstructure of PTCDA/Cu(100) reported by A. Schmidt et al. [J. Phys. Chem. 1995, 99,11770-11779]. However, contrary to Schmidt et al., we have no indication for a dissociation of the PTCDA upon adsorption, and we propose a detailed structure model with two intact PTCDA molecules within the unit cell. Domains of high lateral order are obtained, if the deposition is performed at 400 K. For deposition at room temperature, a significant density of nucleation defects is found pointing to a strong interaction of PTCDA with Cu(100). Quite differently, after preadsorption of oxygen and formation of the (√2 × 2√2)R45° - 2O/Cu(100) superstructure on Cu(100), PTCDA forms an incommensurate monolayer with a structure that corresponds well to that of PTCDA bulk lattice planes.

Lateral ordering of PTCDA on the clean and the oxygen pre-covered Cu(100 surface investigated by scanning tunneling microscopy and low energy electron diffraction

Directory of Open Access Journals (Sweden)

Stefan Gärtner

2014-09-01

Full Text Available We have investigated the adsorption of perylene-3,4,9,10-tetracarboxylic acid dianhydride (PTCDA on the clean and on the oxygen pre-covered Cu(100 surface [referred to as (√2 × 2√2R45° – 2O/Cu(100] by scanning tunneling microscopy (STM and low energy electron diffraction (LEED. Our results confirm the (4√2 × 5√2R45° superstructure of PTCDA/Cu(100 reported by A. Schmidt et al. [J. Phys. Chem. 1995, 99,11770–11779]. However, contrary to Schmidt et al., we have no indication for a dissociation of the PTCDA upon adsorption, and we propose a detailed structure model with two intact PTCDA molecules within the unit cell. Domains of high lateral order are obtained, if the deposition is performed at 400 K. For deposition at room temperature, a significant density of nucleation defects is found pointing to a strong interaction of PTCDA with Cu(100. Quite differently, after preadsorption of oxygen and formation of the (√2 × 2√2R45° – 2O/Cu(100 superstructure on Cu(100, PTCDA forms an incommensurate monolayer with a structure that corresponds well to that of PTCDA bulk lattice planes.

Magnetic susceptibility of oxygen adsorbed on the surface of spherical and fibrous activated carbon.

Directory of Open Access Journals (Sweden)

Kiyoshi Kawamura

2009-02-01

Full Text Available The magnetic susceptibilities of oxygen adsorbed on the surface of bead-shaped activated carbon and activated carbon fibers were evaluated as a function of temperature between 4.2 K and 300 K, and found to exhibit a sharp peak at around 50 K. This implies that the adsorbed oxygen molecules form an antiferromagnetic state. The relation between the susceptibility and the adsorbed mass suggest that the thickness of the adsorbed oxygen is thin enough to consider a two-dimensional structure for bead–shaped activated carbon and carbon fibers across the fiber axis but thick enough to regard it as three-dimensional along the fiber axis. The result is discussed with reference to the study on one-dimensional oxygen array.

Surface layer composition of titania produced by various methods. The change of layer state under illumination

International Nuclear Information System (INIS)

Zakharenko, V; Daibova, E; Zmeeva, O; Kosova, N

2016-01-01

The comparative analysis of experimental data over titanium dioxide powders prepared by various ways under ambient air is carried out. The results over TiO 2 prepared by high-temperature heating of anatase, produced by burning of titanium micro particles and grinding of rutile crystal are used for that comparison. Water and carbon dioxide were the main products released from the surface of the titania powders. It was found that under UV irradiation absorbed by titania, in absent oxygen, water effectively reacts with lattice oxygen of titanium dioxide. (paper)

Surface strontium enrichment on highly active perovskites for oxygen electrocatalysis in solid oxide fuel cells

KAUST Repository

Crumlin, Ethan J.; Mutoro, Eva; Liu, Zhi; Grass, Michael E.; Biegalski, Michael D.; Lee, Yueh-Lin; Morgan, Dane; Christen, Hans M.; Bluhm, Hendrik; Shao-Horn, Yang

2012-01-01

Perovskite oxides have high catalytic activities for oxygen electrocatalysis competitive to platinum at elevated temperatures. However, little is known about the oxide surface chemistry that influences the activity near ambient oxygen partial pressures, which hampers the design of highly active catalysts for many clean-energy technologies such as solid oxide fuel cells. Using in situ synchrotron-based, ambient pressure X-ray photoelectron spectroscopy to study the surface chemistry changes, we show that the coverage of surface secondary phases on a (001)-oriented La 0.8Sr 0.2CoO 3-δ (LSC) film becomes smaller than that on an LSC powder pellet at elevated temperatures. In addition, strontium (Sr) in the perovskite structure enriches towards the film surface in contrast to the pellet having no detectable changes with increasing temperature. We propose that the ability to reduce surface secondary phases and develop Sr-enriched perovskite surfaces of the LSC film contributes to its enhanced activity for O 2 electrocatalysis relative to LSC powder-based electrodes. © 2012 The Royal Society of Chemistry.

Lattice-Boltzmann simulations of droplet evaporation

KAUST Repository

Ledesma-Aguilar, Rodrigo; Vella, Dominic; Yeomans, Julia M.

2014-01-01

© the Partner Organisations 2014. We study the utility and validity of lattice-Boltzmann (LB) simulations to explore droplet evaporation driven by a concentration gradient. Using a binary-fluid lattice-Boltzmann algorithm based on Cahn-Hilliard dynamics, we study the evaporation of planar films and 3D sessile droplets from smooth solid surfaces. Our results show that LB simulations accurately reproduce the classical regime of quasi-static dynamics. Beyond this limit, we show that the algorithm can be used to explore regimes where the evaporative and diffusive timescales are not widely separated, and to include the effect of boundaries of prescribed driving concentration. We illustrate the method by considering the evaporation of a droplet from a solid surface that is chemically patterned with hydrophilic and hydrophobic stripes. This journal is

Lattice-Boltzmann simulations of droplet evaporation

KAUST Repository

Ledesma-Aguilar, Rodrigo

2014-09-04

© the Partner Organisations 2014. We study the utility and validity of lattice-Boltzmann (LB) simulations to explore droplet evaporation driven by a concentration gradient. Using a binary-fluid lattice-Boltzmann algorithm based on Cahn-Hilliard dynamics, we study the evaporation of planar films and 3D sessile droplets from smooth solid surfaces. Our results show that LB simulations accurately reproduce the classical regime of quasi-static dynamics. Beyond this limit, we show that the algorithm can be used to explore regimes where the evaporative and diffusive timescales are not widely separated, and to include the effect of boundaries of prescribed driving concentration. We illustrate the method by considering the evaporation of a droplet from a solid surface that is chemically patterned with hydrophilic and hydrophobic stripes. This journal is

Surface adsorption of lattice HP proteins: Thermodynamics and structural transitions using Wang-Landau sampling

International Nuclear Information System (INIS)

Li Yingwai; Landau, David P; Wüst, Thomas

2012-01-01

Wang-Landau sampling has been applied to investigate the thermodynamics and structural properties of a lattice hydrophobic-polar heteropolymer (the HP protein model) interacting with an attractive substrate. For simplicity, we consider a short HP sequence consisting of only 36 monomers interacting with a substrate which attracts all monomers in the sequence. The conformational “phase transitions” have been identified by a canonical analysis of the specific heat and suitable structural observables. Three major “transitions”, namely, adsorption, hydrophobic core formation and “flattening” of adsorbed structures, are observed. Depending on the surface attractive strength relative to the intra-protein attraction among the H monomers, these processes take place in different sequences upon cooling.

Work function modifications of graphite surface via oxygen plasma treatment

Science.gov (United States)

Duch, J.; Kubisiak, P.; Adolfsson, K. H.; Hakkarainen, M.; Golda-Cepa, M.; Kotarba, A.

2017-10-01

The surface modification of graphite by oxygen plasma was investigated experimentally (X-ray diffraction, nanoparticle tracking analysis, laser desorption ionization mass spectrometry, thermogravimetry, water contact angle) and by molecular modelling (Density Functional Theory). Generation of surface functional groups (mainly sbnd OHsurf) leads to substantial changes in electrodonor properties and wettability gauged by work function and water contact angle, respectively. The invoked modifications were analyzed in terms of Helmholtz model taking into account the theoretically determined surface dipole moment of graphite-OHsurf system (μ = 2.71 D) and experimentally measured work function increase (from 0.75 to 1.02 eV) to determine the sbnd OH surface coverage (from 0.70 to 1.03 × 1014 groups cm-2). Since the plasma treatment was confined to the surface, the high thermal stability of the graphite material was preserved as revealed by the thermogravimetric analysis. The obtained results provide a suitable quantitative background for tuning the key operating parameters of carbon electrodes: electronic properties, interaction with water and thermal stability.

Impurities of oxygen in silicon

International Nuclear Information System (INIS)

Gomes, V.M.S.

1985-01-01

The electronic structure of oxygen complex defects in silicon, using molecular cluster model with saturation by watson sphere into the formalism of Xα multiple scattering method is studied. A systematic study of the simulation of perfect silicon crystal and an analysis of the increasing of atom number in the clusters are done to choose the suitable cluster for the calculations. The divacancy in three charge states (Si:V 2 + , Si:V 2 0 , Si:V 2 - ), of the oxygen pair (Si:O 2 ) and the oxygen-vacancy pair (Si:O.V) neighbours in the silicon lattice, is studied. Distortions for the symmetry were included in the Si:V 2 + and Si:O 2 systems. The behavior of defect levels related to the cluster size of Si:V 2 0 and Si:O 2 systems, the insulated oxygen impurity of silicon in interstitial position (Si:O i ), and the complexes involving four oxygen atoms are analysed. (M.C.K.) [pt

Optical characterization of surface and interface oxygen content in YBa2Cu3O/sub x/

International Nuclear Information System (INIS)

Kelly, M.K.; Chan, S.; Jenkin, K. II; Aspnes, D.E.; Barboux, P.; Tarascon, J.

1988-01-01

Because YBa 2 Cu 3 O/sub x/ exists over a range of oxygen content and low oxygen material is nonsuperconducting, it is important to be able to measure and control this parameter for application purposes. We present an optical technique for determining oxygen loss at surfaces and interfaces, where processing and contacts with other materials may affect composition and where usual techniques are insensitive. Using a strong absorption feature at 4.1 eV which appears at low oxygen composition, we find that overlayers of Al and In remove oxygen from YBa 2 Cu 3 O/sub x/, but Ag, Au, and room-temperature exposure to moderate vacuum do not

Multisite Interactions in Lattice-Gas Models

Science.gov (United States)

Einstein, T. L.; Sathiyanarayanan, R.

For detailed applications of lattice-gas models to surface systems, multisite interactions often play at least as significant a role as interactions between pairs of adatoms that are separated by a few lattice spacings. We recall that trio (3-adatom, non-pairwise) interactions do not inevitably create phase boundary asymmetries about half coverage. We discuss a sophisticated application to an experimental system and describe refinements in extracting lattice-gas energies from calculations of total energies of several different ordered overlayers. We describe how lateral relaxations complicate matters when there is direct interaction between the adatoms, an issue that is important when examining the angular dependence of step line tensions. We discuss the connector model as an alternative viewpoint and close with a brief account of recent work on organic molecule overlayers.

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

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...

Plasma etching to enhance the surface insulating stability of alumina for fusion applications

Directory of Open Access Journals (Sweden)

M. Malo

2016-12-01

Full Text Available A significant increase in the surface electrical conductivity of alumina, considered one of the most promising insulating materials for numerous applications in fusion devices, has been observed during ion bombardment in vacuum due to oxygen loss by preferential sputtering. Although this is expected to cause serious limitations to insulating components functionality, recent studies showed it is possible to restore the damaged lattice by oxygen reincorporation during thermal treatments in air. These studies also revealed a correlation between conductivity and ion beam induced luminescence, which is being used to monitor surface electrical conductivity degradation and help qualify the post irradiation recovery. Work now carried out for Wesgo alumina considers oxygen implantation and plasma etching as additional methods to improve recovered layer depth and quality. Both conductivity and luminescence results indicate the potential use of plasma etching not only for damage recovery, but also as a pre-treatment to enhance material stability during irradiation.

ΔM/sub j/ transitions in homonuclear molecule scattering off corrugated surfaces. Square and rectangular lattice symmetry and purely repulsive interaction

International Nuclear Information System (INIS)

Proctor, T.R.; Kouri, D.J.; Gerber, R.B.

1984-01-01

In this paper, we present the first formal and computational studies of Δm/sub j/ transitions occurring in homonuclear molecule-corrugated surface collisions. The model potential is a pairwise additive one which correctly incorporates the fact that Δm/sub j/ transitions occur only for corrugated surfaces (provided the quantization axis is chosen to be the average surface normal). The principal results are: (a) Δm/sub j/ transitions are extremely sensitive to lattice symmetry; (b) strong selection rules obtain for specular scattering; (c) the magnitude of Δm/sub j/ -transition probabilities are strongly sensitive to surface corrugation; (d) the Δm/sub j/ transitions depend strongly on diffraction peak; (e) the ratio of molecular length to lattice dimension (r/a) has a strong influence on the magnitude of Δm/sub j/ -transition probabilities [with the probabilities increasing as (r/a) increases]; (f) Δm/sub j/ rainbows are predicted to occur as a function of the (r/a) ratio increases; (g) Δm/sub j/ transitions and the Δm/sub j/ rainbow are expected to accompany Δj-rotational rainbows; (h) such magnetic transition rainbows accompanying Δj rainbows are suggested as an explanation of recent experimental observations of quenching of NO polarization for larger Δj transitions in NO/Ag(111) scattering

Lattice QCD

International Nuclear Information System (INIS)

Hasenfratz, P.

1983-01-01

The author presents a general introduction to lattice gauge theories and discusses non-perturbative methods in the gauge sector. He then shows how the lattice works in obtaining the string tension in SU(2). Lattice QCD at finite physical temperature is discussed. Universality tests in SU(2) lattice QCD are presented. SU(3) pure gauge theory is briefly dealt with. Finally, fermions on the lattice are considered. (Auth.)

Dissolution kinetics of small amounts of oxygen in tantalum alloy T-111 and internal oxide displacement reactions during annealing

Science.gov (United States)

Stecura, S.

1976-01-01

Oxygen was added to T-111 (Ta-8W-2Hf, wt. %) at 820 and 990 C at an oxygen pressure of about 0.0003 torr. The technique employed permitted predetermined and reproducible doping of T-111 up to 3.0 at. % oxygen. Based on the temperature dependence of the doping reaction, it is concluded that the initial rates of oxygen pickup are probably controlled by solution of oxygen into the T-111 lattice. Although hafnium oxides are more stable than those of tantalum or tungsten, analyses of extracted residues indicate that the latter oxides predominate in the as-doped specimens, presumably because of the higher concentrations of tantalum and tungsten in the alloy. However, high-temperature annealing promotes gettering of dissolved oxygen and of other oxides to form hafnium oxides. Small amounts of tantalum and tungsten oxides were still present after high-temperature annealing. Tungsten oxide (WO3) volatilizes slightly from the surface of T-111 at 990 C. The vaporization of WO3 has no apparent affect on the doping reaction.

The surface structure of SrTiO{sub 3} at high temperatures under influence of oxygen

Energy Technology Data Exchange (ETDEWEB)

Hesselberth, M. B. S.; Molen, S. J. van der; Aarts, J. [Kamerlingh Onnes Laboratory, Leiden University, P.O. Box 9504, 2300 RA Leiden (Netherlands)

2014-02-03

We use low energy electron microscopy to investigate the structure of the SrTiO{sub 3} (001) surface at elevated temperatures and different oxygen pressures. Upon varying the temperature between 500 °C and 900 °C in oxygen pressures ranging from 10{sup −9} millibar to 10{sup −4} millibar, two surface transitions are found to be present. The lower temperature (1 × 1) → (2 × 1) transition that is known to occur in ultrahigh vacuum can be reversed by increasing the oxygen pressure. At higher temperatures, we observe a (2 × 1) → disordered (1 × 1) transition which is irreversible in the experimental parameter range. The observations are expected to have a strong bearing on the growth of interface structures.

Screening of NiFe₂O₄ Nanoparticles as Oxygen Carrier in Chemical Looping Hydrogen Production

DEFF Research Database (Denmark)

Liu, Shuai; He, Fang; Huang, Zhen

2016-01-01

) methods were used to prepare NiFe2O4 oxygen carriers. Samples were characterized by X-ray diffraction (XRD), Raman spectroscopy, scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), Brunauer-Emmett-Teller (BET) surface area measurement, as well as Barrett-Joyner-Halenda (BJH......The objective of this paper is to systematically investigate the influences of different preparation methods on the properties of NiFe2O4 nanoparticles as oxygen carrier in chemical looping hydrogen production (CLH). The solid state (SS), coprecipitation (CP), hydrothermal (HT), and sol-gel (SG...... gas (24% H2 + 24% CO + 12% CO2 + N2 balance), then reacted with steam to produce H2, and finally fully oxidized by air. The NiFe2O4 oxygen carrier prepared by the sol gel method showed the best capacity for hydrogen production and the highest recovery degree of lattice oxygen, in agreement...

Surface-Selective Preferential Production of Reactive Oxygen Species on Piezoelectric Ceramics for Bacterial Killing

OpenAIRE

Tan, Guoxin; Wang, Shuangying; Zhu, Ye; Zhou, Lei; Yu, Peng; Wang, Xiaolan; He, Tianrui; Chen, Junqi; Mao, Chuanbin; Ning, Chengyun

2016-01-01

Reactive oxygen species (ROS) can be used to kill bacterial cells, and thus the selective generation of ROS from material surfaces is an emerging direction in antibacterial material discovery. We found the polarization of piezoelectric ceramic causes the two sides of the disk to become positively and negatively charged, which translate into cathode and anode surfaces in an aqueous solution. Because of the microelectrolysis of water, ROS are preferentially formed on the cathode surface. Conseq...

Evolution Of Lattice Structure And Chemical Composition Of The Surface Reconstruction Layer In Li1.2Ni0.2Mn0.6O2 Cathode Material For Lithium Ion Batteries

Energy Technology Data Exchange (ETDEWEB)

Yan, Pengfei; Nie, Anmin; Zheng, Jianming; Zhou, Yungang; Lu, Dongping; Zhang, Xiaofeng; Xu, Rui; Belharouak, Ilias; Zu, Xiaotao; Xiao, Jie; Amine, Khalil; Liu, Jun; Gao, Fei; Shahbazian-Yassar, Reza; Zhang, Jiguang; Wang, Chong M.

2015-01-14

Voltage and capacity fading of layer structured lithium and manganese rich (LMR) transition metal oxide is directly related to the structural and composition evolution of the material during the cycling of the battery. However, understanding such evolution at atomic level remains elusive. Based on atomic level structural imaging, elemental mapping of the pristine and cycled samples and density functional theory calculations, it is found that accompanying the hoping of Li ions is the simultaneous migration of Ni ions towards the surface from the bulk lattice, leading to the gradual depletion of Ni in the bulk lattice and thickening of a Ni enriched surface reconstruction layer (SRL). Furthermore, Ni and Mn also exhibit concentration partitions within the thin layer of SRL in the cycled samples where Ni is almost depleted at the very surface of the SRL, indicating the preferential dissolution of Ni ions in the electrolyte. Accompanying the elemental composition evolution, significant structural evolution is also observed and identified as a sequential phase transition of C2/m →I41→Spinel. For the first time, it is found that the surface facet terminated with pure cation is more stable than that with a mixture of cation and anion. These findings firmly established how the elemental species in the lattice of LMR cathode transfer from the bulk lattice to surface layer and further into the electrolyte, clarifying the long standing confusion and debate on the structure and chemistry of the surface layer and their correlation with the voltage fading and capacity decaying of LMR cathode. Therefore, this work provides critical insights for designing of cathode materials with both high capacity and voltage stability during cycling.

The dynamics of ultraviolet-induced oxygen vacancy at the surface of insulating SrTiO{sub 3}(0 0 1)

Energy Technology Data Exchange (ETDEWEB)

Suwanwong, S. [School of Physics, Suranaree University of Technology, Nakhon Ratchasima 30000 (Thailand); Program in General Science Teaching, Faculty of Education, Vongchavalitkul University, Nakhon Ratchasima 30000 (Thailand); Eknapakul, T. [School of Physics, Suranaree University of Technology, Nakhon Ratchasima 30000 (Thailand); Rattanachai, Y. [Department of Applied Physics, Faculty of Sciences and Liberal Arts, Rajamangala University of Technology Isan, Nakhon Ratchasima 30000 (Thailand); Masingboon, C. [School of Physics, Suranaree University of Technology, Nakhon Ratchasima 30000 (Thailand); Faculty of Science and Engineering, Kasetsart University, Chalermphrakiat Sakon Nakhon Province Campus, Sakon Nakhon 47000 (Thailand); Rattanasuporn, S.; Phatthanakun, R.; Nakajima, H. [Synchrotron Light Research Institute, Nakhon Ratchasima 30000 (Thailand); King, P.D.C. [SUPA, School of Physics and Astronomy, University of St. Andrews, St. Andrews, Fife KY16 9SS (United Kingdom); Hodak, S.K. [Department of Physics, Faculty of Science, Chulalongkorn University, Bangkok 10330 (Thailand); Meevasana, W., E-mail: worawat@g.sut.ac.th [School of Physics, Suranaree University of Technology, Nakhon Ratchasima 30000 (Thailand); NANOTEC-SUT Center of Excellence on Advanced Functional Nanomaterials, Suranaree University of Technology, Nakhon Ratchasima 30000 (Thailand); Thailand Center of Excellence in Physics, CHE, Bangkok 10400 (Thailand)

2015-11-15

Highlights: • The dynamics of UV-induced oxygen vacancy is studied from the change of surface resistance. • The formation of 2DEG at the insulating surface of SrTiO{sub 3} is confirmed by ARPES. • The UV-induced change in resistance responds differently to oxygen/gas exposure. • The behavior of resistance recovery suggests an alternative method of low-pressure sensing. - Abstract: The effect of ultra-violet (UV) irradiation on the electronic structure and the surface resistance of an insulating SrTiO{sub 3}(0 0 1) crystal is studied in this work. Upon UV irradiation, we show that the two-dimensional electron gas (2DEG) emerges at the insulating SrTiO{sub 3} surface and there is a pronounced change in the surface resistance. By combining the observations of the change in valance band and the resistance change under different environments of gas pressure and gas species, we find that UV-induced oxygen vacancies at the surface plays a major role in the resistance change. The dynamic of the resistance change at different oxygen pressures also suggests an alternative method of low-pressure sensing.

Pinning by oxygen vacancies in high-Tc superconductors

International Nuclear Information System (INIS)

Chudnovsky, E.M.

1990-01-01

It is shown that recent data of Murray et al. on spatial correlations in flux lattices of Bi-Sr-Ca-Cu-O (BSCCO) may be explained if one assumes that 1% of oxygen atoms in CuO 2 layers are missing. This estimate, being in remarkable agreement with that deduced by Kes and van der Beek from ac-susceptibility measurements, provides strong confidence that oxygen vacancies are the major source of pinning in BSCCO

Ab initio R1 mechanism of photostimulated oxygen isotope exchange reaction on a defect TiO{sub 2} surface: The case of terminal oxygen atom exchange

Energy Technology Data Exchange (ETDEWEB)

Kevorkyants, Ruslan, E-mail: ruslan.kevorkyants@gmail.com; Sboev, Mikhail N.; Chizhov, Yuri V.

2017-05-01

Highlights: • DFT R1 mechanism of photostimulated oxygen isotope exchange between {sup 16}O{sup 18}O and terminal oxygen atom of a defect surface of nanocrystalline TiO{sub 2} is proposed. • The mechanism involves four adsorption intermediates and five transition states. • Activation energy of the reaction is 0.24 eV. • G-tensors of O{sub 3}{sup −} intermediates match EPR data on O{sub 2} adsorbed on UV-irradiated TiO{sub 2} surface. - Abstract: Based on density functional theory we propose R1 mechanism of photostimulated oxygen isotope exchange (POIEx) reaction between {sup 16}O{sup 18}O and terminal oxygen atom of a defect TiO{sub 2} surface, which is modeled by amorphous Ti{sub 8}O{sub 16} nanocluster in excited S{sup 1} electronic state. The proposed mechanism involves four adsorption intermediates and five transition states. The computed activation energy of the POIEx equals 0.24 eV. The computed g-tensors of the predicted ozonide O{sub 3}{sup −} chemisorption species match well EPR data on O{sub 2} adsorption on UV-irradiated nanocrystalline TiO{sub 2}. This match serves a mean of justification of the proposed R1 mechanism of the POIEx reaction. In addition, it is found that the proposed R1 POIEx reaction’s mechanism differs from R1 mechanism of thermo-assisted OIEx reaction on a surface of supported vanadium oxide catalyst VO{sub x}/TiO{sub 2} reported earlier.

The change of steel surface chemistry regarding oxygen partial pressure and dew point

Science.gov (United States)

Norden, Martin; Blumenau, Marc; Wuttke, Thiemo; Peters, Klaus-Josef

2013-04-01

By investigating the surface state of a Ti-IF, TiNb-IF and a MnCr-DP after several series of intercritical annealing, the impact of the annealing gas composition on the selective oxidation process is discussed. On behalf of the presented results, it can be concluded that not the general oxygen partial pressure in the annealing furnace, which is a result of the equilibrium reaction of water and hydrogen, is the main driving force for the selective oxidation process. It is shown that the amounts of adsorbed gases at the strip surface and the effective oxygen partial pressure resulting from the adsorbed gases, which is mainly dependent on the water content of the annealing furnace, is driving the selective oxidation processes occurring during intercritical annealing. Thus it is concluded, that for industrial applications the dew point must be the key parameter value for process control.

Rapid characterization of a nanomaterial structure using X-ray reciprocal-lattice-space imaging

International Nuclear Information System (INIS)

Sakata, Osami; Yoshimoto, Mamoru; Miki, Kazushi

2006-01-01

The X-ray reciprocal-lattice-space imaging method is able to record the reciprocal-lattice-space of nanostructure by sample-and-detector fixed geometry. This method was developed by the surface structure analysis beam line BL13XU of SPring-8. Outline of the X-ray diffraction method and basic principles of the X-ray reciprocal-lattice-space imaging method, and application examples are stated. The method is able to find out the Bragg conditions of nanostructure of surface in the atmosphere. The reciprocal-lattice of the embedded trace atomic wires was observed. The trace atoms of Bi atomic wires embedded in silicone showed the diffraction signal and image by a short exposure time. This method is useful at rapid non-destructive measurement of nanostructure. (S.Y.)

The Design of 3D-Printed Lattice-Reinforced Thickness-Varying Shell Molds for Castings.

Science.gov (United States)

Shangguan, Haolong; Kang, Jinwu; Yi, Jihao; Zhang, Xiaochuan; Wang, Xiang; Wang, Haibin; Huang, Tao

2018-03-30

3D printing technologies have been used gradually for the fabrication of sand molds and cores for castings, even though these molds and cores are dense structures. In this paper, a generation method for lattice-reinforced thickness-varying shell molds is proposed and presented. The first step is the discretization of the STL (Stereo Lithography) model of a casting into finite difference meshes. After this, a shell is formed by surrounding the casting with varying thickness, which is roughly proportional to the surface temperature distribution of the casting that is acquired by virtually cooling it in the environment. A regular lattice is subsequently constructed to support the shell. The outside surface of the shell and lattice in the cubic mesh format is then converted to STL format to serve as the external surface of the new shell mold. The internal surface of the new mold is the casting's surface with the normals of all of the triangles in STL format reversed. Experimental verification was performed on an Al alloy wheel hub casting. Its lattice-reinforced thickness-varying shell mold was generated by the proposed method and fabricated by the binder jetting 3D printing. The poured wheel hub casting was sound and of good surface smoothness. The cooling rate of the wheel hub casting was greatly increased due to the shell mold structure. This lattice-reinforced thickness-varying shell mold generation method is of great significance for mold design for castings to achieve cooling control.

La modified TiO{sub 2} photoanode and its effect on DSSC performance: A comparative study of doping and surface treatment on deep and surface charge trapping

Energy Technology Data Exchange (ETDEWEB)

Ako, Rajour Tanyi [Faculty of Science, Universiti Brunei Darussalam, Jalan Tungku Link, BE1410, Negara Brunei Darussalam (Brunei Darussalam); Ekanayake, Piyasiri, E-mail: piyasiri.ekanayake@ubd.edu.bn [Faculty of Science, Universiti Brunei Darussalam, Jalan Tungku Link, BE1410, Negara Brunei Darussalam (Brunei Darussalam); Centre for Advanced Material and Energy Sciences (CAMES), Universiti Brunei Darussalam, Jalan Tungku Link, BE1410, Negara Brunei Darussalam (Brunei Darussalam); Tan, Ai Ling [Faculty of Science, Universiti Brunei Darussalam, Jalan Tungku Link, BE1410, Negara Brunei Darussalam (Brunei Darussalam); Young, David James [Faculty of Science, Universiti Brunei Darussalam, Jalan Tungku Link, BE1410, Negara Brunei Darussalam (Brunei Darussalam); Faculty of Science, Health, Education and Engineering, University of the Sunshine Coast, Maroochydore DC, Queensland, 4558 (Australia); Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research - A*STAR, #08-03, 2 Fusionopolis Way, Innovis, 138634 (Singapore)

2016-04-01

The effect of Lanthanum ions (La{sup 3+}) on charge trapping in dye-sensitized solar cell (DSSC) photoanodes has been investigated with doped and surface-treated TiO{sub 2} nanoparticles. Doped nanoparticles consisting of 0.5 mol.% Mg and La co-doped TiO{sub 2}, 0.5 mol.% Mg doped TiO{sub 2} and pure TiO{sub 2} were synthesized by the sol gel method. Surface-treated nanoparticles of Mg doped TiO{sub 2} and pure TiO{sub 2} were prepared by ball milling in 0.05 M aqueous La{sup 3+} solution. All materials were analyzed by XRD, XPS and UV–Vis DRS. Cell performance, surface free energy state changes and electron injection efficiency of DSSCs based on these nanoparticles were evaluated using current –voltage measurements, EIS and Incident photon to current conversion efficiency. Doped materials had La and Mg ions incorporated into the TiO{sub 2} lattice, while no lattice changes were observed for the surface-treated materials. Less visible light was absorbed by treated oxides compared with doped oxide samples. The overall power conversion efficiencies (PCE) of DSSC photoanodes based on doped materials were twice those of photoanodes fabricated from treated nanoparticles. Doping establishes deep traps that reduce the recombination of electron–hole (e–h) pairs. Conversely, the presence of absorbed oxygen in treated materials enhances e–h recombination with electrolyte at surface trap sites. - Highlights: • DSSC performance is investigated using photoanodes of doped and La{sup 3+} surface treated TiO{sub 2}. • TiO{sub 2} and Mg–TiO{sub 2} treated with La{sup 3+} absorbed less visible light. • A high concentration of absorbed oxygen on surface treated oxides reduced band bending. • Increased surface free energy in the modified DSSC anodes is caused more by Mg{sup 2+} at Ti{sup 4+} than by La{sup 3+} at the surfaces. • Near surface charge traps due to La{sup 3+} treatment promotes e–h recombination.

Topological Nematic States and Non-Abelian Lattice Dislocations

Directory of Open Access Journals (Sweden)

Maissam Barkeshli

2012-08-01

Full Text Available An exciting new prospect in condensed matter physics is the possibility of realizing fractional quantum Hall states in simple lattice models without a large external magnetic field. A fundamental question is whether qualitatively new states can be realized on the lattice as compared with ordinary fractional quantum Hall states. Here we propose new symmetry-enriched topological states, topological nematic states, which are a dramatic consequence of the interplay between the lattice translational symmetry and topological properties of these fractional Chern insulators. The topological nematic states are realized in a partially filled flat band with a Chern number N, which can be mapped to an N-layer quantum Hall system on a regular lattice. However, in the topological nematic states the lattice dislocations can act as wormholes connecting the different layers and effectively change the topology of the space. Consequently, lattice dislocations become defects with a nontrivial quantum dimension, even when the fractional quantum Hall state being realized is, by itself, Abelian. Our proposal leads to the possibility of realizing the physics of topologically ordered states on high-genus surfaces in the lab even though the sample has only the disk geometry.

Topological Nematic States and Non-Abelian Lattice Dislocations

Science.gov (United States)

Barkeshli, Maissam; Qi, Xiao-Liang

2012-07-01

An exciting new prospect in condensed matter physics is the possibility of realizing fractional quantum Hall states in simple lattice models without a large external magnetic field. A fundamental question is whether qualitatively new states can be realized on the lattice as compared with ordinary fractional quantum Hall states. Here we propose new symmetry-enriched topological states, topological nematic states, which are a dramatic consequence of the interplay between the lattice translational symmetry and topological properties of these fractional Chern insulators. The topological nematic states are realized in a partially filled flat band with a Chern number N, which can be mapped to an N-layer quantum Hall system on a regular lattice. However, in the topological nematic states the lattice dislocations can act as wormholes connecting the different layers and effectively change the topology of the space. Consequently, lattice dislocations become defects with a nontrivial quantum dimension, even when the fractional quantum Hall state being realized is, by itself, Abelian. Our proposal leads to the possibility of realizing the physics of topologically ordered states on high-genus surfaces in the lab even though the sample has only the disk geometry.

Lattice-induced nonadiabatic frequency shifts in optical lattice clocks

International Nuclear Information System (INIS)

Beloy, K.

2010-01-01

We consider the frequency shift in optical lattice clocks which arises from the coupling of the electronic motion to the atomic motion within the lattice. For the simplest of three-dimensional lattice geometries this coupling is shown to affect only clocks based on blue-detuned lattices. We have estimated the size of this shift for the prospective strontium lattice clock operating at the 390-nm blue-detuned magic wavelength. The resulting fractional frequency shift is found to be on the order of 10 -18 and is largely overshadowed by the electric quadrupole shift. For lattice clocks based on more complex geometries or other atomic systems, this shift could potentially be a limiting factor in clock accuracy.

Combustion of methane-oxygen and methane-oxygen-CFC mixtures initiated by a high-current slipping surface discharge

International Nuclear Information System (INIS)

Kossyi, I.A.; Silakov, V.P.; Tarasova, N.M.

2001-01-01

Results are presented from experimental studies of the destruction of chlorofluorocarbon (CF 2 Cl 2 ) molecules in a methane-oxygen (air) gas mixture whose combustion is initiated by a high-current slipping surface discharge. It is found that a three-component CH 4 + O 2 (air)+ CF 2 Cl 2 gas mixture (even with a considerable amount of the third component) demonstrates properties of explosive combustion involving chain reactions that are typical of two-component CH 4 + O 2 mixtures. Experiments show the high degree of destruction (almost complete decomposition) of chlorofluorocarbons contained in the mixture during one combustion event. The combustion dynamics is studied. It is shown that the combustion initiated by a slipping surface discharge has a number of characteristic features that make it impossible to identify the combustion dynamics with the formation of a combustion or detonation wave. The features of the effects observed can be related to intense UV radiation produced by a pulsed high-current surface discharge

Radiation accelerated formation of oxygen and carbon related complexes in silicon

International Nuclear Information System (INIS)

Lazrak, A.; Magnea, N.; Pautrat, J.L.

1984-06-01

During the pulling of silicon monocrystals by the Czochralsky method, oxygen is incorporated into the lattice. It is known from early works that low temperature annealings (400-1000 0 C) make this oxygen to precipitate and a number of different defects to be generated. In order to check whether the fast diffusivity of an oxygen silicon interstitial complex has to be taken in consideration it was interesting to examinate the possible role of radiation damage on the formation of oxygen related defects. Experimental results of an experiment are presented and discussed

Micromechanism of oxygen transport during initial stage oxidation in Si(100) surface: A ReaxFF molecular dynamics simulation study

International Nuclear Information System (INIS)

Sun, Yu; Liu, Yilun; Chen, Xuefeng; Zhai, Zhi; Xu, Fei; Liu, Yijun

2017-01-01

Highlights: • A competition mechanism between thermal actuation and compressive stress blocking was found for the oxygen transport. • At low temperature, a compressive stress was generated in the oxide layer which blocked oxygen transport into the deeper region. • O atoms gained larger possibility to go deeper inward as temperature increase. • The related film quality was well explained by the competition mechanism. - Abstract: The early stage oxidation in Si(100) surface has been investigated in this work by a reactive force field molecular dynamics (ReaxFF MD) simulation, manifesting that the oxygen transport acted as a dominant issue for initial oxidation process. Due to the oxidation, a compressive stress was generated in the oxide layer which blocked the oxygen transport perpendicular to the Si(100) surface and further prevented oxidation in the deeper layer. In contrast, thermal actuation was beneficial to the oxygen transport into deeper layer as temperature increases. Therefore, a competition mechanism was found for the oxygen transport during early stage oxidation in Si(100) surface. At room temperature, the oxygen transport was governed by the blocking effect of compressive stress, so a better quality oxide film with more uniform interface and more stoichiometric oxide structure was obtained. Indeed, the mechanism presented in this work is also applicable for other self-limiting oxidation (e.g. metal oxidation) and is helpful for the design of high-performance electronic devices.

Micromechanism of oxygen transport during initial stage oxidation in Si(100) surface: A ReaxFF molecular dynamics simulation study

Energy Technology Data Exchange (ETDEWEB)

Sun, Yu, E-mail: yu.sun@xjtu.edu.cn [State Key Laboratory for Manufacturing Systems Engineering, School of Mechanical Engineering, Xi’an Jiaotong University, Xi’an 710049 (China); Institute for Computational Mechanics and Its Applications, Northwestern Polytechnical University, Xi’an 710072 (China); Liu, Yilun [State Key Laboratory for Strength and Vibration of Mechanical Structures, School of Aerospace Engineering, Xi’an Jiaotong University, Xi’an 710049 (China); Chen, Xuefeng; Zhai, Zhi [State Key Laboratory for Manufacturing Systems Engineering, School of Mechanical Engineering, Xi’an Jiaotong University, Xi’an 710049 (China); Xu, Fei [Institute for Computational Mechanics and Its Applications, Northwestern Polytechnical University, Xi’an 710072 (China); Liu, Yijun [Institute for Computational Mechanics and Its Applications, Northwestern Polytechnical University, Xi’an 710072 (China); Mechanical Engineering, University of Cincinnati, Cincinnati, OH 45221-0072 (United States)

2017-06-01

Highlights: • A competition mechanism between thermal actuation and compressive stress blocking was found for the oxygen transport. • At low temperature, a compressive stress was generated in the oxide layer which blocked oxygen transport into the deeper region. • O atoms gained larger possibility to go deeper inward as temperature increase. • The related film quality was well explained by the competition mechanism. - Abstract: The early stage oxidation in Si(100) surface has been investigated in this work by a reactive force field molecular dynamics (ReaxFF MD) simulation, manifesting that the oxygen transport acted as a dominant issue for initial oxidation process. Due to the oxidation, a compressive stress was generated in the oxide layer which blocked the oxygen transport perpendicular to the Si(100) surface and further prevented oxidation in the deeper layer. In contrast, thermal actuation was beneficial to the oxygen transport into deeper layer as temperature increases. Therefore, a competition mechanism was found for the oxygen transport during early stage oxidation in Si(100) surface. At room temperature, the oxygen transport was governed by the blocking effect of compressive stress, so a better quality oxide film with more uniform interface and more stoichiometric oxide structure was obtained. Indeed, the mechanism presented in this work is also applicable for other self-limiting oxidation (e.g. metal oxidation) and is helpful for the design of high-performance electronic devices.

Modelling and investigation of partial wetting surfaces for drop dynamics using lattice Boltzmann method

Energy Technology Data Exchange (ETDEWEB)

Pravinraj, T., E-mail: pravinraj1711@gmail.com; Patrikar, Rajendra

2017-07-01

Highlights: • A LBM model on partial wetting surface for droplet dynamics is presented by introducing a simple initial partial wetting boundary condition in SC model. • With our approach one can tune the splitting volume and time by carefully choosing strip width and position. • It is shown that the droplet spreading on chemically heterogeneous surfaces can be controlled not only by Weber number but also by tuning strip width ratio. • The directional transportation of a droplet due to chemical wetting gradient is simulated and analyzed using hybrid thermodynamic-image processing technique. • Microstructure surface and its influence on the directional wetting based transportation of droplet are demonstrated. - Abstract: Partial wetting surfaces and its influence on the droplet movement of micro and nano scale being contemplated for many useful applications. The dynamics of the droplet usually analyzed with a multiphase lattice Boltzmann method (LBM). In this paper, the influence of partial wetting surface on the dynamics of droplet is systematically analyzed for various cases. Splitting of droplets due to chemical gradient of the surface is studied and analyses of splitting time for various widths of the strips for different Weber numbers are computed. With the proposed model one can tune the splitting volume and time by carefully choosing a strip width and droplet position. The droplet spreading on chemically heterogeneous surfaces shows that the spreading can be controlled not only by parameters of Weber number but also by tuning strip width ratio. The transportation of the droplet from hydrophobic surface to hydrophilic surface due to chemical gradient is simulated and analyzed using our hybrid thermodynamic-image processing technique. The results prove that with the progress of time the surface free energy decreases with increase in spreading area. Finally, the transportation of a droplet on microstructure gradient is demonstrated. The model explains

Investigation of ferromagnetism in oxygen deficient hafnium oxide thin films

Energy Technology Data Exchange (ETDEWEB)

Hildebrandt, Erwin; Kurian, Jose; Krockenberger, Yoshiharu; Alff, Lambert [Institut fuer Materialwissenschaft, TU Darmstadt (Germany); Suter, Andreas [PSI, Villingen (Switzerland); Wilhelm, Fabrice; Rogalev, Andrei [ESRF, Grenoble (France)

2008-07-01

Oxygen deficient thin films of hafnium oxide were grown on single crystal r-cut and c-cut sapphire by reactive molecular beam epitaxy. RF-activated oxygen was used for the in situ oxidation of hafnium oxide thin films. Oxidation conditions were varied substantially in order to create oxygen deficiency in hafnium oxide films intentionally. The films were characterized by X-ray and magnetic measurements. X-ray diffraction studies show an increase in lattice parameter with increasing oxygen deficiency. Oxygen deficient hafnium oxide thin films also showed a decreasing bandgap with increase in oxygen deficiency. The magnetisation studies carried out with SQUID did not show any sign of ferromagnetism in the whole oxygen deficiency range. X-ray magnetic circular dichroism measurements also confirmed the absence of ferromagnetism in oxygen deficient hafnium oxide thin films.

Surface monofunctionalized polymethyl pentene hollow fiber membranes by plasma treatment and hemocompatibility modification for membrane oxygenators

Science.gov (United States)

Huang, Xin; Wang, Weiping; Zheng, Zhi; Fan, Wenling; Mao, Chun; Shi, Jialiang; Li, Lei

2016-01-01

The hemocompatibility of polymethyl pentene (PMP) hollow fiber membranes (HFMs) was improved through surface modification for membrane oxygenator applications. The modification was performed stepwise with the following: (1) oxygen plasma treatment, (2) functionalization of monosort hydroxyl groups through NaBH4 reduction, and (3) grafting 2-methacryloyloxyethyl phosphorylcholine (MPC) or heparin. SEM, ATR-FTIR, and XPS analyses were conducted to confirm successful grafting during the modification. The hemocompatibility of PMP HFMs was analyzed and compared through protein adsorption, platelet adhesion, and coagulation tests. Pure CO2 and O2 permeation rates, as well as in vitro gas exchange rates, were determined to evaluate the mass transfer properties of PMP HFMs. SEM results showed that different nanofibril topographies were introduced on the HFM surface. ATR-FTIR and XPS spectra indicated the presence of functionalization of monosort hydroxyl group and the grafting of MPC and heparin. Hemocompatibility evaluation results showed that the modified PMP HFMs presented optimal hemocompatibility compared with pristine HFMs. Gas permeation results revealed that gas permeation flux increased in the modified HFMs because of dense surface etching during the plasma treatment. The results of in vitro gas exchange rates showed that all modified PMP HFMs presented decreased gas exchange rates because of potential surface fluid wetting. The proposed strategy exhibits a potential for fabricating membrane oxygenators for biomedical applications to prevent coagulation formation and alter plasma-induced surface topology and composition.

Surface chemistry and microstructural analysis of CexZr1-xO2-y model catalyst surfaces

International Nuclear Information System (INIS)

Nelson, Alan E.; Schulz, Kirk H.

2003-01-01

Cerium-zirconium mixed metal oxides are widely used as promoters in automotive emissions control catalyst systems (three-way catalysts). The addition of zirconium in the cubic lattice of ceria improves the redox properties and the thermal stability, thereby increasing the catalyst efficiency and longevity. The surface composition and availability of surface oxygen of model ceria-zirconia catalyst promoters was considered to develop a reference for future catalytic reactivity studies. The microstructure was characterized with X-ray diffraction (XRD) to determine the effect of zirconium substitution on crystalline structure and grain size. Additionally, the Ce/Zr surface atomic ratio and existence of Ce 3+ defect sites were examined with X-ray photoelectron spectroscopy (XPS) and Auger electron spectroscopy (AES) for samples with different zirconium concentrations. The surface composition of the model systems with respect to cerium and zirconium concentration is representative of the bulk, indicating no appreciable surface species segregation during model catalyst preparation or exposure to ultrahigh vacuum conditions and analysis techniques. Additionally, the concentration of Ce 3+ defect sites was constant and independent of composition. The quantity of surface oxygen was unaffected by electron bombardment or prolonged exposure to ultrahigh vacuum conditions. Additionally, XRD analysis did not indicate the presence of additional crystalline phases beyond the cubic structure for compositions from 100 to 25 at.% cerium, although additional phases may be present in undetectable quantities. This analysis is an important initial step for determining surface reactions and pathways for the development of efficient and sulfur-tolerant automotive emissions control catalysts

Oxygen diffusion in high-Tc superconductors

International Nuclear Information System (INIS)

Rothman, S.J.; Routbort, J.L.

1992-07-01

The cuprate superconductors are fascinating not only because of their technical promise, but also because of their structures, especially the anisotropy of the crystal lattice. There are some structural similarities among these compounds, but also significant differences. Measurements of the oxygen tracer diffusion coefficients have been carried out as a function of temperature, oxygen partial pressure, crystal orientation, and doping in the La-Sr-Cu-0, Y-Ba-Cu-0, and Bi-Sr-Ca-Cu-0 systems. These measurements have revealed a variety of defect mechanisms operating in these compounds; the exact nature of the mechanism depends on the details of the structure

Density functional study of NO adsorption on undefected and oxygen defective Au–BaO(1 0 0) surfaces

Energy Technology Data Exchange (ETDEWEB)

Añez, Rafael, E-mail: ranez@ivic.gob.ve [Laboratorio de Química Física y Catálisis Computacional, Centro de Química, Instituto Venezolano de Investigaciones Científicas, Apartado, 21827 Caracas (Venezuela, Bolivarian Republic of); Sierraalta, Aníbal; Bastardo, Anelisse [Laboratorio de Química Física y Catálisis Computacional, Centro de Química, Instituto Venezolano de Investigaciones Científicas, Apartado, 21827 Caracas (Venezuela, Bolivarian Republic of); Coll, David [Laboratorio de Físico Química Teórica de Materiales, Centro de Química, Instituto Venezolano de Investigaciones Científicas, Apartado, 21827 Caracas (Venezuela, Bolivarian Republic of); Garcia, Belkis [Instituto Universitario de Tecnología de Valencia IUTVAL, Valencia, Edo. Carabobo (Venezuela, Bolivarian Republic of)

2014-07-01

A periodic density functional approach has been used in order to explore the interaction of NO with undoped and Au doped BaO(1 0 0) surface. Due to oxygen vacancies increase the interaction between the doping metal and the surface, F{sub S} and F{sub S}{sup +} vacancies were studied and compared with the results obtained on the undefected doped BaO(1 0 0). Our results indicate that the high basicity of the BaO surface, besides the electron density changes produced by the oxygen vacancies, modify considerably how the Au atom interacts with the surface increasing the ionic character of the interaction. F{sub S} vacancy shows to be a promise center to activate de NO bond on the BaO(1 0 0) surface.

Chiral d -wave superconductivity in a triangular surface lattice mediated by long-range interaction

Science.gov (United States)

Cao, Xiaodong; Ayral, Thomas; Zhong, Zhicheng; Parcollet, Olivier; Manske, Dirk; Hansmann, Philipp

2018-04-01

Adatom systems on the Si(111) surface have recently attracted an increasing attention as strongly correlated systems with a rich phase diagram. We study these materials by a single band model on the triangular lattice, including 1 /r long-range interaction. Employing the recently proposed TRILEX method, we find an unconventional superconducting phase of chiral d -wave symmetry in hole-doped systems. Contrary to usual scenarios where charge and spin fluctuations are seen to compete, here the superconductivity is driven simultaneously by both charge and spin fluctuations and crucially relies on the presence of the long-range tail of the interaction. We provide an analysis of the relevant collective bosonic modes and predict how a cumulative charge and spin paring mechanism leads to superconductivity in doped silicon adatom materials.

Surface-Selective Preferential Production of Reactive Oxygen Species on Piezoelectric Ceramics for Bacterial Killing.

Science.gov (United States)

Tan, Guoxin; Wang, Shuangying; Zhu, Ye; Zhou, Lei; Yu, Peng; Wang, Xiaolan; He, Tianrui; Chen, Junqi; Mao, Chuanbin; Ning, Chengyun

2016-09-21

Reactive oxygen species (ROS) can be used to kill bacterial cells, and thus the selective generation of ROS from material surfaces is an emerging direction in antibacterial material discovery. We found the polarization of piezoelectric ceramic causes the two sides of the disk to become positively and negatively charged, which translate into cathode and anode surfaces in an aqueous solution. Because of the microelectrolysis of water, ROS are preferentially formed on the cathode surface. Consequently, the bacteria are selectively killed on the cathode surface. However, the cell experiment suggested that the level of ROS is safe for normal mammalian cells.

Roles of Bulk and Surface Chemistry in the Oxygen Exchange Kinetics and Related Properties of Mixed Conducting Perovskite Oxide Electrodes

Directory of Open Access Journals (Sweden)

Nicola H. Perry

2016-10-01

Full Text Available Mixed conducting perovskite oxides and related structures serving as electrodes for electrochemical oxygen incorporation and evolution in solid oxide fuel and electrolysis cells, respectively, play a significant role in determining the cell efficiency and lifetime. Desired improvements in catalytic activity for rapid surface oxygen exchange, fast bulk transport (electronic and ionic, and thermo-chemo-mechanical stability of oxygen electrodes will require increased understanding of the impact of both bulk and surface chemistry on these properties. This review highlights selected work at the International Institute for Carbon-Neutral Energy Research (I2CNER, Kyushu University, set in the context of work in the broader community, aiming to characterize and understand relationships between bulk and surface composition and oxygen electrode performance. Insights into aspects of bulk point defect chemistry, electronic structure, crystal structure, and cation choice that impact carrier concentrations and mobilities, surface exchange kinetics, and chemical expansion coefficients are emerging. At the same time, an understanding of the relationship between bulk and surface chemistry is being developed that may assist design of electrodes with more robust surface chemistries, e.g., impurity tolerance or limited surface segregation. Ion scattering techniques (e.g., secondary ion mass spectrometry, SIMS, or low energy ion scattering spectroscopy, LEIS with high surface sensitivity and increasing lateral resolution are proving useful for measuring surface exchange kinetics, diffusivity, and corresponding outer monolayer chemistry of electrodes exposed to typical operating conditions. Beyond consideration of chemical composition, the use of strain and/or a high density of active interfaces also show promise for enhancing performance.

Biofilm formation in geometries with different surface curvature and oxygen availability

International Nuclear Information System (INIS)

Chang, Ya-Wen; Fragkopoulos, Alexandros A; Kim, Harold D; Fernández-Nieves, Alberto; Marquez, Samantha M; Angelini, Thomas E

2015-01-01

Bacteria in the natural environment exist as interface-associated colonies known as biofilms . Complex mechanisms are often involved in biofilm formation and development. Despite the understanding of the molecular mechanisms involved in biofilm formation, it remains unclear how physical effects in standing cultures influence biofilm development. The topology of the solid interface has been suggested as one of the physical cues influencing bacteria-surface interactions and biofilm development. Using the model organism Bacillus subtilis, we study the transformation of swimming bacteria in liquid culture into robust biofilms in a range of confinement geometries (planar, spherical and toroidal) and interfaces (air/water, silicone/water, and silicone elastomer/water). We find that B. subtilis form submerged biofilms at both solid and liquid interfaces in addition to air-water pellicles. When confined, bacteria grow on curved surfaces of both positive and negative Gaussian curvature. However, the confinement geometry does affect the resulting biofilm roughness and relative coverage. We also find that the biofilm location is governed by oxygen availability as well as by gravitational effects; these compete with each other in some situations. Overall, our results demonstrate that confinement geometry is an effective way to control oxygen availability and subsequently biofilm growth. (paper)

Lattice strings

International Nuclear Information System (INIS)

Thorn, C.B.

1988-01-01

The possibility of studying non-perturbative effects in string theory using a world sheet lattice is discussed. The light-cone lattice string model of Giles and Thorn is studied numerically to assess the accuracy of ''coarse lattice'' approximations. For free strings a 5 by 15 lattice seems sufficient to obtain better than 10% accuracy for the bosonic string tachyon mass squared. In addition a crude lattice model simulating string like interactions is studied to find out how easily a coarse lattice calculation can pick out effects such as bound states which would qualitatively alter the spectrum of the free theory. The role of the critical dimension in obtaining a finite continuum limit is discussed. Instead of the ''gaussian'' lattice model one could use one of the vertex models, whose continuum limit is the same as a gaussian model on a torus of any radius. Indeed, any critical 2 dimensional statistical system will have a stringy continuum limit in the absence of string interactions. 8 refs., 1 fig. , 9 tabs

The Design of 3D-Printed Lattice-Reinforced Thickness-Varying Shell Molds for Castings

Science.gov (United States)

Shangguan, Haolong; Kang, Jinwu; Yi, Jihao; Zhang, Xiaochuan; Wang, Xiang; Wang, Haibin; Huang, Tao

2018-01-01

3D printing technologies have been used gradually for the fabrication of sand molds and cores for castings, even though these molds and cores are dense structures. In this paper, a generation method for lattice-reinforced thickness-varying shell molds is proposed and presented. The first step is the discretization of the STL (Stereo Lithography) model of a casting into finite difference meshes. After this, a shell is formed by surrounding the casting with varying thickness, which is roughly proportional to the surface temperature distribution of the casting that is acquired by virtually cooling it in the environment. A regular lattice is subsequently constructed to support the shell. The outside surface of the shell and lattice in the cubic mesh format is then converted to STL format to serve as the external surface of the new shell mold. The internal surface of the new mold is the casting’s surface with the normals of all of the triangles in STL format reversed. Experimental verification was performed on an Al alloy wheel hub casting. Its lattice-reinforced thickness-varying shell mold was generated by the proposed method and fabricated by the binder jetting 3D printing. The poured wheel hub casting was sound and of good surface smoothness. The cooling rate of the wheel hub casting was greatly increased due to the shell mold structure. This lattice-reinforced thickness-varying shell mold generation method is of great significance for mold design for castings to achieve cooling control. PMID:29601543

The Design of 3D-Printed Lattice-Reinforced Thickness-Varying Shell Molds for Castings

Directory of Open Access Journals (Sweden)

Haolong Shangguan

2018-03-01

Full Text Available 3D printing technologies have been used gradually for the fabrication of sand molds and cores for castings, even though these molds and cores are dense structures. In this paper, a generation method for lattice-reinforced thickness-varying shell molds is proposed and presented. The first step is the discretization of the STL (Stereo Lithography model of a casting into finite difference meshes. After this, a shell is formed by surrounding the casting with varying thickness, which is roughly proportional to the surface temperature distribution of the casting that is acquired by virtually cooling it in the environment. A regular lattice is subsequently constructed to support the shell. The outside surface of the shell and lattice in the cubic mesh format is then converted to STL format to serve as the external surface of the new shell mold. The internal surface of the new mold is the casting’s surface with the normals of all of the triangles in STL format reversed. Experimental verification was performed on an Al alloy wheel hub casting. Its lattice-reinforced thickness-varying shell mold was generated by the proposed method and fabricated by the binder jetting 3D printing. The poured wheel hub casting was sound and of good surface smoothness. The cooling rate of the wheel hub casting was greatly increased due to the shell mold structure. This lattice-reinforced thickness-varying shell mold generation method is of great significance for mold design for castings to achieve cooling control.

Final Report for Award DE-SC0005403. Improved Electrochemical Performance of Strained Lattice Electrolytes via Modulated Doping

Energy Technology Data Exchange (ETDEWEB)

Hertz, Joshua L. [Univ. of Delaware, Newark, DE (United States); Prasad, Ajay K. [Univ. of Delaware, Newark, DE (United States)

2015-09-06

The enclosed document provides a final report to document the research performed at the University of Delaware under Grant DE-SC0005403: Improved Electrochemical Performance of Strained Lattice Electrolytes via Modulated Doping. The ultimate goal of this project was to learn how to systematically strain the inter-atomic distance in thin ceramic films and how to use this newfound control to improve the ease by which oxygen ions can conduct through the films. Increasing the ionic conductivity of ceramics holds the promise of drastic improvements in the performance of solid oxide fuel cells, chemical sensors, gas permeation membranes, and related devices. Before this work, the experimental evidence advocating for strain-based techniques was often controversial and poorly characterized. Enabling much of this work was a new method to quickly create a very wide range of ceramic nanostructures that was established during the first phase of the project. Following this initial phase, we created a variety of promising nanostructured epitaxial films and multilayers with systematic variations in lattice mismatch and dopant content. Over the course of the work, a positive effect of tensile atomic strain on the oxygen conductivity was conclusively found using a few different forms of samples and experimental techniques. The samples were built by sputtering, an industrially scalable technique, and thus the technological implementation of these results may be economically feasible. Still, two other results consistently achieved over multiple efforts in this work give pause. The first of these results was that very specific, pristine surfaces upon which to build the nanostructures were strictly required in order to achieve measurable results. The second of these results was that compressively strained films with concomitant reductions in oxygen conductivity are much easier to obtain relative to tensile-strained films with increased conductivity.

Systematic spatial and stoichiometric screening towards understanding the surface of ultrasmall oxygenated silicon nanocrystal

Science.gov (United States)

Niaz, Shanawer; Zdetsis, Aristides D.; Koukaras, Emmanuel N.; Gülseren, Oǧuz; Sadiq, Imran

2016-11-01

In most of the realistic ab initio and model calculations which have appeared on the emission of light from silicon nanocrystals, the role of surface oxygen has been usually ignored, underestimated or completely ruled out. We investigate theoretically, by density functional theory (DFT/B3LYP) possible modes of oxygen bonding in hydrogen terminated silicon quantum dots using as a representative case of the Si29 nanocrystal. We have considered Bridge-bonded oxygen (BBO), Doubly-bonded oxygen (DBO), hydroxyl (OH) and Mix of these oxidizing agents. Due to stoichiometry, all comparisons performed are unbiased with respect to composition whereas spatial distribution of oxygen species pointed out drastic change in electronic and cohesive characteristics of nanocrytals. From an overall perspective of this study, it is shown that bridge bonded oxygenated Si nanocrystals accompanied by Mix have higher binding energies and large electronic gap compared to nanocrystals with doubly bonded oxygen atoms. In addition, it is observed that the presence of OH along with BBO, DBO and mixed configurations further lowers electronic gaps and binding energies but trends in same fashion. It is also demonstrated that within same composition, oxidizing constituent, along with their spatial distribution substantially alters binding energy, highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) gap (up to 1.48 eV) and localization of frontier orbitals.

Surface reactivity of mercury on the oxygen-terminated hematite(0001) surface: a first-principle study

Science.gov (United States)

Jung, J. E.; Wilcox, J.

2016-12-01

Hematite (α-Fe2O3) is a common mineral found in Earth's near-surface environment. Due to its nontoxicity, corrosion-resistance, and high thermal stability, α-Fe2O3 has attracted attentions as materials for various applications such as photocatalysts, gas sensors, as well as for the removal of heavy metals. In this study, α-Fe2O3 is chosen for potential mercury (Hg) sorbent in order to remove Hg from coal-fired power plants. Specifically, theoretical approaches using density functional theory (DFT) is used to understand surface reactivity of Hg on oxygen (O) terminated α-Fe2O3(0001) surface. The most probable adsorption sites of Hg, chlorine (Cl), and mercury chloride (HgCl) on the α-Fe2O3 surface are found based on adsorption energy calculations, and the oxidation states of the adsorbates are determined by Bader charge analysis. Additionally, projected density of states (PDOS) analysis characterizes the surface-adsorbate bonding mechanism. The results of adsorption energy calculation proposes that Hg physisorbs to the α-Fe2O3(0001) surface with adsorption energy of -0.278 eV, and the subsequent Bader charge analysis confirms that Hg is slightly oxidized. In addition, Cl introduced to the Hg-adsorbed surface strengthens Hg stability on the α-Fe2O3(0001) surface as evidenced by a shortened Hg-surface equilibrium distance. The PDOS analysis also suggests that Cl enhances the chemical bonding between the surface and the adsorbate, thereby increasing adsorption strength. In summary, α-Fe2O3 has ability to adsorb and oxidize Hg, and this reactivity is enhanced in the presence of Cl.

Hydrogen and oxygen behaviors on Porous-Si surfaces observed using a scanning ESD ion microscope

International Nuclear Information System (INIS)

Itoh, Yuki; Ueda, Kazuyuki

2004-01-01

A scanning electron-stimulated desorption (ESD) ion microscope (SESDIM) measured the 2-D images of hydrogen and oxygen distribution on solid surfaces. A primary electron beam at 600 eV, with a pulse width of 220 ns, resulted in ion yields of H + and O + . This SESDIM is applied to the surface analysis of Porous-Si (Po-Si) partially covered with SiN films. During the heating of a specimen of the Po-Si at 800 deg. C under ultra-high-vacuum (UHV) conditions, the components of the surface materials were moved or diffused by thermal decomposition accompanied by a redistribution of hydrogen and oxygen. After cyclic heating of above 800 deg. C, the dynamic behaviors of H + and O + accompanied by the movements of the SiN layers were observed as images of H + and O + . This was because the H + and O + ions have been identified as composite materials by their kinetic energies

Polaron-mediated surface reconstruction in the reduced Rutile TiO2 (110) surface

Science.gov (United States)

Reticcioli, Michele; Setvin, Martin; Hao, Xianfeng; Diebold, Ulrike; Franchini, Cesare

The role of polarons is of key importance for the understanding of the fundamental properties and functionalities of TiO2. We use density functional theory with an on-site Coulomb interaction and molecular dynamics to study the formation and dynamics of small polarons in the reduced rutile (110) surface. We show that excess electrons donated by oxygen-vacancies (VO) form mobile small polarons that hop easily in subsurface and surface Ti-sites. The polaron formation becomes more favorable by increasing the VO concentration level (up to 20%) due to the progressively lower energy cost needed to distort the lattice. However, at higher VO concentration the shortening of the averaged polaron-polaron distance leads to an increased Coulomb repulsion among the trapped charges at the Ti-sites, which weakens this trend. This instability is overtaken by means of a structural 1 × 2 surface reconstruction, characterized by a distinctively more favorable polaron distribution. The calculations are validated by a direct comparison with experimental AFM and STM data. Our study identifies a fundamentally novel mechanism to drive surface reconstructions and resolves a long standing issue on the origin of the reconstruction in rutile (110) surface.

Electron stimulated desorption of positive and negative oxygen ions from YBa{sub 2}Cu{sub 3}O{sub 7} surfaces

Energy Technology Data Exchange (ETDEWEB)

Hoffman, A. [Technion-Israel Inst. of Tech., Haifa (Israel). Solid State Inst.; Moss, S.D.; Paterson, P.J.K. [Royal Melbourne Inst. of Tech., VIC (Australia); McCubbery, D. [La Trobe Univ., Bundoora, VIC (Australia); Petravic, M. [Australian National Univ., Canberra, ACT (Australia)

1996-12-31

The electron stimulated desorption (ESD) of positive and negative oxygen ion from superconducting YBa{sub 2}Cu{sub 3}O{sub 7} surfaces was studied. Based on ion desorption yield measurements as function of electron kinetic energy, primary excitations leading to positive and negative oxygen ion desorption are suggested. To the best of the authors` knowledge this is the first study on electron energy dependent ESD from YBa{sub 2}Cu{sub 3}O{sub 7} surfaces. The YBa{sub 2}Cu{sub 3}O{sub 7} samples were prepared from BaCO{sub 3}, Y{sub 2}O{sub 3} and CuO using standard high temperature sintering and annealing procedures. Slices 2 mm thick were cut and further annealed at 400 C in flowing oxygen for 24 hours prior to insertion into the ultrahigh vacuum (UHV) chamber for ESD. The near surface composition and chemical state of the annealed sample after exposure to air was examined by Auger and XPS analysis. These measurements suggest that the ESD experiments were performed on samples of similar near surface and bulk composition with some OH- chemisorbed groups and Cl surface contaminations and that negative and positive oxygen ion desorption may be initiated via a primary core level ionization. 10 refs., 3 figs.

Electron stimulated desorption of positive and negative oxygen ions from YBa{sub 2}Cu{sub 3}O{sub 7} surfaces

Energy Technology Data Exchange (ETDEWEB)

Hoffman, A [Technion-Israel Inst. of Tech., Haifa (Israel). Solid State Inst.; Moss, S D; Paterson, P J.K. [Royal Melbourne Inst. of Tech., VIC (Australia); McCubbery, D [La Trobe Univ., Bundoora, VIC (Australia); Petravic, M [Australian National Univ., Canberra, ACT (Australia)

1997-12-31

The electron stimulated desorption (ESD) of positive and negative oxygen ion from superconducting YBa{sub 2}Cu{sub 3}O{sub 7} surfaces was studied. Based on ion desorption yield measurements as function of electron kinetic energy, primary excitations leading to positive and negative oxygen ion desorption are suggested. To the best of the authors` knowledge this is the first study on electron energy dependent ESD from YBa{sub 2}Cu{sub 3}O{sub 7} surfaces. The YBa{sub 2}Cu{sub 3}O{sub 7} samples were prepared from BaCO{sub 3}, Y{sub 2}O{sub 3} and CuO using standard high temperature sintering and annealing procedures. Slices 2 mm thick were cut and further annealed at 400 C in flowing oxygen for 24 hours prior to insertion into the ultrahigh vacuum (UHV) chamber for ESD. The near surface composition and chemical state of the annealed sample after exposure to air was examined by Auger and XPS analysis. These measurements suggest that the ESD experiments were performed on samples of similar near surface and bulk composition with some OH- chemisorbed groups and Cl surface contaminations and that negative and positive oxygen ion desorption may be initiated via a primary core level ionization. 10 refs., 3 figs.

Quasi-hexagonal vortex-pinning lattice using anodized aluminum oxide nanotemplates

DEFF Research Database (Denmark)

Hallet, X.; Mátéfi-Tempfli, M.; Michotte, S.

2009-01-01

The bottom barrier layer of well-ordered nanoporous alumina membranes reveals a previously unexploited nanostructured template surface consisting of a triangular lattice of hemispherical nanoscale bumps. Quasi-hexagonal vortex-pinning lattice arrays are created in superconducting Nb films deposited...... onto this template (see image). Matching effects are preserved at higher magnetic fields and lower temperatures when compared to holes on the top face....

Oxygen exchange at gas/oxide interfaces: how the apparent activation energy of the surface exchange coefficient depends on the kinetic regime.

Science.gov (United States)

Fielitz, Peter; Borchardt, Günter

2016-08-10

In the dedicated literature the oxygen surface exchange coefficient KO and the equilibrium oxygen exchange rate [Fraktur R] are considered to be directly proportional to each other regardless of the experimental circumstances. Recent experimental observations, however, contradict the consequences of this assumption. Most surprising is the finding that the apparent activation energy of KO depends dramatically on the kinetic regime in which it has been determined, i.e. surface exchange controlled vs. mixed or diffusion controlled. This work demonstrates how the diffusion boundary condition at the gas/solid interface inevitably entails a correlation between the oxygen surface exchange coefficient KO and the oxygen self-diffusion coefficient DO in the bulk ("on top" of the correlation between KO and [Fraktur R] for the pure surface exchange regime). The model can thus quantitatively explain the range of apparent activation energies measured in the different regimes: in the surface exchange regime the apparent activation energy only contains the contribution of the equilibrium exchange rate, whereas in the mixed or in the diffusion controlled regime the contribution of the oxygen self-diffusivity has also to be taken into account, which may yield significantly higher apparent activation energies and simultaneously quantifies the correlation KO ∝ DO(1/2) observed for a large number of oxides in the mixed or diffusion controlled regime, respectively.

DNA-linked NanoParticle Lattices with Diamond Symmetry: Stability, Shape and Optical Properties

Science.gov (United States)

Emamy, Hamed; Tkachenko, Alexei; Gang, Oleg; Starr, Francis

The linking of nanoparticles (NP) by DNA has been proven to be an effective means to create NP lattices with specific order. Lattices with diamond symmetry are predicted to offer novel photonic properties, but self-assembly of such lattices has proven to be challenging due to the low packing fraction, sensitivity to bond orientation, and local heterogeneity. Recently, we reported an approach to create diamond NP lattices based on the association between anisotropic particles with well-defined tetravalent DNA binding topology and isotropically functionalized NP. Here, we use molecular dynamics simulations to evaluate the Gibbs free energy of these lattices, and thereby determine the stability of these lattices as a function of NP size and DNA stiffness. We also predict the equilibrium shape for the cubic diamond crystallite using the Wulff construction method. Specifically, we predict the equilibrium shape using the surface energy for different crystallographic planes. We evaluate surface energy directly form molecular dynamics simulation, which we correlate with theoretical estimates from the expected number of broken DNA bonds along a facet. Furthermore we study the optical properties of this structure, e.g optical bandgap.

Back-exchange: a novel approach to quantifying oxygen diffusion and surface exchange in ambient atmospheres.

Science.gov (United States)

Cooper, Samuel J; Niania, Mathew; Hoffmann, Franca; Kilner, John A

2017-05-17

A novel two-step Isotopic Exchange (IE) technique has been developed to investigate the influence of oxygen containing components of ambient air (such as H 2 O and CO 2 ) on the effective surface exchange coefficient (k*) of a common mixed ionic electronic conductor material. The two step 'back-exchange' technique was used to introduce a tracer diffusion profile, which was subsequently measured using Time-of-Flight Secondary Ion Mass Spectrometry (ToF-SIMS). The isotopic fraction of oxygen in a dense sample as a function of distance from the surface, before and after the second exchange step, could then be used to determine the surface exchange coefficient in each atmosphere. A new analytical solution was found to the diffusion equation in a semi-infinite domain with a variable surface exchange boundary, for the special case where D* and k* are constant for all exchange steps. This solution validated the results of a numerical, Crank-Nicolson type finite-difference simulation, which was used to extract the parameters from the experimental data. When modelling electrodes, D* and k* are important input parameters, which significantly impact performance. In this study La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O 3-δ (LSCF6428) was investigated and it was found that the rate of exchange was increased by around 250% in ambient air compared to high purity oxygen at the same pO 2 . The three experiments performed in this study were used to validate the back-exchange approach and show its utility.

Near Surface CO2 Triple Oxygen Isotope Composition

Directory of Open Access Journals (Sweden)

Sasadhar Mahata

2016-02-01

Full Text Available The isotopic composition of carbon dioxide in the atmosphere is a powerful tool for constraining its sources and sinks. In particular, the 17O oxygen anomaly [Δ17O = 1000 × ln(1 + δ17O/1000 - 0.516 × 1000 × ln(1 + δ18O/1000], with a value > 0.5‰ produced in the middle atmosphere, provides an ideal tool for probing the exchange of carbon dioxide between the biosphere/hydrosphere and atmosphere. The biosphere/hydrosphere and anthropogenic emissions give values ≤ 0.3‰. Therefore, any anomaly in near surface CO2 would reflect the balance between stratospheric input and exchange with the aforementioned surface sources. We have analyzed Δ17O values of CO2 separated from air samples collected in Taipei, Taiwan, located in the western Pacific region. The obtained mean anomaly is 0.42 ± 0.14‰ (1-σ standard deviation, in good agreement with model prediction and a published decadal record. Apart from typically used δ13C and δ18O values, the Δ17O value could provide an additional tracer for constraining the carbon cycle.

On the nature of oxygen-containing surface groups on carbon nanofibers and their role for platinum deposition—an xps and titration study

NARCIS (Netherlands)

Plomp, A.J.; Su, D.S.; de Jong, K.P.; Bitter, J.H.

2009-01-01

XPS and acid−base titrations were used to investigate the nature and stability of oxygen-containing surface groups on carbon nanofibers (CNF) and platinum-containing CNF. During heat treatments in inert atmosphere at 973 K all acidic (carboxylic) oxygen surface groups were removed for CNF.

High-Resolution Electron Energy Loss Studies of Oxygen, Hydrogen, Nitrogen, Nitric Oxide, and Nitrous Oxide Adsorption on Germanium Surfaces.

Science.gov (United States)

Entringer, Anthony G.

The first high resolution electron energy loss spectroscopy (HREELS) studies of the oxidation and nitridation of germanium surfaces are reported. Both single crystal Ge(111) and disordered surfaces were studied. Surfaces were exposed to H, O_2, NO, N _2O, and N, after cleaning in ultra-high vacuum. The Ge surfaces were found to be non-reactive to molecular hydrogen (H_2) at room temperature. Exposure to atomic hydrogen (H) resulted hydrogen adsorption as demonstrated by the presence of Ge-H vibrational modes. The HREEL spectrum of the native oxide of Ge characteristic of nu -GeO_2 was obtained by heating the oxide to 200^circC. Three peaks were observed at 33, 62, and 106 meV for molecular oxygen (O_2) adsorbed on clean Ge(111) at room temperature. These peaks are indicative of dissociative bonding and a dominant Ge-O-Ge bridge structure. Subsequent hydrogen exposure resulted in a shift of the Ge-H stretch from its isolated value of 247 meV to 267 meV, indicative of a dominant +3 oxidation state. A high density of dangling bonds and defects and deeper oxygen penetration at the amorphous Ge surface result in a dilute bridge structure with a predominant +1 oxidation state for similar exposures. Molecules of N_2O decompose at the surfaces to desorbed N_2 molecules and chemisorbed oxygen atoms. In contrast, both oxygen and nitrogen are detected at the surfaces following exposure to NO molecules. Both NO and N_2O appear to dissociate and bond at the top surface layer. Molecular nitrogen (N_2) does not react with the Ge surfaces, however, a precursor Ge nitride is observed at room temperature following exposure to nitrogen atoms and ions. Removal of oxygen by heating of the NO-exposed surface to 550^circC enabled the identification of the Ge-N vibrational modes. These modes show a structure similar to that of germanium nitride. This spectrum is also identical to that of the N-exposed surface heated to 550^circC. Surface phonon modes of the narrow-gap semiconducting

Osteoblast response to oxygen functionalised plasma polymer surfaces

International Nuclear Information System (INIS)

Kelly, Jonathan M.

2001-01-01

Thin organic films with oxygen-carbon functionalities were deposited from plasmas containing vapour of the small organic compounds: allyI alcohol, methyl vinyl ketone and acrylic acid with octadiene. Characterisation of the deposits was carried out using X-ray photoelectron spectroscopy, in conjunction with chemical derivatisation, and this showed that plasma polymers retained high levels of original monomer functionality when the plasmas were sustained at low power for a given monomer vapour flow rate. High levels of attachment of rat osteosarcoma (ROS 17/2.8) cells were observed on surfaces that had high concentrations of hydroxyl and carbonyl functionalities and intermediate concentrations of carboxyl functionality. Cells did not attach to the octadiene plasma polymer. Cell attachment to carboxyl and methyl functionalised self-assembled monolayers increased with increasing concentration of surface carboxyl groups. Adsorption of the extracellular matrix protein fibronectin to acrylic acid/octadiene plasma copolymers was studied by enzyme linked immunosorbent assays and by I 125 radiolabelling. Fibronectin adsorbed in largest amounts to surfaces with intermediate concentrations of carboxyl functionality. Spreading of ROS cells and rat bone marrow stromal cells (BMSC) was characterised by computer image analysis. Cell spreading in media containing 10% serum, on a surface deposited from a plasma of 5 O/o acrylic acid was much greater than on the octadiene plasma polymer while most extensive cell spreading was observed on these surfaces when preadsorbed with fibronectin. Growth (proliferation) of BMSC was assessed over nine days and was found to be faster on an 50% acrylic acid plasma polymer than on tissue culture polystyrene or a hydrocarbon plasma polymer, though cell growth was fastest on fibronectin precoated substrates. Expression of cellular alkaline phosphatase, collagen and calcium reached similar levels on the 50% acrylic acid plasma polymer, tissue culture

Osteoblast response to oxygen functionalised plasma polymer surfaces

Energy Technology Data Exchange (ETDEWEB)

Kelly, Jonathan M

2001-07-01

Thin organic films with oxygen-carbon functionalities were deposited from plasmas containing vapour of the small organic compounds: allyI alcohol, methyl vinyl ketone and acrylic acid with octadiene. Characterisation of the deposits was carried out using X-ray photoelectron spectroscopy, in conjunction with chemical derivatisation, and this showed that plasma polymers retained high levels of original monomer functionality when the plasmas were sustained at low power for a given monomer vapour flow rate. High levels of attachment of rat osteosarcoma (ROS 17/2.8) cells were observed on surfaces that had high concentrations of hydroxyl and carbonyl functionalities and intermediate concentrations of carboxyl functionality. Cells did not attach to the octadiene plasma polymer. Cell attachment to carboxyl and methyl functionalised self-assembled monolayers increased with increasing concentration of surface carboxyl groups. Adsorption of the extracellular matrix protein fibronectin to acrylic acid/octadiene plasma copolymers was studied by enzyme linked immunosorbent assays and by I{sup 125} radiolabelling. Fibronectin adsorbed in largest amounts to surfaces with intermediate concentrations of carboxyl functionality. Spreading of ROS cells and rat bone marrow stromal cells (BMSC) was characterised by computer image analysis. Cell spreading in media containing 10% serum, on a surface deposited from a plasma of 5 O/o acrylic acid was much greater than on the octadiene plasma polymer while most extensive cell spreading was observed on these surfaces when preadsorbed with fibronectin. Growth (proliferation) of BMSC was assessed over nine days and was found to be faster on an 50% acrylic acid plasma polymer than on tissue culture polystyrene or a hydrocarbon plasma polymer, though cell growth was fastest on fibronectin precoated substrates. Expression of cellular alkaline phosphatase, collagen and calcium reached similar levels on the 50% acrylic acid plasma polymer, tissue

Kinetic model for electric-field induced point defect redistribution near semiconductor surfaces

Science.gov (United States)

Gorai, Prashun; Seebauer, Edmund G.

2014-07-01

The spatial distribution of point defects near semiconductor surfaces affects the efficiency of devices. Near-surface band bending generates electric fields that influence the spatial redistribution of charged mobile defects that exchange infrequently with the lattice, as recently demonstrated for pile-up of isotopic oxygen near rutile TiO2 (110). The present work derives a mathematical model to describe such redistribution and establishes its temporal dependence on defect injection rate and band bending. The model shows that band bending of only a few meV induces significant redistribution, and that the direction of the electric field governs formation of either a valley or a pile-up.

Kinetic model for electric-field induced point defect redistribution near semiconductor surfaces

International Nuclear Information System (INIS)

Gorai, Prashun; Seebauer, Edmund G.

2014-01-01

The spatial distribution of point defects near semiconductor surfaces affects the efficiency of devices. Near-surface band bending generates electric fields that influence the spatial redistribution of charged mobile defects that exchange infrequently with the lattice, as recently demonstrated for pile-up of isotopic oxygen near rutile TiO 2 (110). The present work derives a mathematical model to describe such redistribution and establishes its temporal dependence on defect injection rate and band bending. The model shows that band bending of only a few meV induces significant redistribution, and that the direction of the electric field governs formation of either a valley or a pile-up.

Fabrication of high aspect ratio nanocell lattices by ion beam irradiation

International Nuclear Information System (INIS)

Ishikawa, Osamu; Nitta, Noriko; Taniwaki, Masafumi

2016-01-01

Highlights: • Nanocell lattice with a high aspect ratio on InSb semiconductor surface was fabricated by ion beam irradiation. • The fabrication technique consisting of top-down and bottom-up processes was performed in FIB. • High aspect ratio of 2 was achieved in nanocell lattice with a 100 nm interval. • The intermediate-flux irradiation is favorable for fabrication of nanocell with a high aspect ratio. - Abstract: A high aspect ratio nanocell lattice was fabricated on the InSb semiconductor surface using the migration of point defects induced by ion beam irradiation. The fabrication technique consisting of the top-down (formation of voids and holes) and bottom-up (growth of voids and holes into nanocells) processes was performed using a focused ion beam (FIB) system. A cell aspect ratio of 2 (cell height/cell diameter) was achieved for the nanocell lattice with a 100 nm dot interval The intermediate-flux ion irradiation during the bottom-up process was found to be optimal for the fabrication of a high aspect ratio nanocell.

Colossal positive magnetoresistance in surface-passivated oxygen-deficient strontium titanite

KAUST Repository

David, Adrian

2015-05-15

Modulation of resistance by an external magnetic field, i.e. magnetoresistance effect, has been a long-lived theme of research due to both fundamental science and device applications. Here we report colossal positive magnetoresistance (CPMR) (>30,000% at a temperature of 2 K and a magnetic field of 9 T) discovered in degenerate semiconducting strontium titanite (SrTiO3) single crystals capped with ultrathin SrTiO3/LaAlO3 bilayers. The low-pressure high-temperature homoepitaxial growth of several unit cells of SrTiO3 introduces oxygen vacancies and high-mobility carriers in the bulk SrTiO3, and the three-unit-cell LaAlO3 capping layer passivates the surface and improves carrier mobility by suppressing surface-defect-related scattering. The coexistence of multiple types of carriers and inhomogeneous transport lead to the emergence of CPMR. This unit-cell-level surface engineering approach is promising to be generalized to others oxides, and to realize devices with high-mobility carriers and interesting magnetoelectronic properties.

High temperature thermoelectric properties of strontium titanate thin films with oxygen vacancy and niobium doping

KAUST Repository

Sarath Kumar, S. R.; Barasheed, Abeer Z.; Alshareef, Husam N.

2013-01-01

We report the evolution of high temperature thermoelectric properties of SrTiO3 thin films doped with Nb and oxygen vacancies. Structure-property relations in this important thermoelectric oxide are elucidated and the variation of transport properties with dopant concentrations is discussed. Oxygen vacancies are incorporated during growth or annealing in Ar/H2 above 800 K. An increase in lattice constant due to the inclusion of Nb and oxygen vacancies is found to result in an increase in carrier density and electrical conductivity with simultaneous decrease in carrier effective mass and Seebeck coefficient. The lattice thermal conductivity at 300 K is found to be 2.22 W m-1 K-1, and the estimated figure of merit is 0.29 at 1000 K. © 2013 American Chemical Society.

High temperature thermoelectric properties of strontium titanate thin films with oxygen vacancy and niobium doping

KAUST Repository

Sarath Kumar, S. R.

2013-08-14

We report the evolution of high temperature thermoelectric properties of SrTiO3 thin films doped with Nb and oxygen vacancies. Structure-property relations in this important thermoelectric oxide are elucidated and the variation of transport properties with dopant concentrations is discussed. Oxygen vacancies are incorporated during growth or annealing in Ar/H2 above 800 K. An increase in lattice constant due to the inclusion of Nb and oxygen vacancies is found to result in an increase in carrier density and electrical conductivity with simultaneous decrease in carrier effective mass and Seebeck coefficient. The lattice thermal conductivity at 300 K is found to be 2.22 W m-1 K-1, and the estimated figure of merit is 0.29 at 1000 K. © 2013 American Chemical Society.

Evaporation model for beam based additive manufacturing using free surface lattice Boltzmann methods

International Nuclear Information System (INIS)

Klassen, Alexander; Scharowsky, Thorsten; Körner, Carolin

2014-01-01

Evaporation plays an important role in many technical applications including beam-based additive manufacturing processes, such as selective electron beam or selective laser melting (SEBM/SLM). In this paper, we describe an evaporation model which we employ within the framework of a two-dimensional free surface lattice Boltzmann method. With this method, we solve the hydrodynamics as well as thermodynamics of the molten material taking into account the mass and energy losses due to evaporation and the recoil pressure acting on the melt pool. Validation of the numerical model is performed by measuring maximum melt depths and evaporative losses in samples of pure titanium and Ti–6Al–4V molten by an electron beam. Finally, the model is applied to create processing maps for an SEBM process. The results predict that the penetration depth of the electron beam, which is a function of the acceleration voltage, has a significant influence on evaporation effects. (paper)

Calculations of oscillation spectra of disordered interstitial solid solutions of vanadium-oxygen system

International Nuclear Information System (INIS)

Danilkin, S.A.

1978-01-01

The frequency spectra calculation of disordered solid interstitial solutions of a vanadium-oxygen system for oxygen concentration of 5.9% and 15.8% (V 16 O and V 16 O 3 ) is carried out. The axially-symmetric model of crystal lattice dinamics with consideration of vanadium-oxygen and vanadium-vanadium interactions up to the second coordination sphere is used. On the whole, the obtained spectra are in qualitative agreement with experiment and reflect correctly all the changes in frequency spectra of pure vanadium on doping with oxygen

Elimination of spurious lattice fermion solutions and noncompact lattice QCD

Energy Technology Data Exchange (ETDEWEB)

Lee, T.D.

1997-09-22

It is well known that the Dirac equation on a discrete hyper-cubic lattice in D dimension has 2{sup D} degenerate solutions. The usual method of removing these spurious solutions encounters difficulties with chiral symmetry when the lattice spacing l {ne} 0, as exemplified by the persistent problem of the pion mass. On the other hand, we recall that in any crystal in nature, all the electrons do move in a lattice and satisfy the Dirac equation; yet there is not a single physical result that has ever been entangled with a spurious fermion solution. Therefore it should not be difficult to eliminate these unphysical elements. On a discrete lattice, particle hop from point to point, whereas in a real crystal the lattice structure in embedded in a continuum and electrons move continuously from lattice cell to lattice cell. In a discrete system, the lattice functions are defined only on individual points (or links as in the case of gauge fields). However, in a crystal the electron state vector is represented by the Bloch wave functions which are continuous functions in {rvec {gamma}}, and herein lies one of the essential differences.

Oxygen Plasma Treatment of Rubber Surface by the Atmospheric Pressure Cold Plasma Torch

DEFF Research Database (Denmark)

Lee, Bong-ju; Kusano, Yukihiro; Kato, Nobuko

1997-01-01

adhesive. The adhesion property was improved by treatment of the rubber compound with plasma containing oxygen radicals. Physical and chemical changes of the rubber surface as a result of the plasma treatment were analyzed by field emission scanning electron microscopy (FE-SEM) and fourier transform......A new application of the atmospheric cold plasma torch has been investigated. Namely, the surface treatment of an air-exposed vulcanized rubber compound. The effect of plasma treatment was evaluated by the bondability of the treated rubber compound with another rubber compound using a polyurethane...

Lattice fermions

Energy Technology Data Exchange (ETDEWEB)

Randjbar-Daemi, S

1995-12-01

The so-called doubling problem in the lattice description of fermions led to a proof that under certain circumstances chiral gauge theories cannot be defined on the lattice. This is called the no-go theorem. It implies that if {Gamma}/sub/A is defined on a lattice then its infrared limit, which should correspond to the quantum description of the classical action for the slowly varying fields on lattice scale, is inevitably a vector like theory. In particular, if not circumvented, the no-go theorem implies that there is no lattice formulation of the Standard Weinberg-Salam theory or SU(5) GUT, even though the fermions belong to anomaly-free representations of the gauge group. This talk aims to explain one possible attempt at bypassing the no-go theorem. 20 refs.

Lattice fermions

International Nuclear Information System (INIS)

Randjbar-Daemi, S.

1995-12-01

The so-called doubling problem in the lattice description of fermions led to a proof that under certain circumstances chiral gauge theories cannot be defined on the lattice. This is called the no-go theorem. It implies that if Γ/sub/A is defined on a lattice then its infrared limit, which should correspond to the quantum description of the classical action for the slowly varying fields on lattice scale, is inevitably a vector like theory. In particular, if not circumvented, the no-go theorem implies that there is no lattice formulation of the Standard Weinberg-Salam theory or SU(5) GUT, even though the fermions belong to anomaly-free representations of the gauge group. This talk aims to explain one possible attempt at bypassing the no-go theorem. 20 refs

Periodic density functional theory study of ethylene hydrogenation over Co3O4 (1 1 1) surface: The critical role of oxygen vacancies

International Nuclear Information System (INIS)

Lu, Jinhui; Song, JiaJia; Niu, Hongling; Pan, Lun; Zhang, Xiangwen; Wang, Li; Zou, Ji-Jun

2016-01-01

Highlights: • H 2 dissociates in heterolytic way following H atoms migration to form O−H bond. • H 2 dissociation occurs at low temperature on perfect and oxygen defective Co 3 O 4 . • Oxygen vacancy promotes hydrogenation thermodynamically and kinetically. • O−H bond is weakened on oxygen defective surface. • Hydrogenation requires compromise between H−H activation and O−H breakage. - Abstract: Recently, metal oxides are attracting increasing interests as hydrogenation catalyst. Herein we studied the hydrogenation of ethylene on perfect and oxygen defective Co 3 O 4 (1 1 1) using periodic density functional theory. The energetics and pathways of ethylene hydrogenation to ethane were determined. We have demonstrated that (i) H 2 dissociation on Co 3 O 4 is a complicated two-step process through a heterolytic cleavage, followed by the migration of H atom and finally yields the homolytic product on both perfect and oxygen defective Co 3 O 4 (1 1 1) surfaces easily. (ii) After introducing the surface oxygen vacancy, the stepwise hydrogenation of ethylene by atomic hydrogen is much easier than that on perfect surface due to the weaker bond strength of OH group. The strength of O−H bond is a crucial factor for the hydrogenation reaction which involves the breakage of O−H bond. The formation of oxygen vacancy increases the electronic charges at the adjacent surface O, which reduces its capability of further gaining electrons from adsorbed atomic hydrogen and then weakens the strength of O−H bond. These results emphasize the importance of the oxygen vacancies for hydrogenation on metal oxides.

Oxygen defects in Fe-substituted Tl-system superconductors

Institute of Scientific and Technical Information of China (English)

李阳; 曹国辉; 王耘波; 马庆珠; 熊小涛; 陈宁; 马如璋; 郭应焕; 许祝安; 王劲松; 张小俊; 焦正宽; 彭获田; 周思海

1996-01-01

For Fe-doped T1-1223 phase,the excess oxygen defects induced by Fe dopants are studied by means of Hall coefficient,thermogravimetric measurements,Mossbauer spectroscopy,and the model calculation of the effective bond valence.The extra oxygen defects have effects on carrier density and microstructure of the superconductors.In the light doping level of Fe (x=0-0.05),the superconducting transition and carrier density have significant corresponding relation--the zero resistance temperature Tco and carrier densities decrease linearly with Fe dopants increasing.The thermogravimetric measurements show that the Fe3+ ions’ substituting for Cu2+ ions can bring the extra oxygen into the lattice to form extra oxygen defects.The calculation of the effective bond valence shows that the decrease of carrier density originates the strongly localized binding of the extra oxygen defects.The distortion of Cu-O layer induced by the extra oxygen defects decreases the superconductive transition temperature.The microstructure

Improved surface corrosion resistance of WE43 magnesium alloy by dual titanium and oxygen ion implantation

Energy Technology Data Exchange (ETDEWEB)

Zhao, Ying [Department of Orthopaedics and Traumatology, The University of Hong Kong, Pokfulam, Hong Kong (China); Department of Physics and Materials Science, City University of Hong Kong, Tat Chee Avenue, Kowloon, Hong Kong (China); Wu, Guosong; Lu, Qiuyuan [Department of Physics and Materials Science, City University of Hong Kong, Tat Chee Avenue, Kowloon, Hong Kong (China); Wu, Jun [Department of Orthopaedics and Traumatology, The University of Hong Kong, Pokfulam, Hong Kong (China); Xu, Ruizhen [Department of Physics and Materials Science, City University of Hong Kong, Tat Chee Avenue, Kowloon, Hong Kong (China); Yeung, Kelvin W.K., E-mail: wkkyeung@hku.hk [Department of Orthopaedics and Traumatology, The University of Hong Kong, Pokfulam, Hong Kong (China); Chu, Paul K., E-mail: paul.chu@cityu.edu.hk [Department of Physics and Materials Science, City University of Hong Kong, Tat Chee Avenue, Kowloon, Hong Kong (China)

2013-02-01

Magnesium alloys are potential biodegradable materials and have attracted much attention due to their outstanding biological performance and mechanical properties. However, their rapid degradation inside the human body cannot meet clinical needs. In order to improve the corrosion resistance, dual titanium and oxygen ion implantation is performed to modify the surface of the WE43 magnesium alloy. X-ray photoelectron spectroscopy is used to characterize the microstructures in the near surface layer and electrochemical impedance spectroscopy, potentiodynamic polarization, and immersion tests are employed to investigate the corrosion resistance of the implanted alloys in simulated body fluids. The results indicate that dual titanium and oxygen ion implantation produces a TiO{sub 2}-containing surface film which significantly enhances the corrosion resistance of WE43 magnesium alloy. Our data suggest a simple and practical means to improve the corrosion resistance of degradable magnesium alloys. - Highlights: ► Surface modification of WE43 magnesium alloy using dual ion implantation ► Dual Ti and O ion implantation produces a homogeneous TiO{sub 2}-containing surface film ► Significant improvement of the alloy corrosion resistance after the dual ion implantation.

The coupling effect of gas-phase chemistry and surface reactions on oxygen permeation and fuel conversion in ITM reactors

KAUST Repository

Hong, Jongsup

2015-08-01

© 2015 Elsevier B.V. The effect of the coupling between heterogeneous catalytic reactions supported by an ion transport membrane (ITM) and gas-phase chemistry on fuel conversion and oxygen permeation in ITM reactors is examined. In ITM reactors, thermochemical reactions take place in the gas-phase and on the membrane surface, both of which interact with oxygen permeation. However, this coupling between gas-phase and surface chemistry has not been examined in detail. In this study, a parametric analysis using numerical simulations is conducted to investigate this coupling and its impact on fuel conversion and oxygen permeation rates. A thermochemical model that incorporates heterogeneous chemistry on the membrane surface and detailed chemical kinetics in the gas-phase is used. Results show that fuel conversion and oxygen permeation are strongly influenced by the simultaneous action of both chemistries. It is shown that the coupling somewhat suppresses the gas-phase kinetics and reduces fuel conversion, both attributed to extensive thermal energy transfer towards the membrane which conducts it to the air side and radiates to the reactor walls. The reaction pathway and products, in the form of syngas and C2 hydrocarbons, are also affected. In addition, the operating regimes of ITM reactors in which heterogeneous- or/and homogeneous-phase reactions predominantly contribute to fuel conversion and oxygen permeation are elucidated.

Inelastic neutron scattering and lattice dynamics of GaPO4

International Nuclear Information System (INIS)

Mittal, R.; Chaplot, S.L.; Kolesnikov, A.I.; Loong, C.K.; Jayakumar, O.D.; Kulshreshtha, S.K.

2004-01-01

We report here measurements of phonon spectrum and lattice dynamical calculations for GaPO 4 . The measurements in low-cristobalite phase of GaPO 4 are carried out using high-resolution medium-energy chopper spectrometer at ANL, USA in the energy transfer range 0-160 MeV. Semiempirical interatomic potential in GaPO 4 , previously determined using ab-initio calculations have been widely used in studying the phase transitions among various polymorphs. The calculated phonon spectrum using the available potential show fair agreement with the experimental data. However, the agreement between the two is improved by including the polarisability of the oxygen atoms in the framework of the shell model. The lattice dynamical models are also exploited for calculations of various thermodynamic properties of GaPO 4 . (author)

Measurement of oxygen thermomigration in a hypostoichiometric mixed oxide

International Nuclear Information System (INIS)

Norris, D.I.R.; Coleman, S.C.; Kay, P.

1978-08-01

A method of determining oxygen to metal ratios in hypostoichiometric (U, Ce)Osub(2-x) by means of lattice parameter measurement and its application to thermomigration experiments is described. The technique is shown to compare favourably with other methods when a simple structure prevails. It is found that oxygen redistributes down an imposed temperature gradient, confirming theoretical predictions, and that the measured Arrhenius slope decreases as the cerium valency decreases. This effect is more marked than in (U, Pu)Osub(2-x). The results are attributable to solid state transport of oxygen vacancies and suggest that immobile complexes incorporating some oxygen deficiency are more easily formed in (U, Ce)Osub(2-x) than in (U, Pu)Osub(2-x). (author)

Theory and development of fluorescence-based optochemical oxygen sensors: oxygen optodes.

Science.gov (United States)

Opitz, N; Lübbers, D W

1987-01-01

As the preceding considerations concerning the physical and technical features of oxygen optodes have demonstrated, fluorescence-based optochemical oxygen sensors possess certain advantages and peculiarities compared to conventionally applied electrochemical sensors such as polarographic oxygen electrodes. First, in contrast to oxygen electrodes, oxygen measurements with oxygen optodes do not suffer from distortions caused by the reference electrodes. In addition, because of the polarographic process, platinum electrodes continuously consume oxygen, which falsifies the results, especially when small sample volumes or long-term measurements, or both, are involved, whereas the sensor layer of oxygen optodes must only be equilibrated. Moreover, the surface of the platinum wire has to be catalytically clean in order to obtain a plateau of the polarogram and, consequently, to achieve a low rest current at zero PO2. Unfortunately, the demand for catalytically clean platinum surfaces turns out to be rather critical, since surface contamination occurs even with membranized electrodes, resulting in the well-known phenomenon of "electrode poisoning." The question of the specificity of oxygen electrodes also must be considered. In this context, CO2 and halothane may interfere with oxygen measurements, whereas fluorescence quenching is unaffected by CO2 and halothane affects the measurements only slightly, depending on the special indicator used. Furthermore, because of the flow dependence, oxygen measurements with the oxygen electrode show a distinct "stirring effect" caused by the turbulence in front of the electrode, which disturbs the diffusion field. Because of the completely different physical principle of fluorescence optical sensors, such influences are not observed with oxygen optodes. In addition, isolation and shielding of electrical circuits found in electrodes are not necessary for optodes. Furthermore, the sensitivity of oxygen optodes can be tuned to the desired

ReaxFF Grand Canonical Monte Carlo simulation of adsorption and dissociation of oxygen on platinum (111)

Science.gov (United States)

Valentini, Paolo; Schwartzentruber, Thomas E.; Cozmuta, Ioana

2011-12-01

Atomic-level Grand Canonical Monte Carlo (GCMC) simulations equipped with a reactive force field (ReaxFF) are used to study atomic oxygen adsorption on a Pt(111) surface. The off-lattice GCMC calculations presented here rely solely on the interatomic potential and do not necessitate the pre-computation of surface adlayer structures and their interpolation. As such, they provide a predictive description of adsorbate phases. In this study, validation is obtained with experimental evidence (steric heats of adsorption and isotherms) as well as DFT-based state diagrams available in the literature. The ReaxFF computed steric heats of adsorption agree well with experimental data, and this study clearly shows that indirect dissociative adsorption of O2 on Pt(111) is an activated process at non-zero coverages, with an activation energy that monotonically increases with coverage. At a coverage of 0.25 ML, a highly ordered p(2 × 2) adlayer is found, in agreement with several low-energy electron diffraction observations. Isotherms obtained from the GCMC simulations compare qualitatively and quantitatively well with previous DFT-based state diagrams, but are in disagreement with the experimental data sets available. ReaxFF GCMC simulations at very high coverages show that O atoms prefer to bind in fcc hollow sites, at least up to 0.8 ML considered in the present work. At moderate coverages, little to no disorder appears in the Pt lattice. At high coverages, some Pt atoms markedly protrude out of the surface plane. This observation is in qualitative agreement with recent STM images of an oxygen covered Pt surface. The use of the GCMC technique based on a transferable potential is particularly valuable to produce more realistic systems (adsorbent and adsorbate) to be used in subsequent dynamical simulations (Molecular Dynamics) to address recombination reactions (via either Eley-Rideal or Langmuir-Hinshelwood mechanisms) on variously covered surfaces. By using GCMC and Molecular

Lattice gauge theory

International Nuclear Information System (INIS)

Mack, G.

1982-01-01

After a description of a pure Yang-Mills theory on a lattice, the author considers a three-dimensional pure U(1) lattice gauge theory. Thereafter he discusses the exact relation between lattice gauge theories with the gauge groups SU(2) and SO(3). Finally he presents Monte Carlo data on phase transitions in SU(2) and SO(3) lattice gauge models. (HSI)

A density functional theory study of partial oxidation of propylene on Cu2O(0 0 1) and CuO(0 0 1) surfaces

Science.gov (United States)

Düzenli, Derya; Atmaca, Deniz Onay; Gezer, Miray Gülbiter; Onal, Isik

2015-11-01

This work theoretically investigates propylene epoxidation reaction on Cu2O(0 0 1) and CuO(0 0 1) surfaces using periodical DFT method to determine the active copper species within the reaction mechanism. The transition states and energy profiles are calculated for the formation of surface intermediates such as oxametallopropylene (OMP) over Cu2O(0 0 1) and oxygen bridging (OB) over CuO(0 0 1) and allylic H-stripping reaction (AHS) over both surfaces as well as for formation of products. Propylene oxide (PO) and acetone are obtained through OMP and OB surface intermediates and acrolein generation is observed through allylic H-stripping reaction (AHS). The calculations revealed that the corresponding surface intermediates for epoxidation reaction need to overcome an activation barrier of 13 kcal/mol over CuO surface whereas they occur without an energy barrier over Cu2O surface indicating the higher activity of Cu+ species. Acrolein is also found to be a thermodynamically more favorable product for both surfaces especially over CuO surface due to the presence of more surface oxygen atoms on which the basicity has been evaluated by the adsorption of sulfur dioxide. This indicates that the lattice oxygen inherent in both surface types does not participate in PO production.

Surface Pourbaix diagrams and oxygen reduction activity of Pt, Ag and Ni(111) surfaces studied by DFT

DEFF Research Database (Denmark)

Hansen, Heine Anton; Rossmeisl, Jan; Nørskov, Jens Kehlet

2008-01-01

The electrochemical most stable surface structures is investigated as function of pH and potential for Pt, Ag and Ni based on DFT calculations and constructed surface Pourbaix diagrams. It is also explained why metals such as Ag and Ni may be used successfully in alkaline fuel cells but not in ac......The electrochemical most stable surface structures is investigated as function of pH and potential for Pt, Ag and Ni based on DFT calculations and constructed surface Pourbaix diagrams. It is also explained why metals such as Ag and Ni may be used successfully in alkaline fuel cells...... but not in acidic PEM fuel cells. Based on density functional theory calculations we investigate the electrochemically most stable surface structures as a function of pH and electrostatic potential for Pt(111), Ag(111) and Ni(111), and we construct surface Pourbaix diagrams. We study the oxygen reduction reaction......, on the other hand, is constant vs. the standard hydrogen electrode (SHE). For Ag, this means that where the potential for dissolution and ORR are about the same at pH = 0, Ag becomes more stable relative to RHE as pH is increased. Hence the pH dependent stability offers an explanation for the possible use...

A Dirac-Kaehler approach to the two dimensional Wess-Zumino N=2 model on the lattice

International Nuclear Information System (INIS)

Zimerman, A.H.; Aratyn, H.

1983-08-01

We introduce a Dirac-Kaehler model for the two dimensional Wess-Zumino N=2 Lagrangean. We can show that in the model, when we go to the euclidean space-time lattive, we have no energy doubling, the action has no lattice surface terms (contrary to other authors), while the Hamiltonians (when time is continuous) present lattice surface terms. (orig.)

Error sources in the retrieval of aerosol information over bright surfaces from satellite measurements in the oxygen A band

Science.gov (United States)

Nanda, Swadhin; de Graaf, Martin; Sneep, Maarten; de Haan, Johan F.; Stammes, Piet; Sanders, Abram F. J.; Tuinder, Olaf; Pepijn Veefkind, J.; Levelt, Pieternel F.

2018-01-01

Retrieving aerosol optical thickness and aerosol layer height over a bright surface from measured top-of-atmosphere reflectance spectrum in the oxygen A band is known to be challenging, often resulting in large errors. In certain atmospheric conditions and viewing geometries, a loss of sensitivity to aerosol optical thickness has been reported in the literature. This loss of sensitivity has been attributed to a phenomenon known as critical surface albedo regime, which is a range of surface albedos for which the top-of-atmosphere reflectance has minimal sensitivity to aerosol optical thickness. This paper extends the concept of critical surface albedo for aerosol layer height retrievals in the oxygen A band, and discusses its implications. The underlying physics are introduced by analysing the top-of-atmosphere reflectance spectrum as a sum of atmospheric path contribution and surface contribution, obtained using a radiative transfer model. Furthermore, error analysis of an aerosol layer height retrieval algorithm is conducted over dark and bright surfaces to show the dependence on surface reflectance. The analysis shows that the derivative with respect to aerosol layer height of the atmospheric path contribution to the top-of-atmosphere reflectance is opposite in sign to that of the surface contribution - an increase in surface brightness results in a decrease in information content. In the case of aerosol optical thickness, these derivatives are anti-correlated, leading to large retrieval errors in high surface albedo regimes. The consequence of this anti-correlation is demonstrated with measured spectra in the oxygen A band from the GOME-2 instrument on board the Metop-A satellite over the 2010 Russian wildfires incident.

Detection of submonolayer oxygen-18 on a gold surface by nuclear reaction analysis

Energy Technology Data Exchange (ETDEWEB)

Wielunski, L.S.; Kenny, M.J.; Wieczorek, L. [Commonwealth Scientific and Industrial Research Organisation (CSIRO), Lindfield, NSW (Australia). Div. of Applied Physics

1993-12-31

A gold substrate is the preferred solid surface for formation of an organic self-assembled monolayer ( SAM ). Device fabrication process may require the gold film to be exposed to photolithographic processing and plasma treatment prior to molecular assembly. It has been observed that oxygen plasma treatment prevents the formation of SAMs; however, subsequent treatment with an argon plasma allows assembly of the organic monolayers. To understand the mechanisms involved, a plasma containing 98% {sup 18}O was used and the film surface was analysed using the {sup 18}O (p,{alpha}){sup 15}N nuclear reaction. 5 refs., 1 tab., 3 figs.

Detection of submonolayer oxygen-18 on a gold surface by nuclear reaction analysis

Energy Technology Data Exchange (ETDEWEB)

Wielunski, L S; Kenny, M J; Wieczorek, L [Commonwealth Scientific and Industrial Research Organisation (CSIRO), Lindfield, NSW (Australia). Div. of Applied Physics

1994-12-31

A gold substrate is the preferred solid surface for formation of an organic self-assembled monolayer ( SAM ). Device fabrication process may require the gold film to be exposed to photolithographic processing and plasma treatment prior to molecular assembly. It has been observed that oxygen plasma treatment prevents the formation of SAMs; however, subsequent treatment with an argon plasma allows assembly of the organic monolayers. To understand the mechanisms involved, a plasma containing 98% {sup 18}O was used and the film surface was analysed using the {sup 18}O (p,{alpha}){sup 15}N nuclear reaction. 5 refs., 1 tab., 3 figs.

Weyl solitons in three-dimensional optical lattices

Science.gov (United States)

Shang, Ce; Zheng, Yuanlin; Malomed, Boris A.

2018-04-01

Weyl fermions are massless chiral quasiparticles existing in materials known as Weyl semimetals. Topological surface states, associated with the unusual electronic structure in the Weyl semimetals, have been recently demonstrated in linear systems. Ultracold atomic gases, featuring laser-assisted tunneling in three-dimensional optical lattices, can be used for the emulation of Weyl semimetals, including nonlinear effects induced by the collisional nonlinearity of atomic Bose-Einstein condensates. We demonstrate that this setting gives rise to topological states in the form of Weyl solitons at the surface of the underlying optical lattice. These nonlinear modes, being exceptionally robust, bifurcate from linear states for a given quasimomentum. The Weyl solitons may be used to design an efficient control scheme for topologically protected unidirectional propagation of excitations in light-matter-interaction physics. After the recently introduced Majorana and Dirac solitons, the Weyl solitons proposed in this work constitute the third (and the last) member in this family of topological solitons.

Periodic density functional theory study of ethylene hydrogenation over Co3O4 (1 1 1) surface: The critical role of oxygen vacancies

Science.gov (United States)

Lu, Jinhui; Song, JiaJia; Niu, Hongling; Pan, Lun; Zhang, Xiangwen; Wang, Li; Zou, Ji-Jun

2016-05-01

Recently, metal oxides are attracting increasing interests as hydrogenation catalyst. Herein we studied the hydrogenation of ethylene on perfect and oxygen defective Co3O4 (1 1 1) using periodic density functional theory. The energetics and pathways of ethylene hydrogenation to ethane were determined. We have demonstrated that (i) H2 dissociation on Co3O4 is a complicated two-step process through a heterolytic cleavage, followed by the migration of H atom and finally yields the homolytic product on both perfect and oxygen defective Co3O4 (1 1 1) surfaces easily. (ii) After introducing the surface oxygen vacancy, the stepwise hydrogenation of ethylene by atomic hydrogen is much easier than that on perfect surface due to the weaker bond strength of OH group. The strength of Osbnd H bond is a crucial factor for the hydrogenation reaction which involves the breakage of Osbnd H bond. The formation of oxygen vacancy increases the electronic charges at the adjacent surface O, which reduces its capability of further gaining electrons from adsorbed atomic hydrogen and then weakens the strength of Osbnd H bond. These results emphasize the importance of the oxygen vacancies for hydrogenation on metal oxides.

On non local elasticity and its relation with lattice dynamics

International Nuclear Information System (INIS)

Idiodi, J.O.A.

1984-11-01

In this paper we have modelled a three-dimensional discrete lattice by a nonlocal continuum which possesses dispersive phonons. Previous efforts in the development of non-local theories appear not to have paid much attention to establishing actual contact with the nontrivial models frequently employed in lattice dynamics. As a first attempt in this direction, we present in this paper explicit results for the form of a non-local stress-tensor that describes exactly the lattice dynamical model of Gazis, Herman and Wallis. This model takes into account angular stiffness forces involving consecutive nearest neighbours forming a right angle at equilibrium. In addition, a general result for the surface eigenmodes of a semi-finite isotropic medium is derived. One of the justifications for this kind of study is the simpler approach it offers to the problems of interest in lattice dynamics. (author)

Continuous surface force based lattice Boltzmann equation method for simulating thermocapillary flow

International Nuclear Information System (INIS)

Zheng, Lin; Zheng, Song; Zhai, Qinglan

2016-01-01

In this paper, we extend a lattice Boltzmann equation (LBE) with continuous surface force (CSF) to simulate thermocapillary flows. The model is designed on our previous CSF LBE for athermal two phase flow, in which the interfacial tension forces and the Marangoni stresses as the results of the interface interactions between different phases are described by a conception of CSF. In this model, the sharp interfaces between different phases are separated by a narrow transition layers, and the kinetics and morphology evolution of phase separation would be characterized by an order parameter via Cahn–Hilliard equation which is solved in the frame work of LBE. The scalar convection–diffusion equation for temperature field is resolved by thermal LBE. The models are validated by thermal two layered Poiseuille flow, and two superimposed planar fluids at negligibly small Reynolds and Marangoni numbers for the thermocapillary driven convection, which have analytical solutions for the velocity and temperature. Then thermocapillary migration of two/three dimensional deformable droplet are simulated. Numerical results show that the predictions of present LBE agreed with the analytical solution/other numerical results. - Highlights: • A CSF LBE to thermocapillary flows. • Thermal layered Poiseuille flows. • Thermocapillary migration.

Continuous surface force based lattice Boltzmann equation method for simulating thermocapillary flow

Energy Technology Data Exchange (ETDEWEB)

Zheng, Lin, E-mail: lz@njust.edu.cn [School of Energy and Power Engineering, Nanjing University of Science and Technology, Nanjing 210094 (China); Zheng, Song [School of Mathematics and Statistics, Zhejiang University of Finance and Economics, Hangzhou 310018 (China); Zhai, Qinglan [School of Economics Management and Law, Chaohu University, Chaohu 238000 (China)

2016-02-05

In this paper, we extend a lattice Boltzmann equation (LBE) with continuous surface force (CSF) to simulate thermocapillary flows. The model is designed on our previous CSF LBE for athermal two phase flow, in which the interfacial tension forces and the Marangoni stresses as the results of the interface interactions between different phases are described by a conception of CSF. In this model, the sharp interfaces between different phases are separated by a narrow transition layers, and the kinetics and morphology evolution of phase separation would be characterized by an order parameter via Cahn–Hilliard equation which is solved in the frame work of LBE. The scalar convection–diffusion equation for temperature field is resolved by thermal LBE. The models are validated by thermal two layered Poiseuille flow, and two superimposed planar fluids at negligibly small Reynolds and Marangoni numbers for the thermocapillary driven convection, which have analytical solutions for the velocity and temperature. Then thermocapillary migration of two/three dimensional deformable droplet are simulated. Numerical results show that the predictions of present LBE agreed with the analytical solution/other numerical results. - Highlights: • A CSF LBE to thermocapillary flows. • Thermal layered Poiseuille flows. • Thermocapillary migration.

Function of TiO2 Lattice Defects toward Photocatalytic Processes: View of Electronic Driven Force

Directory of Open Access Journals (Sweden)

Huanan Cui

2013-01-01

Full Text Available Oxygen vacancies and Ti-related defects (OTDs are the main lattice defects of TiO2, which have great influence on its photocatalytic activity. To understand the relationship between the defects and photocatalytic activities, detailed discussions based on the electronic driven force provided by these defects are carried out during the three commonly accepted processes in photocatalytic reactions. It is found that these defects inevitably (i influence the energy structure of the pristine TiO2 as the isolate acceptor/donor level or hybrid with the original orbital, (ii provide a disordered short-range force that confuses the charge carriers transferring to surface active sites, (iii act not only as the surface active sites for trapping the charge carriers but also as the main chemisorption sites for O2, H2O, and organic species. These effects of the defects make them one of the key factors that determine the efficiency of heterogeneous photocatalysis. Clarifying the role of the defects will further facilitate the exploration and the construction of high-performance photocatalysts for practical applications.

Atomic scale study of the chemistry of oxygen, hydrogen and water at SiC surfaces

International Nuclear Information System (INIS)

Amy, Fabrice

2007-01-01

Understanding the achievable degree of homogeneity and the effect of surface structure on semiconductor surface chemistry is both academically challenging and of great practical interest to enable fabrication of future generations of devices. In that respect, silicon terminated SiC surfaces such as the cubic 3C-SiC(1 0 0) 3 x 2 and the hexagonal 6H-SiC(0 0 0 1) 3 x 3 are of special interest since they give a unique opportunity to investigate the role of surface morphology on oxygen or hydrogen incorporation into the surface. In contrast to silicon, the subsurface structure plays a major role in the reactivity, leading to unexpected consequences such as the initial oxidation starting several atomic planes below the top surface or the surface metallization by atomic hydrogen. (review article)

Area of Lattice Polygons

Science.gov (United States)

Scott, Paul

2006-01-01

A lattice is a (rectangular) grid of points, usually pictured as occurring at the intersections of two orthogonal sets of parallel, equally spaced lines. Polygons that have lattice points as vertices are called lattice polygons. It is clear that lattice polygons come in various shapes and sizes. A very small lattice triangle may cover just 3…

Investigation on Selective Laser Melting AlSi10Mg Cellular Lattice Strut: Molten Pool Morphology, Surface Roughness and Dimensional Accuracy

Directory of Open Access Journals (Sweden)

Xuesong Han

2018-03-01

Full Text Available AlSi10Mg inclined struts with angle of 45° were fabricated by selective laser melting (SLM using different scanning speed and hatch spacing to gain insight into the evolution of the molten pool morphology, surface roughness, and dimensional accuracy. The results show that the average width and depth of the molten pool, the lower surface roughness and dimensional deviation decrease with the increase of scanning speed and hatch spacing. The upper surface roughness is found to be almost constant under different processing parameters. The width and depth of the molten pool on powder-supported zone are larger than that of the molten pool on the solid-supported zone, while the width changes more significantly than that of depth. However, if the scanning speed is high enough, the width and depth of the molten pool and the lower surface roughness almost keep constant as the density is still high. Therefore, high dimensional accuracy and density as well as good surface quality can be achieved simultaneously by using high scanning speed during SLMed cellular lattice strut.

Investigation on Selective Laser Melting AlSi10Mg Cellular Lattice Strut: Molten Pool Morphology, Surface Roughness and Dimensional Accuracy.

Science.gov (United States)

Han, Xuesong; Zhu, Haihong; Nie, Xiaojia; Wang, Guoqing; Zeng, Xiaoyan

2018-03-07

AlSi10Mg inclined struts with angle of 45° were fabricated by selective laser melting (SLM) using different scanning speed and hatch spacing to gain insight into the evolution of the molten pool morphology, surface roughness, and dimensional accuracy. The results show that the average width and depth of the molten pool, the lower surface roughness and dimensional deviation decrease with the increase of scanning speed and hatch spacing. The upper surface roughness is found to be almost constant under different processing parameters. The width and depth of the molten pool on powder-supported zone are larger than that of the molten pool on the solid-supported zone, while the width changes more significantly than that of depth. However, if the scanning speed is high enough, the width and depth of the molten pool and the lower surface roughness almost keep constant as the density is still high. Therefore, high dimensional accuracy and density as well as good surface quality can be achieved simultaneously by using high scanning speed during SLMed cellular lattice strut.

Photogeneration of singlet oxygen by the phenothiazine derivatives covalently bound to the surface-modified glassy carbon

Energy Technology Data Exchange (ETDEWEB)

Blacha-Grzechnik, Agata, E-mail: agata.blacha@polsl.pl [Faculty of Chemistry, Silesian University of Technology, Strzody 9, 44-100 Gliwice (Poland); Piwowar, Katarzyna; Krukiewicz, Katarzyna [Faculty of Chemistry, Silesian University of Technology, Strzody 9, 44-100 Gliwice (Poland); Koscielniak, Piotr; Szuber, Jacek [Institute of Electronics, Silesian University of Technology, Akademicka 16, 44-100 Gliwice (Poland); Zak, Jerzy K. [Faculty of Chemistry, Silesian University of Technology, Strzody 9, 44-100 Gliwice (Poland)

2016-05-15

Highlights: • The selected group of four NH{sub 2}-derivatives of phenothiazine was grafted to Glassy Carbon (GC) surface. • The grafted phenothiazines are able to generate {sup 1}O{sub 2} when activated by the radiation. • Such modified solid surfaces may find their application in the wastewater treatment. - Abstract: The selected group of four amine-derivatives of phenothiazine was covalently grafted to the glassy carbon surface in the four-step procedure consisting of the electrochemical reduction of the diazonium salt followed by the electrochemical and chemical post-modification steps. The proposed strategy involves the bonding of linker molecule to which the photosensitizer is attached. The synthesized organic layers were characterized by means of cyclic voltammetry, XPS and Raman Spectroscopy. It was shown that the phenothiazines immobilized via proposed strategy retain their photochemical properties and are able to generate {sup 1}O{sub 2} when activated by the laser radiation. The effectiveness of in situ singlet oxygen generation by those new solid photoactive materials was determined by means of UVVis spectroscopy. The reported, covalently modified solid surfaces may find their application as the singlet oxygen photogenerators in the fine chemicals’ synthesis or in the wastewater treatment.

Enhanced thermoelectric property of oxygen deficient nickel doped SnO2 for high temperature application

Science.gov (United States)

Paulson, Anju; Sabeer, N. A. Muhammad; Pradyumnan, P. P.

2018-04-01

Motivated by the detailed investigation on the thermoelectric performance of oxide materials our work concentrated on the influence of acceptor dopants and defect density in the lattice plane for the enhancement of thermoelectric power. The series of Sn1‑x Nix O2 (0.01 ≤ x ≤ 0.05) compositions were prepared by solid state reaction mechanism and found that 3 atomic percentage Ni doped SnO2 can be considered as a good candidate due to its promising electrical and transport properties. Defect lattices were introduced in the sample and the deviation from oxygen stochiometry was ensured using photoluminescence measurement. High power factor was obtained for the 3 atomic percentage nickel doped SnO2 due to the effective number of charge carrier concentration and the depletion of oxygen rich layers. Defect centered and acceptor doped SnO2 lattice opens a new door for energy harvesting at higher temperatures.

A quantum-chemical study of oxygen-vacancy defects in PbTiO3 crystals

International Nuclear Information System (INIS)

Stashans, Arvids; Serrano, Sheyla; Medina, Paul

2006-01-01

Investigation of an oxygen vacancy and F center in the cubic and tetragonal lattices of PbTiO 3 crystals is done by means of quantum-chemical simulations. Displacements of defect-surrounding atoms, electronic and optical properties, lattice relaxation energies and some new effects due to the defects presence are reported and analyzed. A comparison with similar studies is made and conclusions are drawn on the basis of the obtained results

Oxygen-enabled control of Dzyaloshinskii-Moriya Interaction in ultra-thin magnetic films

KAUST Repository

Belabbes, Abderrezak; Bihlmayer, Gustav; Blü gel, Stefan; Manchon, Aurelien

2016-01-01

ferromagnets, resulting in spin spirals and nanoskyrmion lattices. Here, using relativistic first-principles calculations, we demonstrate that the magnitude and sign of DMI can be entirely controlled by tuning the oxygen coverage of the magnetic film, therefore

Stability and oxygen transport property of La0.8Sr0.2Cr0.5Fe0.5O3 -δ

DEFF Research Database (Denmark)

He, Wei; Huang, Hua; Chen, Ming

2014-01-01

vacancies in the lattice. LSCrF powder exposed to flowing concentrated hydrogen for 30 h was found to decompose partially. The decomposition oxygen partial pressure of LSCrF at 950 °C was estimated to be 6.3 × 10- 28 atm from thermodynamic calculations. The stability of LSCrF under an oxygen chemical......The stability of La0.8Sr0.2Cr0.5Fe 0.5O3 -δ (LSCrF) in reducing atmosphere was investigated by examining the extent of its reaction with hydrogen at elevated temperature. LSCrF powder exposed to diluted hydrogen was found to loss a weight of only ~ 0.5%, corresponding to the formation of oxygen...... potential gradient was also examined by exposing a disk-shaped dense sample to air at one side and to reducing atmosphere (CO) at the other side at elevated temperatures. A thin, porous layer was found to form on the CO side surface. An oxygen permeation flux of 2.5 × 10- 7 mol cm- 2 s- 1 was observed...

Theory of the oxygen-induced restructuring of Cu(110) and Cu(100) surfaces

DEFF Research Database (Denmark)

Jacobsen, Karsten Wedel; Nørskov, Jens Kehlet

1990-01-01

A model calculation based on the effective-medium theory of the oxygen-induced reconstruction of the (110) and (100) surfaces of Cu is presented. Equilibrium structures are calculated from a minimization of the total energy of the system. Missing-row-type reconstructions are found to be most stable...... in both cases, and an analysis is presented, showing what the driving force is behind these reconstructions....

Lattice Constant Dependence on Particle Size for Ceria prepared from a Citrate Sol-Gel

International Nuclear Information System (INIS)

Morris, V N; Farrell, R A; Sexton, A M; Morris, M A

2006-01-01

High surface area ceria nanoparticles have been prepared using a citrate solgel precipitation method. Changes to the particle size have been made by calcining the ceria powders at different temperatures, and X-ray methods used to determine their lattice parameters. The particle sizes have been assessed using transmission electron microscopy (TEM) and the lattice parameter found to fall with decreasing particle size. The results are discussed in the light of the role played by surface tension effects

Identifying the Active Surfaces of Electrochemically Tuned LiCoO2 for Oxygen Evolution Reaction

International Nuclear Information System (INIS)

Lu, Zhiyi; Chen, Guangxu; Li, Yanbin; Wang, Haotian; Xie, Jin

2017-01-01

Identification of active sites for catalytic processes has both fundamental and technological implications for rational design of future catalysts. Herein, we study the active surfaces of layered lithium cobalt oxide (LCO) for the oxygen evolution reaction (OER) using the enhancement effect of electrochemical delithiation (De-LCO). Our theoretical results indicate that the most stable (0001) surface has a very large overpotential for OER independent of lithium content. In contrast, edge sites such as the nonpolar (1120) and polar (0112) surfaces are predicted to be highly active and dependent on (de)lithiation. The effect of lithium extraction from LCO on the surfaces and their OER activities can be understood by the increase of Co 4+ sites relative to Co 3+ and by the shift of active oxygen 2p states. Experimentally, it is demonstrated that LCO nanosheets, which dominantly expose the (0001) surface show negligible OER enhancement upon delithiation. However, a noticeable increase in OER activity (~0.1 V in overpotential shift at 10 mA cm –2 ) is observed for the LCO nanoparticles, where the basal plane is greatly diminished to expose the edge sites, consistent with the theoretical simulations. In addition, we find that the OER activity of De-LCO nanosheets can be improved if we adopt an acid etching method on LCO to create more active edge sites, which in turn provides a strong evidence for the theoretical indication.

Analyzing the dependence of oxygen incorporation current density on overpotential and oxygen partial pressure in mixed conducting oxide electrodes.

Science.gov (United States)

Guan, Zixuan; Chen, Di; Chueh, William C

2017-08-30

The oxygen incorporation reaction, which involves the transformation of an oxygen gas molecule to two lattice oxygen ions in a mixed ionic and electronic conducting solid, is a ubiquitous and fundamental reaction in solid-state electrochemistry. To understand the reaction pathway and to identify the rate-determining step, near-equilibrium measurements have been employed to quantify the exchange coefficients as a function of oxygen partial pressure and temperature. However, because the exchange coefficient contains contributions from both forward and reverse reaction rate constants and depends on both oxygen partial pressure and oxygen fugacity in the solid, unique and definitive mechanistic assessment has been challenging. In this work, we derive a current density equation as a function of both oxygen partial pressure and overpotential, and consider both near and far from equilibrium limits. Rather than considering specific reaction pathways, we generalize the multi-step oxygen incorporation reaction into the rate-determining step, preceding and following quasi-equilibrium steps, and consider the number of oxygen ions and electrons involved in each. By evaluating the dependence of current density on oxygen partial pressure and overpotential separately, one obtains the reaction orders for oxygen gas molecules and for solid-state species in the electrode. We simulated the oxygen incorporation current density-overpotential curves for praseodymium-doped ceria for various candidate rate-determining steps. This work highlights a promising method for studying the exchange kinetics far away from equilibrium.

Orientation of quartz nanocrystallites in the silicon lattice

International Nuclear Information System (INIS)

Kalanov, M.U.; Ibragimova, E.M.; Khamraeva, R.N.; Rustamova, V.M.; Ummatov, Kh.D.

2006-01-01

Full text: Basing on the study of medium angle diffuse X-ray scattering from silicon single crystals, it was supposed to be due to rod like oxygen precipitates. It was shown by us later, that depending on the growth conditions, as-grown silicon single crystals contain quartz crystal inclusions at an amount of 0.3 / 0.5 wt. % . Since it has not been done before, the aim of this work was to study the shape and orientation of quartz inclusions relative to a chosen axis of the silicon crystal lattice. We studied p-Si single crystals of one crucible origin with the specific resistance ρ 0 ≅ 1/10 Ohm· cm with different cut surfaces parallel to the crystal planes (100), (110) and (111). All the samples were cut and polished in the bar form with the sizes of 20x12x1.5 mm 3 . The dislocation density was N D ≅ 10 1 /10 3 cm -2 , the concentrations of oxygen and boron were N O ≅ 2/ 4 x10 17 cm -3 and N B ≅ 3· 10 1 5 c m -3 . Structure was analyzed at the set-up DRON-3M ( λ Cu K∝ = 0.1542 nm) at the room temperature in the angle range of angles 2Θ = 10/70 deg. The diffraction spectrum of the sample cut in (111) includes 5 selective reflections and the only diffuse one at 2Θ≅ 20 deg (d/n≅ 0.3136 nm), having a large width 0.1032 rad, which is due to presence of amorphous SiO x precipitate in the surface layer of silicon single crystal. The dominative selective line with d/n≅ 0.3136 nm at 2Θ≅ 28.5 deg belongs to reflection from (111) planes of the silicon lattice and the second less intensive one comes from the same planes with Cu K β radiation. Another selective reflection of a medium intensity at 2Θ≅ 59 deg with d/n≅ 0.1568 nm is its second order (222) and forbidden by the weakening laws. The rest narrow but weak lines with d/n≅ 0.3345 nm at 2Θ≅ 26.6 deg and 0.2468 nm at≅36.6 deg correspond to the diffraction reflections (101) and (110) from the crystal quartz lattice SiO 2 . It means that they are caused by optimally oriented quartz

SnO2 promoted by alkali metal oxides for soot combustion: The effects of surface oxygen mobility and abundance on the activity

Science.gov (United States)

Rao, Cheng; Shen, Jiating; Wang, Fumin; Peng, Honggen; Xu, Xianglan; Zhan, Hangping; Fang, Xiuzhong; Liu, Jianjun; Liu, Wenming; Wang, Xiang

2018-03-01

In this study, SnO2-based catalysts promoted by different alkali metal oxides with a Sn/M (M = Li, Na, K, Cs) molar ratio of 9/1 have been prepared for soot combustion. In comparison with the un-modified SnO2 support, the activity of the modified catalysts has been evidently enhanced, following the sequence of CsSn1-9 > KSn1-9 > NaSn1-9 > LiSn1-9 > SnO2. As testified by Raman, H2-TPR, soot-TPR-MS, XPS and O2-TPD results, the incorporation of various alkali metal oxides can induce the formation of more abundant and mobile oxygen species on the surface of the catalysts. Moreover, quantified results have proved that the amount of the surface active oxygen species is nearly proportional to the activity of the catalysts. CsSn1-9, the catalyst promoted by cesium oxide, owns the largest amount of surface mobile oxygen species, thus having the highest activity among all the studied catalysts. It is concluded that the amount of surface active and mobile oxygen species is the major factor determining the activity of the catalysts for soot combustion.

Oxygen depletion of bismuth molybdates

Energy Technology Data Exchange (ETDEWEB)

Yong, L.K.; Howe, R.F.; Keulks, G.W.; Hall, W.K.

1978-05-01

Pure ..cap alpha..-phase bismuth molybdate (Bi/sub 2/Mo/sub 3/O/sub 12/), which is known to be weakly active for selective oxidation, and pure ..gamma..-phase bismuth molybdate (Bi/sub 2/MoO/sub 6/), which has good activity, were subjected to oxidation-reduction cycles with known amounts of hydrogen and oxygen, at 300/sup 0/-570/sup 0/C and with evacuation steps between treatments. The volume of oxygen consumed during reoxidation was equal to half the hydrogen consumed during the reduction on the ..cap alpha..-phase, which indicated that no hydrogen was retained during reduction. For the ..gamma..-phase, the oxygen consumption was greater than half of the hydrogen consumption and it increased with extent of reduction. The excess oxygen was apparently consumed by filling anion vacancies formed during outgassing subsequent to the reduction step. ESR spectroscopy and temperature-programed oxidation-reduction indicated that lattice oxide ions which bridge between bismuth and molybdenum layers of the koechlinite structure become more labile when the catalyst is in a partially reduced state, and that this effect is greater in the ..gamma..- than the ..cap alpha..-phase. Table and 15 references.

New integrable lattice hierarchies

International Nuclear Information System (INIS)

Pickering, Andrew; Zhu Zuonong

2006-01-01

In this Letter we give a new integrable four-field lattice hierarchy, associated to a new discrete spectral problem. We obtain our hierarchy as the compatibility condition of this spectral problem and an associated equation, constructed herein, for the time-evolution of eigenfunctions. We consider reductions of our hierarchy, which also of course admit discrete zero curvature representations, in detail. We find that our hierarchy includes many well-known integrable hierarchies as special cases, including the Toda lattice hierarchy, the modified Toda lattice hierarchy, the relativistic Toda lattice hierarchy, and the Volterra lattice hierarchy. We also obtain here a new integrable two-field lattice hierarchy, to which we give the name of Suris lattice hierarchy, since the first equation of this hierarchy has previously been given by Suris. The Hamiltonian structure of the Suris lattice hierarchy is obtained by means of a trace identity formula

Unraveling the facet-dependent and oxygen vacancy role for ethylene hydrogenation on Co_3O_4 (110) surface: A DFT+U study

International Nuclear Information System (INIS)

Zhang, Yong-Chao; Pan, Lun; Lu, Jinhui; Song, Jiajia; Li, Zheng; Zhang, Xiangwen; Wang, Li; Zou, Ji-Jun

2017-01-01

Highlights: • The mechanism of ethylene hydrogenation on perfect and oxygen defective Co_3O_4(110) is investigated by using DFT + U. • Oxygen vacancy promotes ethylene hydrogenation thermodynamically and kinetically. • The Co3O4 (110) facet is more active than the (111) one for ethylene hydrogenation. - Abstract: Crystal facet engineering and defect engineering are both critical strategies to improve the catalytic hydrogenation performance of catalyst. Herein, ethylene hydrogenation on the perfect and oxygen defective Co_3O_4(110) surfaces has been studied by using periodic density functional theory calculations. The results are compared with that on Co_3O_4(111) surface to clarify the problem of which facet for Co_3O_4 is more reactive, and to illuminate the role of oxygen vacancy. The low oxygen vacancy formation energy suggests that Co_3O_4(110) surface with defective site is easily formed. The whole mechanism of H_2 dissociation and stepwise hydrogenation of ethylene to ethane is examined, and the most favorable pathway is heterolytic dissociation of H_2 follows two stepwise hydrogenation of ethylene process. The results show that ethyl hydrogenation to ethane on perfect Co_3O_4(110) surface is the rate limiting step with an activation energy of 1.19 eV, and the presence of oxygen vacancy strongly reduces the activation energies of main elementary steps, and the activation energy of rate limiting step is only 0.47 eV. Compared with that on Co_3O_4(111), ethylene hydrogenation is preferred on Co_3O_4(110) surface. Therefore, Co_3O_4 with exposed (110) facet is predicted as an excellent catalyst for ethylene hydrogenation.

Lattice gauge theories

International Nuclear Information System (INIS)

Creutz, M.

1983-04-01

In the last few years lattice gauge theory has become the primary tool for the study of nonperturbative phenomena in gauge theories. The lattice serves as an ultraviolet cutoff, rendering the theory well defined and amenable to numerical and analytical work. Of course, as with any cutoff, at the end of a calculation one must consider the limit of vanishing lattice spacing in order to draw conclusions on the physical continuum limit theory. The lattice has the advantage over other regulators that it is not tied to the Feynman expansion. This opens the possibility of other approximation schemes than conventional perturbation theory. Thus Wilson used a high temperature expansion to demonstrate confinement in the strong coupling limit. Monte Carlo simulations have dominated the research in lattice gauge theory for the last four years, giving first principle calculations of nonperturbative parameters characterizing the continuum limit. Some of the recent results with lattice calculations are reviewed

Evidence for strong electron-lattice coupling in La2-xSrxNiO4

International Nuclear Information System (INIS)

McQueeney, R.J.; Sarrao, J.L.

1999-01-01

The inelastic neutron scattering spectra were measured for several Sr concentrations of polycrystalline La 2-x Sr x NiO 4 . The authors find that the generalized phonon density-of-states is identical for x = 0 and x = 1/8. For x = 1/3 and x = 1/2, the band of phonons corresponding to the in-plane oxygen vibrations (> 65 meV) splits into two subbands centered at 75 meV and 85 meV. The lower frequency band increases in amplitude for the x = 1/2 sample, indicating that it is directly related to the hole concentration. These changes are associated with the coupling of oxygen vibrations to doped holes which reside in the NiO 2 planes and are a signature of strong electron-lattice coupling. Comparison of La 1.9 Sr 0.1 CuO 4 and La 1.875 Sr 0.125 NiO 4 demonstrates that much stronger electron-lattice coupling occurs for particular modes in the cuprate for modest doping and is likely related to the metallic nature of the cuprate

Initial oxidation behavior of Ni{sub 3}Al (210) surface induced by supersonic oxygen molecular beam at room temperature

Energy Technology Data Exchange (ETDEWEB)

Xu, Ya, E-mail: XU.Ya@nims.go.jp [Hydrogen Materials Unit, National Institute for Materials Science, 1-2-1 Sengen, Tsukuba, Ibaraki 305-0047 (Japan); Sakurai, Junya [Hydrogen Materials Unit, National Institute for Materials Science, 1-2-1 Sengen, Tsukuba, Ibaraki 305-0047 (Japan); Teraoka, Yuden; Yoshigoe, Akitaka [Quantum Beam Science Center, Japan Atomic Energy Research Agency, 1-1-1 Kouto, Sayo-cho, Hyogo 679-5148 (Japan); Demura, Masahiko; Hirano, Toshiyuki [Hydrogen Materials Unit, National Institute for Materials Science, 1-2-1 Sengen, Tsukuba, Ibaraki 305-0047 (Japan)

2017-01-01

Graphical abstract: - Highlights: • Initial oxidation of Ni{sub 3}Al (210) induced by O{sub 2} beam was investigated. • This was done using real-time synchrotron radiation XPS. • Both the Al and the Ni atoms on the surface were oxidized. • Oxidation of Al progressed much faster than that of Ni. - Abstract: The initial oxidation behavior of a clean Ni{sub 3}Al (210) surface was studied at 300 K using a supersonic O{sub 2} molecular beam (O{sub 2} SSMB) having an O{sub 2} translational energy of 2.3 eV, and real-time photoemission spectroscopy performed with high-brilliance synchrotron radiation. The evolution behaviors of the O 1s, Ni 2p, Al 2p, and Ni 3p spectra were examined during irradiation with the O{sub 2} SSMB. The spectral analysis revealed that both the Al atoms and the Ni atoms on the surface were oxidized; however, the oxidation of Al progressed much faster than that of Ni. The oxidation of Al began to occur and AlO{sub x} was formed at an oxygen coverage of 0.26 monolayer (ML) (1 ML was defined as the atomic density of the Ni{sub 3}Al (210) surface) and saturated at an oxygen coverage of 2.5 ML. In contrast, the oxidation of Ni commenced a little late at an oxygen coverage of 1.6 ML and slowly progressed to saturation, which occurred at an oxygen coverage of 4.89 ML.

Multiple surface plasmon polaritons modes on thin silver film controlled by a two-dimensional lattice of silver nanodimers

Energy Technology Data Exchange (ETDEWEB)

Chang, Ying; Jiang, Yongyuan, E-mail: jiangyy@hit.edu.cn [Harbin Institute of Technology, Department of Physics (China)

2015-01-15

We study the optical resonant spectrum of a two-dimensional periodic array of silver nanodimers on a thin silver film using multiple scattering formalism. The excited multiple plasmonic modes on two interfaces of the silver film reveal that the dispersion relationships of surface plasmon polaritons on metallic film are modified by doubly periodic lattice due to the fact that wave vectors matching conditions are satisfied. Moreover, we demonstrate that the plasmonic modes are directly controlled by the thickness of silver film, as well as the gap between nanodimer array and silver film. These effects provide novel high-efficient and steady way for excitation in future plasmonic nanodevices.

Convection-diffusion lattice Boltzmann scheme for irregular lattices

NARCIS (Netherlands)

Sman, van der R.G.M.; Ernst, M.H.

2000-01-01

In this paper, a lattice Boltzmann (LB) scheme for convection diffusion on irregular lattices is presented, which is free of any interpolation or coarse graining step. The scheme is derived using the axioma that the velocity moments of the equilibrium distribution equal those of the

Oxygen Evolution at Manganite Perovskite Ruddlesden-Popper Type Particles: Trends of Activity on Structure, Valence and Covalence

Directory of Open Access Journals (Sweden)

Majid Ebrahimizadeh Abrishami

2016-11-01

Full Text Available An improved understanding of the correlation between the electronic properties of Mn-O bonds, activity and stability of electro-catalysts for the oxygen evolution reaction (OER is of great importance for an improved catalyst design. Here, an in-depth study of the relation between lattice structure, electronic properties and catalyst performance of the perovskite Ca1−xPrxMnO3 and the first-order RP-system Ca2−xPrxMnO4 at doping levels of x = 0, 0.25 and 0.5 is presented. Lattice structure is determined by X-ray powder diffraction and Rietveld refinement. X-ray absorption spectroscopy of Mn-L and O-K edges gives access to Mn valence and covalency of the Mn-O bond. Oxygen evolution activity and stability is measured by rotating ring disc electrode studies. We demonstrate that the highest activity and stability coincidences for systems with a Mn-valence state of +3.7, though also requiring that the covalency of the Mn-O bond has a relative minimum. This observation points to an oxygen evolution mechanism with high redox activity of Mn. Covalency should be large enough for facile electron transfer from adsorbed oxygen species to the MnO6 network; however, it should not be hampered by oxidation of the lattice oxygen, which might cause a crossover to material degradation. Since valence and covalency changes are not entirely independent, the introduction of the energy position of the eg↑ pre-edge peak in the O-K spectra as a new descriptor for oxygen evolution is suggested, leading to a volcano-like representation of the OER activity.

Contact angle determination in multicomponent lattice Boltzmann simultations

NARCIS (Netherlands)

Schmieschek, S.M.P.; Harting, J.D.R.

2011-01-01

Droplets on hydrophobic surfaces are ubiquitous in microfluidic applications and there exists a number of commonly used multicomponent and multiphase lattice Boltzmann schemes to study such systems. In this paper we focus on a popular implementation of a multicomponent model as introduced by Shan

Doping Li-rich cathode material Li2MnO3 : Interplay between lattice site preference, electronic structure, and delithiation mechanism

Science.gov (United States)

Hoang, Khang

2017-12-01

We report a detailed first-principles study of doping in Li2MnO3 , in both the dilute doping limit and heavy doping, using hybrid density-functional calculations. We find that Al, Fe, Mo, and Ru impurities are energetically most favorable when incorporated into Li2MnO3 at the Mn site, whereas Mg is most favorable when doped at the Li sites. Nickel, on the other hand, can be incorporated at the Li site and/or the Mn site, and the distribution of Ni over the lattice sites can be tuned by tuning the material preparation conditions. There is a strong interplay among the lattice site preference and charge and spin states of the dopant, the electronic structure of the doped material, and the delithiation mechanism. The calculated electronic structure and voltage profile indicate that in Ni-, Mo-, or Ru-doped Li2MnO3 , oxidation occurs on the electrochemically active transition-metal ion(s) before it does on oxygen during the delithiation process. The role of the dopants is to provide charge compensation and bulk electronic conduction mechanisms in the initial stages of delithiation, hence enabling the oxidation of the lattice oxygen in the later stages. This work thus illustrates how the oxygen-oxidation mechanism can be used in combination with the conventional mechanism involving transition-metal cations in design of high-capacity battery cathode materials.

Numerical simulation of vapor film collapse behavior on high-temperature droplet surface with three-dimensional lattice gas cellular automata

International Nuclear Information System (INIS)

Tochio, Daisuke; Abe, Yutaka; Matsukuma, Yosuke

2008-01-01

It is pointed out that a vapor film on a premixed high-temperature droplet surface is needed to be collapsed to trigger vapor explosion. Thus, it is important to clarify the micromechanism of vapor film collapse behavior for the occurrence of vapor explosion. In a previous study, it is suggested experimentally that vapor film collapse behavior is dominated by phase change phenomena rather than by the surrounding fluid motion. In the present study, vapor film collapse behavior is investigated to clarify the dominant factor of vapor film collapse behavior with lattice gas automata of three-dimensional immiscible lattice gas model (3-D ILG model). First, in order to represent the boiling and phase change phenomena, the thermal model of a heat wall model and a phase change model is newly constructed. Next, the numerical simulation of vapor film collapse behavior is performed with and without the phase change effect. As a result, the computational result with the phase change effect is observed to be almost same as the experimental result. It can be considered that vapor film collapse behavior is dominated by phase change phenomena. (author)

Lattices with unique complements

CERN Document Server

Saliĭ, V N

1988-01-01

The class of uniquely complemented lattices properly contains all Boolean lattices. However, no explicit example of a non-Boolean lattice of this class has been found. In addition, the question of whether this class contains any complete non-Boolean lattices remains unanswered. This book focuses on these classical problems of lattice theory and the various attempts to solve them. Requiring no specialized knowledge, the book is directed at researchers and students interested in general algebra and mathematical logic.

Ni-Doping Effects on Oxygen Removal from an Orthorhombic Mo ₂ C (001) Surface: A Density Functional Theory Study

Energy Technology Data Exchange (ETDEWEB)

Zhou, Mingxia [Department; Cheng, Lei [Materials; Choi, Jae-Soon [Oak Ridge National Laboratory, 1 Bethel Valley Road, Oak Ridge, TN 37831, Unites States; Liu, Bin [Department; Curtiss, Larry A. [Materials; Assary, Rajeev S. [Materials

2018-01-11

Density functional theory (DFT) calculations were used to investigate the effect of Ni dopants on the removal of chemisorbed oxygen (O*) from the Mo-terminated (T-Mo) and C-terminated (Tc) Mo2C(001) surfaces. The removal of adsorbed oxygen from the catalytic site is essential to maintain the long-term activity and selectivity of the carbide catalysts in the deoxygenation process related to bio-oil stabilization and upgrading. In this contribution, the computed reaction energetics and reaction barriers of O* removal were compared among undoped and Ni-doped Mo2C(001) surfaces. The DFT calculations indicate that selected Ni-doped surfaces such as Ni adsorbed on T-Mo and Tc Mo2C(001) surfaces enable weaker binding of important reactive intermediates (O*, OH*) compared to the undoped counterparts, which is beneficial for the O* removal from the catalyst surface. This study thus confirms the promoting effect of the Ni dopant on O* removal reaction on the T-Mo Mo2C(001) and Tc Mo2C(001) surfaces. This computational prediction has been confirmed by the temperature-programmed reduction profiles of Mo2C and Ni-doped Mo2C catalysts, which had been passivated and stored in an oxygen environment.

Direct observation of the lattice precursor of the metal-to-insulator transition in V2O3 thin films by surface acoustic waves

Science.gov (United States)

Kündel, J.; Pontiller, P.; Müller, C.; Obermeier, G.; Liu, Z.; Nateprov, A. A.; Hörner, A.; Wixforth, A.; Horn, S.; Tidecks, R.

2013-03-01

A surface acoustic wave (SAW) delay line is used to study the metal-to-insulator (MI) transition of V2O3 thin films deposited on a piezoelectric LiNbO3 substrate. Effects contributing to the sound velocity shift of the SAW which are caused by elastic properties of the lattice of the V2O3 films when changing the temperature are separated from those originating from the electrical conductivity. For this purpose the electric field accompanying the elastic wave of the SAW has been shielded by growing the V2O3 film on a thin metallic Cr interlayer (coated with Cr2O3), covering the piezoelectric substrate. Thus, the recently discovered lattice precursor of the MI transition can be directly observed in the experiments, and its fine structure can be investigated.

The Lattice-Valued Turing Machines and the Lattice-Valued Type 0 Grammars

Directory of Open Access Journals (Sweden)

Juan Tang

2014-01-01

Full Text Available Purpose. The purpose of this paper is to study a class of the natural languages called the lattice-valued phrase structure languages, which can be generated by the lattice-valued type 0 grammars and recognized by the lattice-valued Turing machines. Design/Methodology/Approach. From the characteristic of natural language, this paper puts forward a new concept of the l-valued Turing machine. It can be used to characterize recognition, natural language processing, and dynamic characteristics. Findings. The mechanisms of both the generation of grammars for the lattice-valued type 0 grammar and the dynamic transformation of the lattice-valued Turing machines were given. Originality/Value. This paper gives a new approach to study a class of natural languages by using lattice-valued logic theory.

Lattice Boltzmann model for free-surface flow and its application to filling process in casting

CERN Document Server

Ginzburg, I

2003-01-01

A generalized lattice Boltzmann model to simulate free-surface is constructed in both two and three dimensions. The proposed model satisfies the interfacial boundary conditions accurately. A distinctive feature of the model is that the collision processes is carried out only on the points occupied partially or fully by the fluid. To maintain a sharp interfacial front, the method includes an anti-diffusion algorithm. The unknown distribution functions at the interfacial region are constructed according to the first-order Chapman-Enskog analysis. The interfacial boundary conditions are satisfied exactly by the coefficients in the Chapman-Enskog expansion. The distribution functions are naturally expressed in the local interfacial coordinates. The macroscopic quantities at the interface are extracted from the least-square solutions of a locally linearized system obtained from the known distribution functions. The proposed method does not require any geometric front construction and is robust for any interfacial ...

Nitrogen diffusion in hafnia and the impact of nitridation on oxygen and hydrogen diffusion: A first-principles study

Energy Technology Data Exchange (ETDEWEB)

Sathiyanarayanan, Rajesh, E-mail: rajessat@in.ibm.com, E-mail: rajesh.sathiyanarayanan@gmail.com; Pandey, R. K.; Murali, K. V. R. M. [IBM Semiconductor Research and Development Center, Bangalore 560045 (India)

2015-01-21

Using first-principles simulations, we have computed incorporation energies and diffusion barriers of ammonia, the nitrogen molecule and atomic nitrogen in monoclinic hafnia (m-HfO{sub 2}). Our calculations show that ammonia is likely to dissociate into an NH{sub 2} molecular unit, whereas the nitrogen molecule remains as a molecule either in the interstitial space or at an oxygen lattice site. The lowest energy pathway for the diffusion of atomic nitrogen interstitials consists of the hopping of the nitrogen interstitial between neighboring three-coordinated lattice oxygen atoms that share a single Hf atom, and the barrier for such hops is determined by a switching mechanism. The substitutional nitrogen atom shows a preference for diffusion through the doubly positive oxygen vacancy-mediated mechanism. Furthermore, we have investigated the impact of nitrogen atoms on the diffusion barriers of oxygen and hydrogen interstitials in m-HfO{sub 2}. Our results show that nitrogen incorporation has a significant impact on the barriers for oxygen and hydrogen diffusion: nitrogen atoms attract oxygen and hydrogen interstitials diffusing in the vicinity, thereby slowing down (reducing) their diffusion (diffusion length)

The adsorption of NO on an oxygen pre-covered Pt(1 1 1) surface: in situ high-resolution XPS combined with molecular beam studies

Science.gov (United States)

Zhu, J. F.; Kinne, M.; Fuhrmann, T.; Tränkenschuh, B.; Denecke, R.; Steinrück, H.-P.

2003-12-01

Adsorption of NO on a Pt(1 1 1) surface pre-covered with a p(2 × 2) atomic oxygen layer has been studied in situ by high-resolution X-ray photoelectron spectroscopy and temperature-programmed XPS using third-generation synchrotron radiation at BESSY II, Berlin, combined with molecular beam techniques and ex situ by low energy electron diffraction and temperature-programmed desorption. O 1s XP spectra reveal that an ordered p(2 × 2)-O layer dramatically changes the adsorption behavior of NO as compared to the clean surface. The atomic oxygen occupies fcc hollow sites, and therefore blocks NO adsorption on these sites, which are energetically preferred on clean Pt(1 1 1). As a consequence, NO populates on-top sites at low coverage. At 110 K for higher coverages, NO can additionally adsorb on hcp hollow sites, thereby inducing a shift of the O 1s binding energy of atomic oxygen towards lower energies by about 0.25 eV. The bond strength of the hcp hollow NO species to the substrate is weakened by the presence of atomic oxygen. A sharp p(2 × 2) LEED pattern is observed for NO adsorption on the oxygen pre-covered surface, up to saturation coverage. The total saturation coverage of NO on Pt(1 1 1) pre-covered with varying amounts of oxygen (below 0.25 ML) decreases linearly with the coverage of oxygen. The initial sticking coefficient of NO is reduced from 0.96 on clean Pt(1 1 1) to 0.88 on a p(2 × 2) oxygen pre-covered surface.

Additive lattice kirigami.

Science.gov (United States)

Castle, Toen; Sussman, Daniel M; Tanis, Michael; Kamien, Randall D

2016-09-01

Kirigami uses bending, folding, cutting, and pasting to create complex three-dimensional (3D) structures from a flat sheet. In the case of lattice kirigami, this cutting and rejoining introduces defects into an underlying 2D lattice in the form of points of nonzero Gaussian curvature. A set of simple rules was previously used to generate a wide variety of stepped structures; we now pare back these rules to their minimum. This allows us to describe a set of techniques that unify a wide variety of cut-and-paste actions under the rubric of lattice kirigami, including adding new material and rejoining material across arbitrary cuts in the sheet. We also explore the use of more complex lattices and the different structures that consequently arise. Regardless of the choice of lattice, creating complex structures may require multiple overlapping kirigami cuts, where subsequent cuts are not performed on a locally flat lattice. Our additive kirigami method describes such cuts, providing a simple methodology and a set of techniques to build a huge variety of complex 3D shapes.

Surface and local electronic structure modification of MgO film using Zn and Fe ion implantation

Science.gov (United States)

Singh, Jitendra Pal; Lim, Weon Cheol; Lee, Jihye; Song, Jonghan; Lee, Ik-Jae; Chae, Keun Hwa

2018-02-01

Present work is motivated to investigate the surface and local electronic structure modifications of MgO films implanted with Zn and Fe ions. MgO film was deposited using radio frequency sputtering method. Atomic force microscopy measurements exhibit morphological changes associated with implantation. Implantation of Fe and Zn ions leads to the reduction of co-ordination geometry of Mg2+ ions in host lattice. The effect is dominant at bulk of film rather than surface as the large concentration of implanted ions resides inside bulk. Moreover, the evidences of interaction among implanted ions and oxygen are not being observed using near edge fine structure measurements.

Lattice Boltzmann study of slip flow over structured surface with transverse slots

Science.gov (United States)

Chen, Wei; Wang, Kai; Wang, Lei; Hou, Guoxiang; Leng, Wenjun

2018-04-01

Slip flow over structured superhydrophobic surface with transverse slots is investigated by the lattice Boltzmann method. The Shan-Chen multiphase model is employed to simulate the flow over gas bubbles in the slots. The Carnahan-Starling equation of state is applied to obtain large density ratio. The interface thickness of the multiphase model is discussed. We find that the Cahn number Cn should be smaller than 0.02 when the temperature T = 0.5T c to restrict the influence of interface thickness on slip length. Influences of slot fraction on slip length is then studied, and the result is compared with single LB simulation of which the interface is treated as free-slip boundary. The slip length obtained by the multiphase model is a little smaller. After that, the shape of the liquid-gas interface is considered, and simulations with different initial protrusion angles and capillary numbers are performed. Effective slip length as a function of initial protrusion angle is obtained. The result is in qualitative agreement with a previous study and main features are reproduced. Furthermore, the influence of Capillary number Ca is studied. Larger Ca causes larger interface deformation and smaller slip length. But when the interface is concaving into the slot, this influence is less obvious.

Thermal and non-thermal lattice gas models for a dimer-trimer surface catalytic reaction: a Monte-Carlo simulation study

International Nuclear Information System (INIS)

Iqbal, K.; Khand, P.A.

2012-01-01

The kinetics of an irreversible dimer-trimer reaction of the type 2 A/sub 3/ +3 B/sub 2/ -- 6 AB by considering the precursor motion of the dimer (B/sub 2) on a square, as well as on a hexagonal surface, by using a Monte Carlo simulation have been studied. When the movement of precursors is limited to the first nearest neighborhood, the model gives reactive window widths of the order of 0.22 and 0.29 for the square and the hexagonal lattices, respectively, which are quite large compared to those predicted by the LH model. In our model, the reactive window width for a square lattice increases significantly as compared to that for the LH models of the same system on square and hexagonal lattices. The width of the reactive region increases when the precursor motion is extended to the second and the third nearest neighborhood. The continuous transition disappears when the precursor motion is extended to the third nearest neighborhood. The diffusion of B atoms does not change the situation qualitatively for both the precursor and the LH models. However, desorption of the dimer changes the situation significantly; i.e., the width of the reactive window shows an exponential growth with respect to the desorption probability of the dimer for both the precursor and the LH models. In our opinion, the inclusion of precursors in the LH model of the dimer-trimer reactions leads to a better and more realistic description of the heterogeneous catalytic reactions. Consequently, further numerical and theoretical activity in this field will be very useful for understanding complex heterogeneous reactions. (orig./A.B.)

Fabrication of high surface area graphene electrodes with high performance towards enzymatic oxygen reduction

International Nuclear Information System (INIS)

Di Bari, Chiara; Goñi-Urtiaga, Asier; Pita, Marcos; Shleev, Sergey; Toscano, Miguel D.; Sainz, Raquel; De Lacey, Antonio L.

2016-01-01

High surface area graphene electrodes were prepared by simultaneous electrodeposition and electroreduction of graphene oxide. The electrodeposition process was optimized in terms of pH and conductivity of the solution and the obtained graphene electrodes were characterized by X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, scanning electron microscopy and electrochemical methods (cyclic voltammetry and impedance spectroscopy). Electrodeposited electrodes were further functionalized to carry out covalent immobilization of two oxygen-reducing multicopper oxidases: laccase and bilirubin oxidase. The enzymatic electrodes were tested as direct electron transfer based biocathodes and catalytic currents as high as 1 mA/cm 2 were obtained. Finally, the mechanism of the enzymatic oxygen reduction reaction was studied for both enzymes calculating the Tafel slopes and transfer coefficients.

Return polynomials for non-intersecting paths above a surface on the directed square lattice

Energy Technology Data Exchange (ETDEWEB)

Brak, R. [Deartment of Mathematics, University of Melbourne, Parkville, VIC (Australia)]. E-mail: r.brak@ms.unimelb.edu.au; Essam, J.W. [Department of Mathematics, Royal Holloway College, University of London, Egham, Surrey (United Kingdom)]. E-mail: j.essam@alpha1.rhul.ac.uk

2001-12-14

We enumerate sets of n non-intersecting, t-step paths on the directed square lattice which are excluded from the region below the surface y=0 to which they are initially attached. In particular we obtain a product formula for the number of star configurations in which the paths have arbitrary fixed endpoints. We also consider the 'return' polynomial, R-'{sup W}{sub t}(y;k)={sigma}{sub m{>=}}{sub 0}r-'{sup W}{sub t}(y;m)k{sup m} where r-'{sup W}{sub t}(y;m) is the number of n-path configurations of watermelon type having deviation {gamma} for which the path closest to the surface returns to the surface m times. The 'marked return' polynomial is defined by u-'{sup W}{sub t}(y;k{sub 1}){identical_to}R-'{sup W}{sub 1}(y;k{sub 1}+l)={sigma}{sub m{>=}}{sub 0}u-'{sup W}{sub t}(y;m)k{sub 1}{sup m} where u-'{sup W}{sub t}(y;m) is the number of marked configurations having at least m returns, just m of which are marked. Both r-'{sup W}{sub t}(y;m) and u-'{sup W}(y;m) are expressed in terms of the numbers of paths ignoring returns but introducing a suitably modified endpoint condition. This enables u-'{sup W}{sub t}(y;m) to be written in product form for arbitrary y, but for r-'{sup W}{sub t}(y;m) this can only be done in the case y=0. (author)

Entanglement scaling in lattice systems

Energy Technology Data Exchange (ETDEWEB)

Audenaert, K M R [Institute for Mathematical Sciences, Imperial College London, 53 Prince' s Gate, Exhibition Road, London SW7 2PG (United Kingdom); Cramer, M [QOLS, Blackett Laboratory, Imperial College London, Prince Consort Road, London SW7 2BW (United Kingdom); Eisert, J [Institute for Mathematical Sciences, Imperial College London, 53 Prince' s Gate, Exhibition Road, London SW7 2PG (United Kingdom); Plenio, M B [Institute for Mathematical Sciences, Imperial College London, 53 Prince' s Gate, Exhibition Road, London SW7 2PG (United Kingdom)

2007-05-15

We review some recent rigorous results on scaling laws of entanglement properties in quantum many body systems. More specifically, we study the entanglement of a region with its surrounding and determine its scaling behaviour with its size for systems in the ground and thermal states of bosonic and fermionic lattice systems. A theorem connecting entanglement between a region and the rest of the lattice with the surface area of the boundary between the two regions is presented for non-critical systems in arbitrary spatial dimensions. The entanglement scaling in the field limit exhibits a peculiar difference between fermionic and bosonic systems. In one-spatial dimension a logarithmic divergence is recovered for both bosonic and fermionic systems. In two spatial dimensions in the setting of half-spaces however we observe strict area scaling for bosonic systems and a multiplicative logarithmic correction to such an area scaling in fermionic systems. Similar questions may be posed and answered in classical systems.

Free-energy analysis of spin models on hyperbolic lattice geometries.

Science.gov (United States)

Serina, Marcel; Genzor, Jozef; Lee, Yoju; Gendiar, Andrej

2016-04-01

We investigate relations between spatial properties of the free energy and the radius of Gaussian curvature of the underlying curved lattice geometries. For this purpose we derive recurrence relations for the analysis of the free energy normalized per lattice site of various multistate spin models in the thermal equilibrium on distinct non-Euclidean surface lattices of the infinite sizes. Whereas the free energy is calculated numerically by means of the corner transfer matrix renormalization group algorithm, the radius of curvature has an analytic expression. Two tasks are considered in this work. First, we search for such a lattice geometry, which minimizes the free energy per site. We conjecture that the only Euclidean flat geometry results in the minimal free energy per site regardless of the spin model. Second, the relations among the free energy, the radius of curvature, and the phase transition temperatures are analyzed. We found out that both the free energy and the phase transition temperature inherit the structure of the lattice geometry and asymptotically approach the profile of the Gaussian radius of curvature. This achievement opens new perspectives in the AdS-CFT correspondence theories.

First principles density functional theory study of Pb doped α-MnO2 catalytic materials

Science.gov (United States)

Song, Zilin; Yan, Zhiguo; Yang, Xiaojun; Bai, Hang; Duan, Yuhua; Yang, Bin; Leng, Li

2018-03-01

The impact of Pb in the tunnels of manganese oxide octahedral molecular sieves on chemical state of Mn species and lattice oxygen were investigated utilizing density functional theory calculations. The results show that the Pb dopant in the tunnels of OMS-2 could reduce the average valence states of Mn. The lower energy required for bulk oxygen defects formation in Pb-OMS-2 validates the activation of lattice oxygen by inclusion of tunnel dopant. The inclusion of Pb promotes the catalytic oxidation activity of OMS-2 by reducing the energy required for the surface lattice oxygen migration during the Mars - van Krevelen oxidation process.

Porous boron doped diamonds as metal-free catalysts for the oxygen reduction reaction in alkaline solution

Science.gov (United States)

Suo, Ni; Huang, Hao; Wu, Aimin; Cao, Guozhong; Hou, Xiaoduo; Zhang, Guifeng

2018-05-01

Porous boron doped diamonds (BDDs) were obtained on foam nickel substrates with a porosity of 80%, 85%, 90% and 95% respectively by hot filament chemical vapor deposition (HFCVD) technology. Scanning electron microscopy (SEM) reveals that uniform and compact BDDs with a cauliflower-like morphology have covered the overall frame of the foam nickel substrates. Raman spectroscopy shows that the BDDs have a poor crystallinity due to heavily doping boron. X-ray photoelectron spectroscopy (XPS) analysis effectively demonstrates that boron atoms can be successfully incorporated into the crystal lattice of diamonds. Electrochemical measurements indicate that the oxygen reduction potential is unaffected by the specific surface area (SSA), and both the onset potential and the limiting diffusion current density are enhanced with increasing SSA. It is also found that the durability and methanol tolerance of the boron doped diamond catalysts are attenuated as the increasing of SSA. The SSA of the catalyst is directly proportional to the oxygen reduction activity and inversely to the durability and methanol resistance. These results provide a reference to the application of porous boron doped diamonds as potential cathodic catalysts for the oxygen reduction reaction in alkaline solution by adjusting the SSA.

Magnetism, Spin Texture, and In-Gap States: Atomic Specialization at the Surface of Oxygen-Deficient SrTiO_{3}.

Science.gov (United States)

Altmeyer, Michaela; Jeschke, Harald O; Hijano-Cubelos, Oliver; Martins, Cyril; Lechermann, Frank; Koepernik, Klaus; Santander-Syro, Andrés F; Rozenberg, Marcelo J; Valentí, Roser; Gabay, Marc

2016-04-15

Motivated by recent spin- and angular-resolved photoemission (SARPES) measurements of the two-dimensional electronic states confined near the (001) surface of oxygen-deficient SrTiO_{3}, we explore their spin structure by means of ab initio density functional theory (DFT) calculations of slabs. Relativistic nonmagnetic DFT calculations display Rashba-like spin winding with a splitting of a few meV and when surface magnetism on the Ti ions is included, bands become spin-split with an energy difference ∼100  meV at the Γ point, consistent with SARPES findings. While magnetism tends to suppress the effects of the relativistic Rashba interaction, signatures of it are still clearly visible in terms of complex spin textures. Furthermore, we observe an atomic specialization phenomenon, namely, two types of electronic contributions: one is from Ti atoms neighboring the oxygen vacancies that acquire rather large magnetic moments and mostly create in-gap states; another comes from the partly polarized t_{2g} itinerant electrons of Ti atoms lying further away from the oxygen vacancy, which form the two-dimensional electron system and are responsible for the Rashba spin winding and the spin splitting at the Fermi surface.

Finite-lattice-spacing corrections to masses and g factors on a lattice

International Nuclear Information System (INIS)

Roskies, R.; Wu, J.C.

1986-01-01

We suggest an alternative method for extracting masses and g factors from lattice calculations. Our method takes account of more of the infrared and ultraviolet lattice effects. It leads to more reasonable results in simulations of QED on a lattice

Lattices for laymen: a non-specialist's introduction to lattice gauge theory

International Nuclear Information System (INIS)

Callaway, D.J.E.

1985-01-01

The review on lattice gauge theory is based upon a series of lectures given to the Materials Science and Technology Division at Argonne National Laboratory. Firstly the structure of gauge theories in the continuum is discussed. Then the lattice formulation of these theories is presented, including quantum electrodynamics and non-abelian lattice gauge theories. (U.K.)

Tracking Oxygen Vacancies in Thin Film SOFC Cathodes

Science.gov (United States)

Leonard, Donovan; Kumar, Amit; Jesse, Stephen; Kalinin, Sergei; Shao-Horn, Yang; Crumlin, Ethan; Mutoro, Eva; Biegalski, Michael; Christen, Hans; Pennycook, Stephen; Borisevich, Albina

2011-03-01

Oxygen vacancies have been proposed to control the rate of the oxygen reduction reaction and ionic transport in complex oxides used as solid oxide fuel cell (SOFC) cathodes [1,2]. In this study oxygen vacancies were tracked, both dynamically and statically, with the combined use of scanned probe microscopy (SPM) and scanning transmission electron microscopy (STEM). Epitaxial films of La 0.8 Sr 0.2 Co O3 (L SC113) and L SC113 / LaSrCo O4 (L SC214) on a GDC/YSZ substrate were studied, where the latter showed increased electrocatalytic activity at moderate temperature. At atomic resolution, high angle annular dark field STEM micrographs revealed vacancy ordering in L SC113 as evidenced by lattice parameter modulation and EELS studies. The evolution of oxygen vacancy concentration and ordering with applied bias and the effects of bias cycling on the SOFC cathode performance will be discussed. Research is sponsored by the of Materials Sciences and Engineering Division, U.S. DOE.

A quantum-chemical study of oxygen-vacancy defects in PbTiO{sub 3} crystals

Energy Technology Data Exchange (ETDEWEB)

Stashans, Arvids [Laboratorio de Fisica, Escuela de Electronica y Telecomunicaciones, Universidad Tecnica Particular de Loja, Apartado 11-01-608, Loja (Ecuador)]. E-mail: arvids@utpl.edu.ec; Serrano, Sheyla [Centro de Investigacion en Fisica de Materia Condensada, Corporacion de Fisica Fundamental y Aplicada, Apartado 17-12-637, Quito (Ecuador); Escuela de Ingenierias, Universidad Politecnica Salesiana, Campus Sur, Rumichaca s/n y Moran Valverde, Apartado 17-12-536, Quito (Ecuador); Medina, Paul [Centro de Investigacion en Fisica de Materia Condensada, Corporacion de Fisica Fundamental y Aplicada, Apartado 17-12-637, Quito (Ecuador)

2006-05-31

Investigation of an oxygen vacancy and F center in the cubic and tetragonal lattices of PbTiO{sub 3} crystals is done by means of quantum-chemical simulations. Displacements of defect-surrounding atoms, electronic and optical properties, lattice relaxation energies and some new effects due to the defects presence are reported and analyzed. A comparison with similar studies is made and conclusions are drawn on the basis of the obtained results.

A Lattice Boltzmann Approach to Multi-Phase Surface Reactions with Heat Effects

NARCIS (Netherlands)

Kamali, M.R.

2013-01-01

The aim of the present research was to explore the promises and shift the limits of the numerical framework of lattice Boltzmann (LB) for studying the physics behind multi-component two-phase heterogeneous non-isothermal reactive flows under industrial conditions. An example of such an industrially

Universality in Oxygen Reduction Electrocatalysis on Metal Surfaces

DEFF Research Database (Denmark)

Viswanathan, Venkatasubramanian; Hansen, Heine Anton; Rossmeisl, Jan

2012-01-01

In this work, we extend the activity volcano for oxygen reduction from the face-centered cubic (fcc) metal (111) facet to the (100) facet. Using density functional theory calculations, we show that the recent findings of constant scaling between OOH* and OH* holds on the fcc metal (100) facet......, as well. Using this fact, we show the existence of a universal activity volcano to describe oxygen reduction electrocatalysis with a minimum overpotential, ηmin = 0.37 ± 0.1 V. Specifically, we find that the (100) facet of Pt is found to bind oxygen intermediates too strongly and is not active for oxygen...... reduction reaction (ORR). In contrast, Au(100) is predicted to be more active than Au(111) and comparable in activity to Pt alloys. Using this activity volcano, we further predict that Au alloys that bind OH more strongly could display improved ORR activity on the (100) facet. We carry out a computational...

Lattice QCD on fine lattices

Energy Technology Data Exchange (ETDEWEB)

Schaefer, Stefan [DESY (Germany). Neumann Inst. for Computing

2016-11-01

These configurations are currently in use in many on-going projects carried out by researchers throughout Europe. In particular this data will serve as an essential input into the computation of the coupling constant of QCD, where some of the simulations are still on-going. But also projects computing the masses of hadrons and investigating their structure are underway as well as activities in the physics of heavy quarks. As this initial project of gauge field generation has been successful, it is worthwhile to extend the currently available ensembles with further points in parameter space. These will allow to further study and control systematic effects like the ones introduced by the finite volume, the non-physical quark masses and the finite lattice spacing. In particular certain compromises have still been made in the region where pion masses and lattice spacing are both small. This is because physical pion masses require larger lattices to keep the effects of the finite volume under control. At light pion masses, a precise control of the continuum extrapolation is therefore difficult, but certainly a main goal of future simulations. To reach this goal, algorithmic developments as well as faster hardware will be needed.

In vitro study of 3D PLGA/n-HAp/β-TCP composite scaffolds with etched oxygen plasma surface modification in bone tissue engineering

Energy Technology Data Exchange (ETDEWEB)

Roh, Hee-Sang [Department of Dental Materials, School of Dentistry, Chosun University, 309 Pilmun-daero, Dong-gu, Gwangju 61452 (Korea, Republic of); Jung, Sang-Chul [Department of Environmental Engineering, Sunchon National University, 255 Jungang-ro, Sunchon 57922 (Korea, Republic of); Kook, Min-Suk [Department of Oral and Maxillofacial Surgery, School of Dentistry, Chonnam National University, 77 Yongbong-ro, Buk-gu, Gwangju 61186 (Korea, Republic of); Kim, Byung-Hoon, E-mail: kim5055@chosun.ac.kr [Department of Dental Materials, School of Dentistry, Chosun University, 309 Pilmun-daero, Dong-gu, Gwangju 61452 (Korea, Republic of)

2016-12-01

Highlights: • PLGA and PLGA/n-HAp/β-TCP scaffolds were successfully fabricated by 3D printing. • Oxygen plasma etching increases the wettability and surface roughness. • Bioceramics and oxygen plasma etching and could be used to improve the cell affinity. - Abstract: Three-dimensional (3D) scaffolds have many advantageous properties for bone tissue engineering application, due to its controllable properties such as pore size, structural shape and interconnectivity. In this study, effects on oxygen plasma surface modification and adding of nano-hydroxyapatite (n-HAp) and β-tricalcium phosphate (β-TCP) on the 3D PLGA/n-HAp/β-TCP scaffolds for improving preosteoblast cell (MC3T3-E1) adhesion, proliferation and differentiation were investigated. The 3D PLGA/n-HAp/β-TCP scaffolds were fabricated by 3D Bio-Extruder equipment. The 3D scaffolds were prepared with 0°/90° architecture and pore size of approximately 300 μm. In addition 3D scaffolds surface were etched by oxygen plasma to enhance the hydrophilic property and surface roughness. After oxygen plasma treatment, the surface chemistry and morphology were investigated by Fourier transform infrared spectroscopy, scanning electron microscopy, and atomic force microscopy. And also hydrophilic property was measured by contact angle. The MC3T3-E1 cell proliferation and differentiation were investigated by MTT assay and ALP activity. In present work, the 3D PLGA/HAp/beta-TCP composite scaffold with suitable structure for the growth of osteoblast cells was successfully fabricated by 3D rapid prototyping technique. The surface hydrophilicity and roughness of 3D scaffold increased by oxygen plasma treatment had a positive effect on cell adhesion, proliferation, and differentiation. Furthermore, the differentiation of MC3T3-E1 cell was significantly enhanced by adding of n-HAp and β-TCP on 3D PLGA scaffold. As a result, combination of bioceramics and oxygen plasma treatment showed a synergistic effect on

Nonlinear localized modes in dipolar Bose-Einstein condensates in optical lattices

International Nuclear Information System (INIS)

Rojas-Rojas, S.; Vicencio, R. A.; Molina, M. I.; Abdullaev, F. Kh.

2011-01-01

Modulational instability and discrete matter wave solitons in dipolar BECs, loaded into a deep optical lattice, are investigated analytically and numerically. The process of modulational instability of nonlinear plane matter waves in a dipolar nonlinear lattice is studied and the regions of instability are established. The existence and stability of bulk discrete solitons are analyzed analytically and confirmed by numerical simulations. In marked contrast with the usual discrete nonlinear Schroedinger behavior (no dipolar interactions), we found a region where the two fundamental modes are simultaneously unstable, allowing enhanced mobility across the lattice for large norm values. To study the existence and properties of surface discrete solitons, an analysis of the dimer configuration is performed. The properties of symmetric and antisymmetric modes including stability diagrams and bifurcations are investigated in closed form. For the case of a bulk medium, properties of fundamental on-site and intersite localized modes are analyzed. On-site and intersite surface localized modes are studied, and we find that they do not exist when nonlocal interactions predominate with respect to local ones.

Shape of the nuclear magnetic resonance line in anisotropic superconductors with an irregular vortex lattice

International Nuclear Information System (INIS)

Minkin, A.V.; Tsarevskij, S.L.

2006-01-01

For high-temperature superconductors the shape of a NMR spectrum line is built regarding for variation of inhomogeneity of irregular vortex lattice magnetic field near superconductor surface. It is shown that the shape of a NMR line is not simply widened but noticeably varies depending on the degree of irregularity of a superconductor vortex lattice. This variation is associated with a local symmetry decrease in an irregular vortex lattice of the superconductor. Taking into account these circumstances may considerably change conclusions about the type of a vortex lattice and superconductor parameters which are commonly gained from NMR line shape analysis [ru

Investigation of the niobium-oxygen system under low pressure and between 550 K and 2350 K: solid solution, surface overlay and reactivity

International Nuclear Information System (INIS)

Jupille, Jacques

1974-09-01

This research thesis addresses the behaviour of transition metals when interacting with oxygen, more particularly in the case of phase formation, but also adsorption and desorption which occur in the case of interaction with low pressure oxygen. It focuses on the case of niobium in solid solution. After a description of phases present in the niobium-oxygen system, and a discussion of reactivities of oxygen and water vapour, the author describes the experimental methods (apparatus and installations, samples, measured values), discusses the study of the surface-volume transfer constant of the niobium-oxygen solution, and the niobium-oxygen interaction mechanisms at high (superior to 1700 K) and low (inferior to 1000 K) temperatures: oxide desorption, oxygen reaction kinetics

Poly-epoxide lattices used for the coating of radioactive wastes: aging analysis in storage conditions and effects on the diffusional properties of materials

International Nuclear Information System (INIS)

Damian Pellissier, C.

1999-01-01

This work deals with the long term forecasting of the aging behaviour of epoxy-amine lattices used for the coating of radioactive wastes. In storage conditions, the oxygen of air, the radiations and the water are the three factors at the origin of the aging. The main goals have been to study the morphology changes during the aging and to model the oxidation phenomena. The transport properties allow to determine the oxygen diffusivities and solubilities. A wide range of poly-epoxide lattices has been studied, from the classical DGEBA/DDM classical lattice to the commercial coating matrix with contains both an important molar fraction of mono-epoxy and a plasticizer which lowers the vitreous transition temperature from 175 deg. C to 55 deg. C. The analysis of the diffusional parameters of these lattices shows that the solubility increases and the diffusivity decreases when the reticulation increases or when the lattice contains no plasticizer. The transport parameters necessary for the modeling laws have been determined for all lattices. The aging under thermo-activated air involves oxidation reactions which take place preferentially at the level of epoxy constituents and lead to the formation of carbonyl and amide polar oxygenated functions and to chain cleavage with the departure of phenol-type volatile products or higher mass compounds. Using a theoretical model, the hyperbolic-type oxide sites concentration profile has been precised and an important parameter, the thickness of the oxidized layer has been calculated. The radio-oxidation, performed in extreme conditions with respect to the real storage conditions, leads to the formation of polar functions without any significant degradation of lattices. The hygro-thermal aging is characterized, for the commercial matrix only, by the leaching possibility of various products initially present in the lattice and of hydrolysis products, and by the occurrence of osmotic pressure bags at the origin of cracks. This raises

XPS study of surface state of novel perovskite system Dy{sub 0.5}Sr{sub 0.5}Co{sub 0.8}Fe{sub 0.2}O{sub 3-δ} as cathode for solid oxide fuel cells

Energy Technology Data Exchange (ETDEWEB)

Kautkar, Pranay R.; Acharya, Smita A., E-mail: saha275@yahoo.com; Tumram, Priya V. [Depatment of Physics, Rashtrasant Tukadoji Maharaj Nagpur University Campus, Nagpur-440033 (India); Deshpande, U. P. [UGC-DAE Consortium for scientific Research, University Campus, Khandwa Road, Indore-452001, Madhya Pradesh,India (India)

2016-05-06

In the present attempt,novel perovskite oxide Dy{sub 0.5}Sr{sub 0.5}Co{sub 0.8}Fe{sub 0.2}O{sub 3–δ} (DSCF) as cathode material has been synthesized by an Ethylene glycol-citrate combined sol-gel combustion route. Orthorhombic symmetry structure is confirmed by X-ray diffraction (XRD) and data is well fitted using Rietveld refinement by Full-Prof software suite. Chemical natureof surface of DSCF has been analyzed by using X-ray photoelectron spectroscopy (XPS). XPS result shows that Dy ions are in +3 oxidation state and Sr in +2 states. However Co2p and Fe2p spectra indicates partial change in oxidation state from Co3+/Fe3+ to Co4+/Fe4+. These attribute to develop active sites on the surface for oxygen ions. O1s XPS spectra shows two oxygen peaks relatedto lattice oxygen in perovskite and absorbed oxygen in oxygen vacancy are detected. O1s spectra demonstrate the existence of adsorbed oxygen species on the surface of DSCF oxide which is quite beneficial for intermediate temperature of Solid Oxide Fuel Cell.

No oxygen isotope exchange between water and APS-sulfate at surface temperature: Evidence from quantum chemical modeling and triple-oxygen isotope experiments

Science.gov (United States)

Kohl, Issaku E.; Asatryan, Rubik; Bao, Huiming

2012-10-01

In both laboratory experiments and natural environments where microbial dissimilatory sulfate reduction (MDSR) occurs in a closed system, the δ34S ((34S/32S)sample/(34S/32S)standard - 1) for dissolved SO42- has been found to follow a typical Rayleigh-Distillation path. In contrast, the corresponding δ18O ((18O/16O)sample/(18O/16O)standard) - 1) is seen to plateau with an apparent enrichment of between 23‰ and 29‰ relative to that of ambient water under surface conditions. This apparent steady-state in the observed difference between δ18O and δ18OO can be attributed to any of these three steps: (1) the formation of adenosine-5'-phosphosulfate (APS) from ATP and SO42-, (2) oxygen exchange between sulfite (or other downstream sulfoxy-anions) and water later in the MDSR reaction chain and its back reaction to APS and sulfate, and (3) the re-oxidation of produced H2S or precursor sulfoxy-anions to sulfate in environments containing Fe(III) or O2. This study examines the first step as a potential pathway for water oxygen incorporation into sulfate. We examined the structures and process of APS formation using B3LYP/6-31G(d,p) hybrid density functional theory, implemented in the Gaussian-03 program suite, to predict the potential for oxygen exchange. We conducted a set of in vitro, enzyme-catalyzed, APS formation experiments (with no further reduction to sulfite) to determine the degree of oxygen isotope exchange between the APS-sulfate and water. Triple-oxygen-isotope labeled water was used in the reactor solutions to monitor oxygen isotope exchange between water and APS sulfate. The formation and hydrolysis of APS were identified as potential steps for oxygen exchange with water to occur. Quantum chemical modeling indicates that the combination of sulfate with ATP has effects on bond strength and symmetry of the sulfate. However, these small effects impart little influence on the integrity of the SO42- tetrahedron due to the high activation energy required for

On singularities of lattice varieties

OpenAIRE

Mukherjee, Himadri

2013-01-01

Toric varieties associated with distributive lattices arise as a fibre of a flat degeneration of a Schubert variety in a minuscule. The singular locus of these varieties has been studied by various authors. In this article we prove that the number of diamonds incident on a lattice point $\\a$ in a product of chain lattices is more than or equal to the codimension of the lattice. Using this we also show that the lattice varieties associated with product of chain lattices is smooth.

Bulk and surface properties of magnesium peroxide MgO2

Science.gov (United States)

Esch, Tobit R.; Bredow, Thomas

2016-12-01

Magnesium peroxide has been identified in Mg/air batteries as an intermediate in the oxygen reduction reaction (ORR) [1]. It is assumed that MgO2 is involved in the solid-electrolyte interphase on the cathode surface. Therefore its structure and stability play a crucial role in the performance of Mg/air batteries. In this work we present a theoretical study of the bulk and low-index surface properties of MgO2. All methods give a good account of the experimental lattice parameters for MgO2 and MgO bulk. The reaction energies, enthalpies and free energies for MgO2 formation from MgO are compared among the different DFT methods and with the local MP2 method. A pronounced dependence from the applied functional is found. At variance with a previous theoretical study but in agreement with recent experiments we find that the MgO2 formation reaction is endothermic (HSE06-D3BJ: ΔH = 51.9 kJ/mol). The stability of low-index surfaces MgO2 (001) (Es = 0.96 J/m2) and (011) (Es = 1.98 J/m2) is calculated and compared to the surface energy of MgO (001). The formation energy of neutral oxygen vacancies in the topmost layer of the MgO2 (001) surface is calculated and compared with defect formation energies for MgO (001).

Emergent dynamic structures and statistical law in spherical lattice gas automata

Science.gov (United States)

Yao, Zhenwei

2017-12-01

Various lattice gas automata have been proposed in the past decades to simulate physics and address a host of problems on collective dynamics arising in diverse fields. In this work, we employ the lattice gas model defined on the sphere to investigate the curvature-driven dynamic structures and analyze the statistical behaviors in equilibrium. Under the simple propagation and collision rules, we show that the uniform collective movement of the particles on the sphere is geometrically frustrated, leading to several nonequilibrium dynamic structures not found in the planar lattice, such as the emergent bubble and vortex structures. With the accumulation of the collision effect, the system ultimately reaches equilibrium in the sense that the distribution of the coarse-grained speed approaches the two-dimensional Maxwell-Boltzmann distribution despite the population fluctuations in the coarse-grained cells. The emergent regularity in the statistical behavior of the system is rationalized by mapping our system to a generalized random walk model. This work demonstrates the capability of the spherical lattice gas automaton in revealing the lattice-guided dynamic structures and simulating the equilibrium physics. It suggests the promising possibility of using lattice gas automata defined on various curved surfaces to explore geometrically driven nonequilibrium physics.

Emergent dynamic structures and statistical law in spherical lattice gas automata.

Science.gov (United States)

Yao, Zhenwei

2017-12-01

Various lattice gas automata have been proposed in the past decades to simulate physics and address a host of problems on collective dynamics arising in diverse fields. In this work, we employ the lattice gas model defined on the sphere to investigate the curvature-driven dynamic structures and analyze the statistical behaviors in equilibrium. Under the simple propagation and collision rules, we show that the uniform collective movement of the particles on the sphere is geometrically frustrated, leading to several nonequilibrium dynamic structures not found in the planar lattice, such as the emergent bubble and vortex structures. With the accumulation of the collision effect, the system ultimately reaches equilibrium in the sense that the distribution of the coarse-grained speed approaches the two-dimensional Maxwell-Boltzmann distribution despite the population fluctuations in the coarse-grained cells. The emergent regularity in the statistical behavior of the system is rationalized by mapping our system to a generalized random walk model. This work demonstrates the capability of the spherical lattice gas automaton in revealing the lattice-guided dynamic structures and simulating the equilibrium physics. It suggests the promising possibility of using lattice gas automata defined on various curved surfaces to explore geometrically driven nonequilibrium physics.

Reactor lattice codes

International Nuclear Information System (INIS)

Kulikowska, T.

2001-01-01

The description of reactor lattice codes is carried out on the example of the WIMSD-5B code. The WIMS code in its various version is the most recognised lattice code. It is used in all parts of the world for calculations of research and power reactors. The version WIMSD-5B is distributed free of charge by NEA Data Bank. The description of its main features given in the present lecture follows the aspects defined previously for lattice calculations in the lecture on Reactor Lattice Transport Calculations. The spatial models are described, and the approach to the energy treatment is given. Finally the specific algorithm applied in fuel depletion calculations is outlined. (author)

In vivo XCT bone characterization of lattice structured implants fabricated by additive manufacturing

Directory of Open Access Journals (Sweden)

A-F. Obaton

2017-08-01

Full Text Available Several cylindrical specimens and dental implants, presenting diagonal lattice structures with different cell sizes (600, 900 and 1200 μm were additively manufactured by selective laser melting process. Then they were implanted for two months in a sheep. After removal, they were studied by Archimedes’ method as well as X-ray computed tomography in order to assess the penetration of bone into the lattice. We observed that the additive manufactured parts were geometrically conformed to the theoretical specifications. However, several particles were left adhering to the surface of the lattice, thereby partly or entirely obstructing the cells. Nevertheless, bone penetration was clearly visible. We conclude that the 900 μm lattice cell size is more favourable to bone penetration than the 1200 μm lattice cell size, as the bone penetration is 84% for 900 μm against 54% for 1200 μm cell structures. The lower bone penetration value for the 1200 μm lattice cell could possibly be attributed to the short residence time in the sheep. Our results lead to the conclusion that lattice implants additively manufactured by selective laser melting enable better bone integration.

Lattice topology dictates photon statistics.

Science.gov (United States)

Kondakci, H Esat; Abouraddy, Ayman F; Saleh, Bahaa E A

2017-08-21

Propagation of coherent light through a disordered network is accompanied by randomization and possible conversion into thermal light. Here, we show that network topology plays a decisive role in determining the statistics of the emerging field if the underlying lattice is endowed with chiral symmetry. In such lattices, eigenmode pairs come in skew-symmetric pairs with oppositely signed eigenvalues. By examining one-dimensional arrays of randomly coupled waveguides arranged on linear and ring topologies, we are led to a remarkable prediction: the field circularity and the photon statistics in ring lattices are dictated by its parity while the same quantities are insensitive to the parity of a linear lattice. For a ring lattice, adding or subtracting a single lattice site can switch the photon statistics from super-thermal to sub-thermal, or vice versa. This behavior is understood by examining the real and imaginary fields on a lattice exhibiting chiral symmetry, which form two strands that interleave along the lattice sites. These strands can be fully braided around an even-sited ring lattice thereby producing super-thermal photon statistics, while an odd-sited lattice is incommensurate with such an arrangement and the statistics become sub-thermal.

Oxygen Electrode Kinetics and Surface Composition of Dense (La0.75Sr0.25)0.95MnO3 on YSZ

DEFF Research Database (Denmark)

Wu, Yuehua; Hansen, Karin Vels; Norrman, Kion

2013-01-01

in situ at temperatures from 660 to 860 C using a controlled atmosphere high temperature scanning probe microscope (CAHT-SPM) setup for measurements of impedance spectroscopy and potential sweep. The oxygen partial pressure, pO2, was varied. Further, ex situ surface analysis by time of flight secondary...... ion mass spectrometry (TOF-SIMS) and structure examination by scanning electron microscopy (SEM) were performed. Segregation of Sr and La oxides to LSM surfaces and Mn rich oxide to the three phase boundary (TPB) was observed. YSZ and LSM attract different oxides/impurities. The oxygen electrode...

Void lattices

International Nuclear Information System (INIS)

Chadderton, L.T.; Johnson, E.; Wohlenberg, T.

1976-01-01

Void lattices in metals apparently owe their stability to elastically anisotropic interactions. An ordered array of voids on the anion sublattice in fluorite does not fit so neatly into this scheme of things. Crowdions may play a part in the formation of the void lattice, and stability may derive from other sources. (Auth.)

Introduction of oxygen vacancies and fluorine into TiO2 nanoparticles by co-milling with PTFE

International Nuclear Information System (INIS)

Senna, Mamoru; Šepelák, Vladimir; Shi, Jianmin; Bauer, Benjamin; Feldhoff, Armin; Laporte, Vincent; Becker, Klaus-Dieter

2012-01-01

Solid-state processes of introducing oxygen vacancies and transference of fluorine to n-TiO 2 nanoparticles by co-milling with poly(tetrafluoroethylene) (PTFE) powder were examined by diffuse reflectance spectroscopy (DRS) of UV, visual, near- and mid-IR regions, thermal analyses (TG-DTA), energy-dispersive X-ray spectroscopy (EDXS), X-ray photoelectron spectroscopy (XPS), high-resolution transmission electron microscopy (HRTEM) and X-ray diffraction (XRD). The broad absorption peak at around 8800 cm −1 (1140 nm) was attributed to the change in the electronic states, viz. electrons trapped at the oxygen vacancies (Vo) and d–d transitions of titanium ions. Incorporation of fluorine into n-TiO 2 was concentrated at the near surface region and amounted to ca. 40 at% of the total fluorine in PTFE, after co-milling for 3 h, as confirmed by the F1s XPS spectrum. The overall atomic ratio, F/Ti, determined by EDXS was 0.294. By combining these analytical results, a mechanism of the present solid state processes at the boundary between PTFE and n-TiO 2 was proposed. The entire process is triggered by the partial oxidative decomposition of PTFE. This is accompanied by the abstraction of oxygen atoms from the n-TiO 2 lattices. Loss of the oxygen atoms results in the formation of the diverse states of locally distorted coordination units of titania, i.e. TiO 6−n Vo n , located at the near surface region. This leads subsequent partial ligand exchange between F and O, to incorporate fluorine preferentially to the near surface region of n-TiO 2 particles, where local non-crystalline states predominate. - Graphical abstract: Scheme of the reaction processes: (a) pristine mixture, (b) oxygen abstraction from TiO 2 and (c) fluorine migration from PTFE to TiO 2 . Highlights: Transfer of fluorine from PTFE to n-TiO 2 in a dry solid state process was confirmed. ► 40% of F in PTFE was incorporated to the near surface region of n-TiO 2 nanoparticles. ► The transfer process is

Polaron-Driven Surface Reconstructions

Directory of Open Access Journals (Sweden)

Michele Reticcioli

2017-09-01

Full Text Available Geometric and electronic surface reconstructions determine the physical and chemical properties of surfaces and, consequently, their functionality in applications. The reconstruction of a surface minimizes its surface free energy in otherwise thermodynamically unstable situations, typically caused by dangling bonds, lattice stress, or a divergent surface potential, and it is achieved by a cooperative modification of the atomic and electronic structure. Here, we combined first-principles calculations and surface techniques (scanning tunneling microscopy, non-contact atomic force microscopy, scanning tunneling spectroscopy to report that the repulsion between negatively charged polaronic quasiparticles, formed by the interaction between excess electrons and the lattice phonon field, plays a key role in surface reconstructions. As a paradigmatic example, we explain the (1×1 to (1×2 transition in rutile TiO_{2}(110.

The formation of non-oxidic oxygen phases on Ru(0001). From the first stages of the oxygen take-up to oxidation

International Nuclear Information System (INIS)

Blume, R.

2005-01-01

The aim of the thesis presented here was the investigation of the formation of non oxidic oxygen phases on the Ru(0001) surface. Smooth and defect rich surfaces were exposed to high oxygen pressures (up to 1 bar) at moderate temperatures (550 K). The characterisation was performed under UHV conditions using Thermal Desorption Spectroscopy (TDS), Scanning Photoemission Microscopy (SPEM), Thermal Energy Atomic Scattering (TEAS), Ultraviolett Photoelectron Spectroscopy (UPS) and Low Energy Electron Diff raction (LEED) as well as In situ by the In Situ X-Ray Photoelectron Spectroscopy (In Situ XPS). The application of this Low Temperature preparation procedure (LT) leads to an Oxygen uptake up to 3 MLE of ''subsurface'' oxygen into a smooth Ru(0001) surface without the typical indications of oxidation (MLE: Monolayer Equivalent). The accumulation of oxygen beneath the surface starts immediatly after the completion of a full chemisorbed layer. Here, the local saturation of the adsorbed oxygen is the decisive step. Diff usion of oxygen directly through the chemisorbed layer only slightly contributes to the overall uptake. Oxygen is mostly accomodated in the vicinity of the surface via surface defects which has been shown on defect rich surfaces created by mild Ar+ sputtering. The maximum oxygen capacity is 10 Atoms/Defect. The uptake is thermally activated with an activation energy of 0.15 eV. The oxygen uptake causes a massive structural change of at least the top two ruthenium layers. Whereas the ruthenium atoms of the first layer are coordinated with up to four, those of the second layer are coordinated with up to two oxygen atoms. These binding condition are metastable and can be changed by annealing the surface. With reaching the desorption temperature two distinct desorption peaks are observed with TDS. For an accumulation of about 0.5 MLE of ''subsurface'' oxygen the desorption proceeds exclusively at the characteristic temperature of the chemisorbed layer at 1040

Lattice theory for nonspecialists

International Nuclear Information System (INIS)

Hari Dass, N.D.

1984-01-01

These lectures were delivered as part of the academic training programme at the NIKHEF-H. These lectures were intended primarily for experimentalists, and theorists not specializing in lattice methods. The goal was to present the essential spirit behind the lattice approach and consequently the author has concentrated mostly on issues of principle rather than on presenting a large amount of detail. In particular, the author emphasizes the deep theoretical infra-structure that has made lattice studies meaningful. At the same time, he has avoided the use of heavy formalisms as they tend to obscure the basic issues for people trying to approach this subject for the first time. The essential ideas are illustrated with elementary soluble examples not involving complicated mathematics. The following subjects are discussed: three ways of solving the harmonic oscillator problem; latticization; gauge fields on a lattice; QCD observables; how to solve lattice theories. (Auth.)

Wetting of the diamond surface

International Nuclear Information System (INIS)

Hansen, J.O.

1987-01-01

The surface conditions which lead to a wide variation in the wettability of diamond surfaces have been investigated using macroscopic surfaces to allow for the crystal anisotropy. A wetting balance method of calculating adhesion tension and hence contact angle has been used for diamonds having major faces near the [111] and [110] lattice planes. Three classes of behaviour have been identified. Surface analyses by Rutherford Backscattering of helium ions, X-ray Photoelectron Spectroscopy and Low Energy Electron Diffraction (LEED) have been used to define the role of the oxygen coverage of the surface in the transition I → O → H. Ferric ion has a hydrophilizing effect on the diamond surface, thought to be the consequence of attachment to the hydroxyl groups at the surface by a ligand mechanism. Other transition metal ions did not show this effect. The phenomenon of hydration of the surface, i.e. progressively more hydrophilic behaviour on prolonged exposure to liquid water, has been quantified. Imbibition or water penetration at microcracks are thought unlikely, and a water cluster build-up at hydrophilic sites is thought to be the best explanation. Dynamic studies indicate little dependence of the advancing contact angle on velocity for velocities up to 10 -4 m/s, and slight dependence of the receding contact angle. Hence advancing angles by this technique are similar to equilibrated contact angles found by optical techniques, but the receding angles are lower than found by other non-dynamic measurements

Unraveling the facet-dependent and oxygen vacancy role for ethylene hydrogenation on Co{sub 3}O{sub 4} (110) surface: A DFT+U study

Energy Technology Data Exchange (ETDEWEB)

Zhang, Yong-Chao; Pan, Lun; Lu, Jinhui; Song, Jiajia; Li, Zheng; Zhang, Xiangwen; Wang, Li [Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Tianjin University (China); Collaborative Innovative Center of Chemical Science and Engineering (Tianjin), Tianjin 300072 (China); Zou, Ji-Jun, E-mail: jj_zou@tju.edu.cn [Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Tianjin University (China); Collaborative Innovative Center of Chemical Science and Engineering (Tianjin), Tianjin 300072 (China)

2017-04-15

Highlights: • The mechanism of ethylene hydrogenation on perfect and oxygen defective Co{sub 3}O{sub 4}(110) is investigated by using DFT + U. • Oxygen vacancy promotes ethylene hydrogenation thermodynamically and kinetically. • The Co3O4 (110) facet is more active than the (111) one for ethylene hydrogenation. - Abstract: Crystal facet engineering and defect engineering are both critical strategies to improve the catalytic hydrogenation performance of catalyst. Herein, ethylene hydrogenation on the perfect and oxygen defective Co{sub 3}O{sub 4}(110) surfaces has been studied by using periodic density functional theory calculations. The results are compared with that on Co{sub 3}O{sub 4}(111) surface to clarify the problem of which facet for Co{sub 3}O{sub 4} is more reactive, and to illuminate the role of oxygen vacancy. The low oxygen vacancy formation energy suggests that Co{sub 3}O{sub 4}(110) surface with defective site is easily formed. The whole mechanism of H{sub 2} dissociation and stepwise hydrogenation of ethylene to ethane is examined, and the most favorable pathway is heterolytic dissociation of H{sub 2} follows two stepwise hydrogenation of ethylene process. The results show that ethyl hydrogenation to ethane on perfect Co{sub 3}O{sub 4}(110) surface is the rate limiting step with an activation energy of 1.19 eV, and the presence of oxygen vacancy strongly reduces the activation energies of main elementary steps, and the activation energy of rate limiting step is only 0.47 eV. Compared with that on Co{sub 3}O{sub 4}(111), ethylene hydrogenation is preferred on Co{sub 3}O{sub 4}(110) surface. Therefore, Co{sub 3}O{sub 4} with exposed (110) facet is predicted as an excellent catalyst for ethylene hydrogenation.

A semiflexible alternating copolymer chain adsorption on a flat and a fluctuating surface

International Nuclear Information System (INIS)

Mishra, Pramod Kumar

2010-01-01

A lattice model of a directed self-avoiding walk is used to investigate adsorption properties of a semiflexible alternating copolymer chain on an impenetrable flat and fluctuating surface in two (square, hexagonal and rectangular lattice) and three dimensions (cubic lattice). In the cubic lattice case the surface is two-dimensional impenetrable flat and in two dimensions the surface is a fluctuating impenetrable line (hexagonal lattice) and also flat impenetrable line (square and rectangular lattice). Walks of the copolymer chains are directed perpendicular to the plane of the surface and at a suitable value of monomer surface attraction, the copolymer chain gets adsorbed on the surface. To calculate the exact value of the monomer surface attraction, the directed walk model has been solved analytically using the generating function method to discuss results when one type of monomer of the copolymer chain has attractive, repulsive or no interaction with the surface. Results obtained in the flat surface case show that, for a stiffer copolymer chain, adsorption transition occurs at a smaller value of monomer surface attraction than a flexible copolymer chain while in the case of a fluctuating surface, the adsorption transition point is independent of bending energy of the copolymer chain. These features are similar to that of a semiflexible homopolymer chain adsorption.

A semiflexible alternating copolymer chain adsorption on a flat and a fluctuating surface.

Science.gov (United States)

Mishra, Pramod Kumar

2010-04-21

A lattice model of a directed self-avoiding walk is used to investigate adsorption properties of a semiflexible alternating copolymer chain on an impenetrable flat and fluctuating surface in two (square, hexagonal and rectangular lattice) and three dimensions (cubic lattice). In the cubic lattice case the surface is two-dimensional impenetrable flat and in two dimensions the surface is a fluctuating impenetrable line (hexagonal lattice) and also flat impenetrable line (square and rectangular lattice). Walks of the copolymer chains are directed perpendicular to the plane of the surface and at a suitable value of monomer surface attraction, the copolymer chain gets adsorbed on the surface. To calculate the exact value of the monomer surface attraction, the directed walk model has been solved analytically using the generating function method to discuss results when one type of monomer of the copolymer chain has attractive, repulsive or no interaction with the surface. Results obtained in the flat surface case show that, for a stiffer copolymer chain, adsorption transition occurs at a smaller value of monomer surface attraction than a flexible copolymer chain while in the case of a fluctuating surface, the adsorption transition point is independent of bending energy of the copolymer chain. These features are similar to that of a semiflexible homopolymer chain adsorption.

Fundamental Mechanistic Understanding of Electrocatalysis of Oxygen Reduction on Pt and Non-Pt Surfaces: Acid versus Alkaline Media

Directory of Open Access Journals (Sweden)

Nagappan Ramaswamy

2012-01-01

Full Text Available Complex electrochemical reactions such as Oxygen Reduction Reaction (ORR involving multi-electron transfer is an electrocatalytic inner-sphere electron transfer process that exhibit strong dependence on the nature of the electrode surface. This criterion (along with required stability in acidic electrolytes has largely limited ORR catalysts to the platinum-based surfaces. New evidence in alkaline media, discussed here, throws light on the involvement of surface-independent outer-sphere electron transfer component in the overall electrocatalytic process. This surface non-specificity gives rise to the possibility of using a wide-range of non-noble metal surfaces as electrode materials for ORR in alkaline media. However, this outer-sphere process predominantly leads only to peroxide intermediate as the final product. The importance of promoting the electrocatalytic inner-sphere electron transfer by facilitation of direct adsorption of molecular oxygen on the active site is emphasized by using pyrolyzed metal porphyrins as electrocatalysts. A comparison of ORR reaction mechanisms between acidic and alkaline conditions is elucidated here. The primary advantage of performing ORR in alkaline media is found to be the enhanced activation of the peroxide intermediate on the active site that enables the complete four-electron transfer. ORR reaction schemes involving both outer- and inner-sphere electron transfer mechanisms are proposed.

Spin wave relaxation and magnetic properties in [M/Cu] super-lattices; M=Fe, Co and Ni

International Nuclear Information System (INIS)

Fahmi, A.; Qachaou, A.

2009-01-01

In this work, we study the elementary excitations and magnetic properties of the [M/Cu] super-lattices with: M=Fe, Co and Ni, represented by a Heisenberg ferromagnetic system with N atomic planes. The nearest neighbour (NN), next nearest neighbour (NNN) exchange, dipolar interactions and surface anisotropy effects are taken into account and the Hamiltonian is studied in the framework of the linear spin wave theory. In the presence of the exchange alone, the excitation spectrum E(k) and the magnetization z >/S analytical expressions are obtained using the Green's function formalism. The obtained relaxation time of the magnon populations is nearly the same in the Fe and Co-based super-lattices, while these magnetic excitations would last much longer in the Ni-based super lattice. A numerical study of the surface anisotropy and long-ranged dipolar interaction combined effects are also reported. The exchange integral values deduced from a comparison with experience for the three super-lattices are coherent.

MEETING: Lattice 88

Energy Technology Data Exchange (ETDEWEB)

Mackenzie, Paul

1989-03-15

The forty-year dream of understanding the properties of the strongly interacting particles from first principles is now approaching reality. Quantum chromodynamics (QCD - the field theory of the quark and gluon constituents of strongly interacting particles) was initially handicapped by the severe limitations of the conventional (perturbation) approach in this picture, but Ken Wilson's inventions of lattice gauge theory and renormalization group methods opened new doors, making calculations of masses and other particle properties possible. Lattice gauge theory became a major industry around 1980, when Monte Carlo methods were introduced, and the first prototype calculations yielded qualitatively reasonable results. The promising developments over the past year were highlighted at the 1988 Symposium on Lattice Field Theory - Lattice 88 - held at Fermilab.

MEETING: Lattice 88

International Nuclear Information System (INIS)

Mackenzie, Paul

1989-01-01

The forty-year dream of understanding the properties of the strongly interacting particles from first principles is now approaching reality. Quantum chromodynamics (QCD - the field theory of the quark and gluon constituents of strongly interacting particles) was initially handicapped by the severe limitations of the conventional (perturbation) approach in this picture, but Ken Wilson's inventions of lattice gauge theory and renormalization group methods opened new doors, making calculations of masses and other particle properties possible. Lattice gauge theory became a major industry around 1980, when Monte Carlo methods were introduced, and the first prototype calculations yielded qualitatively reasonable results. The promising developments over the past year were highlighted at the 1988 Symposium on Lattice Field Theory - Lattice 88 - held at Fermilab

Iodine doping effects on the lattice thermal conductivity of oxidized polyacetylene nanofibers

Energy Technology Data Exchange (ETDEWEB)

Bi, Kedong, E-mail: lishi@mail.utexas.edu, E-mail: kedongbi@seu.edu.cn [Jiangsu Key Laboratory for Design and Manufacture of Micro-Nano Biomedical Instruments, School of Mechanical Engineering, Southeast University, Nanjing 211189 (China); Department of Mechanical Engineering, University of Texas at Austin, Austin, Texas 78712 (United States); Weathers, Annie; Pettes, Michael T.; Shi, Li, E-mail: lishi@mail.utexas.edu, E-mail: kedongbi@seu.edu.cn [Department of Mechanical Engineering, University of Texas at Austin, Austin, Texas 78712 (United States); Matsushita, Satoshi; Akagi, Kazuo [Department of Polymer Chemistry, Kyoto University, Kyoto 615-8510 (Japan); Goh, Munju [Department of Polymer Chemistry, Kyoto University, Kyoto 615-8510 (Japan); Institute of Advanced Composite Materials, Korea Institute of Science and Technology (KIST), Eunha-ri san 101, Bondong-eup, Wanju-gun, Jeolabuk-do 565-905 (Korea, Republic of)

2013-11-21

Thermal transport in oxidized polyacetylene (PA) nanofibers with diameters in the range between 74 and 126 nm is measured with the use of a suspended micro heater device. With the error due to both radiation and contact thermal resistance corrected via a differential measurement procedure, the obtained thermal conductivity of oxidized PA nanofibers varies in the range between 0.84 and 1.24 W m{sup −1} K{sup −1} near room temperature, and decreases by 40%–70% after iodine doping. It is also found that the thermal conductivity of oxidized PA nanofibers increases with temperature between 100 and 350 K. Because of exposure to oxygen during sample preparation, the PA nanofibers are oxidized to be electrically insulating before and after iodine doping. The measurement results reveal that iodine doping can result in enhanced lattice disorder and reduced lattice thermal conductivity of PA nanofibers. If the oxidation issue can be addressed via further research to increase the electrical conductivity via doping, the observed suppressed lattice thermal conductivity in doped polymer nanofibers can be useful for the development of such conducting polymer nanostructures for thermoelectric energy conversion.

Iodine doping effects on the lattice thermal conductivity of oxidized polyacetylene nanofibers

International Nuclear Information System (INIS)

Bi, Kedong; Weathers, Annie; Pettes, Michael T.; Shi, Li; Matsushita, Satoshi; Akagi, Kazuo; Goh, Munju

2013-01-01

Thermal transport in oxidized polyacetylene (PA) nanofibers with diameters in the range between 74 and 126 nm is measured with the use of a suspended micro heater device. With the error due to both radiation and contact thermal resistance corrected via a differential measurement procedure, the obtained thermal conductivity of oxidized PA nanofibers varies in the range between 0.84 and 1.24 W m −1  K −1 near room temperature, and decreases by 40%–70% after iodine doping. It is also found that the thermal conductivity of oxidized PA nanofibers increases with temperature between 100 and 350 K. Because of exposure to oxygen during sample preparation, the PA nanofibers are oxidized to be electrically insulating before and after iodine doping. The measurement results reveal that iodine doping can result in enhanced lattice disorder and reduced lattice thermal conductivity of PA nanofibers. If the oxidation issue can be addressed via further research to increase the electrical conductivity via doping, the observed suppressed lattice thermal conductivity in doped polymer nanofibers can be useful for the development of such conducting polymer nanostructures for thermoelectric energy conversion

Surface modification of carbon/epoxy prepreg using oxygen plasma and its effect on the delamination resistance behavior of carbon/epoxy composites

International Nuclear Information System (INIS)

Kim, M.H.; Rhee, K.Y.; Kim, H.J.; Jung, D.H.

2007-01-01

It was shown in previous study that the fracture toughness of carbon/epoxy laminated composites could be significantly improved by modifying the surface of the prepreg using Ar + irradiation in an oxygen environment. In this study, the surface of carbon/epoxy prepreg was modified using an oxygen plasma to improve the delamination resistance behavior of carbon/epoxy laminated composites. The variation of the contact angle on the prepreg surface was determined as a function of the modification time, in order to determine the optimal modification time. An XPS analysis was conducted to investigate the chemical changes on the surface of the prepreg caused by the plasma modification. Mode I delamination resistance curves of the composites with and without surface modification were plotted as a function of the delamination increment. The results showed that the contact angle varied from ∼64 o to ∼47 o depending on the modification time and reached a minimum for a modification time of 30 min. The XPS analysis showed that the hydrophilic carbonyl C=O group was formed by the oxygen plasma modification. The results also showed that the delamination resistance behavior was significantly improved by the plasma modification of the prepreg. This improvement was caused by the better layer-to-layer adhesion as well as increased interfacial strength between the fibers and matrix

Surface oxygenation of polypropylene using an air dielectric barrier discharge: the effect of different electrode-platen combinations