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Sample records for local electronic structure

  1. Electronic-structure calculation for metals by local optimization

    SciTech Connect

    Woodward, C.; Min, B.I.; Benedek, R.; Garner, J.

    1989-03-15

    Recent work by Car and Parrinello has generated considerable interest in the calculation of electronic structure by nonlinear optimization. The technique introduced by these authors, dynamical simulated annealing, is designed for problems that involve energy barriers. When local optimization suffices to determine the energy minimum, more direct methods are available. In this paper we apply the algorithm suggested by Williams and Soler to calculate the electronic structure of metals, using a plane-wave expansion for the electronic orbitals and an electron-ion pseudopotential of the Kleinman-Bylander form. Radial pseudopotentials were taken from the compilation of Bachelet, Hamann, and Schlueter. Calculations are performed to optimize the electronic structure (i) with fixed atomic configuration, or (ii) with the atomic volume being optimized simultaneously. It is found that the dual optimization (ii) converges in essentially the same number of steps as the static lattice optimization (i). Numerical results are presented for Li, K, Al, and simple-cubic P.

  2. Correlation of Local Structure and Electronic Properties of Glass Materials

    NASA Astrophysics Data System (ADS)

    Lordi, Vincenzo; Adelstein, Nicole

    2015-03-01

    Wide band gap glasses such as silica and its derivatives are typically considered insulators. However, electronic transport in glasses can be important for certain applications, such as when used as the host material for a scintillator radiation detector. Here we explore the relationship between local structure in glass materials and the corresponding electronic properties of carrier transport and charge trapping. We present a novel analysis that decomposes the distribution of localized band tail states in terms of specific local structural features in the glass. Comparison of the structure-related transport properties of different glass compositions is given, using silica and sodium silicate as prototypes. Prepared by LLNL under Contract DE-AC52-07NA27344.

  3. Local atomic order, electronic structure and electron transport properties of Cu-Zr metallic glasses

    SciTech Connect

    Antonowicz, J. Pietnoczka, A.; Pękała, K.; Latuch, J.; Evangelakis, G. A.

    2014-05-28

    We studied atomic and electronic structures of binary Cu-Zr metallic glasses (MGs) using combined experimental and computational methods including X-ray absorption fine structure spectroscopy, electrical resistivity, thermoelectric power (TEP) measurements, molecular dynamics (MD) simulations, and ab-initio calculations. The results of MD simulations and extended X-ray absorption fine structure analysis indicate that atomic order of Cu-Zr MGs and can be described in terms of interpenetrating icosahedral-like clusters involving five-fold symmetry. MD configurations were used as an input for calculations of theoretical electronic density of states (DOS) functions which exhibits good agreement with the experimental X-ray absorption near-edge spectra. We found no indication of minimum of DOS at Fermi energy predicted by Mott's nearly free electron (NFE) model for glass-forming alloys. The theoretical DOS was subsequently used to test Mott's model describing the temperature variation of electrical resistivity and thermoelectric power of transition metal-based MGs. We demonstrate that the measured temperature variations of electrical resistivity and TEP remain in a contradiction with this model. On the other hand, the experimental temperature dependence of electrical resistivity can be explained by incipient localization of conduction electrons. It is shown that weak localization model works up to relatively high temperatures when localization is destroyed by phonons. Our results indicate that electron transport properties of Cu-Zr MGs are dominated by localization effects rather than by electronic structure. We suggest that NFE model fails to explain a relatively high glass-forming ability of binary Cu-Zr alloys.

  4. Local atomic order, electronic structure and electron transport properties of Cu-Zr metallic glasses

    NASA Astrophysics Data System (ADS)

    Antonowicz, J.; Pietnoczka, A.; Pekała, K.; Latuch, J.; Evangelakis, G. A.

    2014-05-01

    We studied atomic and electronic structures of binary Cu-Zr metallic glasses (MGs) using combined experimental and computational methods including X-ray absorption fine structure spectroscopy, electrical resistivity, thermoelectric power (TEP) measurements, molecular dynamics (MD) simulations, and ab-initio calculations. The results of MD simulations and extended X-ray absorption fine structure analysis indicate that atomic order of Cu-Zr MGs and can be described in terms of interpenetrating icosahedral-like clusters involving five-fold symmetry. MD configurations were used as an input for calculations of theoretical electronic density of states (DOS) functions which exhibits good agreement with the experimental X-ray absorption near-edge spectra. We found no indication of minimum of DOS at Fermi energy predicted by Mott's nearly free electron (NFE) model for glass-forming alloys. The theoretical DOS was subsequently used to test Mott's model describing the temperature variation of electrical resistivity and thermoelectric power of transition metal-based MGs. We demonstrate that the measured temperature variations of electrical resistivity and TEP remain in a contradiction with this model. On the other hand, the experimental temperature dependence of electrical resistivity can be explained by incipient localization of conduction electrons. It is shown that weak localization model works up to relatively high temperatures when localization is destroyed by phonons. Our results indicate that electron transport properties of Cu-Zr MGs are dominated by localization effects rather than by electronic structure. We suggest that NFE model fails to explain a relatively high glass-forming ability of binary Cu-Zr alloys.

  5. Electron Spectroscopy of Single Quantum Objects To Directly Correlate the Local Structure to Their Electronic Transport and Optical Properties.

    PubMed

    Senga, Ryosuke; Pichler, Thomas; Suenaga, Kazu

    2016-06-01

    Physical property of a single quantum object is governed by its precise atomic arrangement. The direct correlation of localized physical properties with the atomic structures has been therefore strongly desired but still limited in the theoretical studies. Here, we have successfully examined the localized electronic properties of individual carbon nanotubes by means of high-resolution electron energy-loss spectroscopy combined with high-resolution transmission electron microscopy. Well-separated sharp peaks at the carbon K(1s) absorption edge and in the valence-loss spectra are obtained from a single freestanding carbon nanotube with the local chiral index and unambiguously identified as the transitions between the van Hove singularities. The spectra features clearly vary upon the different areas even in the individual carbon nanotube. Variations in interband transitions, plasmonic behaviors, and unoccupied electronic structures are clearly attributed to the local irregular atomic arrangement such as topological defect and/or elastic bond stretching. PMID:27171894

  6. Local electronic structures and 2D topological phase transition of ultrathin Sb films

    NASA Astrophysics Data System (ADS)

    Kim, Sunghwan; Jin, Kyung-Hwan; Park, Joonbum; Kim, Jun Sung; Jhi, Seung-Hoon; Yeom, Han Woong

    We investigate local electronic structures of ultrathin Sb islands and their edges grown on Bi2Te2Se by scanning tunneling microscopy/spectroscopy (STM/STS) and density functional theory (DFT) calculations. The Sb islands of various thickness are grown with atomically well ordered edge structure over the 3 bilayers (BL). On the surfaces and edges of these islands, we clearly resolve edge-localized electronic states by STS measurements, which depend on the thickness. The DFT calculations identify that the strongly localized edge states of 4 and 5 BL films correspond to a quantum spin Hall (QSH) states while the edge states of 3 BL are trivial. Our experimental and theoretical results confirm the 2D topological phase transition of the ultrathin Sb films from trivial to QSH phase. Center for Artificial Low Dimensional Electronic Systems, Institute for Basic Science and Department of Physics, Pohang University of Science and Technology, Korea.

  7. On the robustness of the localized spatiotemporal structures in electron-positron-ion plasmas

    SciTech Connect

    Mahajan, S.M.; Berezhiani, V.I. |; Miklaszewski, R.

    1998-04-01

    It is shown that, in an electron-positron plasma with a small fraction of ions, large-amplitude localized spatiotemporal structures (light bullets) can be readily generated and sustained. These light bullets are found to be exceptionally robust: they can emerge from a large variety of initial field distributions and are remarkably stable.

  8. Distinct local electronic structure and magnetism for Mn in amorphous Si and Ge

    SciTech Connect

    Zeng, Li; Cao, J. X.; Helgren, E.; Karel, J.; Arenholz, E.; Ouyang, Lu; Smith, David J.; Wu, R. Q.; Hellman, F.

    2010-06-01

    Transition metals such as Mn generally have large local moments in covalent semiconductors due to their partially filled d shells. However, Mn magnetization in group-IV semiconductors is more complicated than often recognized. Here we report a striking crossover from a quenched Mn moment (<0.1 {mu}{sub B}) in amorphous Si (a-Si) to a large distinct local Mn moment ({ge}3{mu}{sub B}) in amorphous Ge (a-Ge) over a wide range of Mn concentrations (0.005-0.20). Corresponding differences are observed in d-shell electronic structure and the sign of the Hall effect. Density-functional-theory calculations show distinct local structures, consistent with different atomic density measured for a-Si and a-Ge, respectively, and the Mn coordination number N{sub c} is found to be the key factor. Despite the amorphous structure, Mn in a-Si is in a relatively well-defined high coordination interstitial type site with broadened d bands, low moment, and electron (n-type) carriers, while Mn in a-Ge is in a low coordination substitutional type site with large local moment and holes (p-type) carriers. Moreover, the correlation between N{sub c} and the magnitude of the local moment is essentially independent of the matrix; the local Mn moments approach zero when N{sub c} > 7 for both a-Si and a-Ge.

  9. Local, global and electronic structure of supported gold nanoclusters determined by EXAFS, XRD and XPS methods

    NASA Astrophysics Data System (ADS)

    Aldea, Nicolae; Rednic, Vasile; Pintea, Stelian; Marginean, Petru; Barz, Bogdan; Gluhoi, Andreea; Nieuwenhuys, Bernard E.; Neumann, Manfred; Yaning, Xie; Matei, Florica

    2009-07-01

    We analyze gold nanoclusters as supported catalysts by extended X-ray absorption fine structure, X-ray diffraction and X-ray photoelectron spectroscopy in order to determine their local, global and electronic structure. The present study points out a strong deformation of the local structure of the metal due to its interaction with oxide supports. We determine the particle size distribution and microstrain functions of the Au nanoclusters by X-ray diffraction method. Based on X-ray absorption fine structure spectroscopy analysis we show that the entire local structure of the investigated systems is strongly distorted regarding the average Au-Au coordination number. The distances between atoms are practically the same as standard Au foil. The strong metal-support interaction is confirmed by the change in shape of the electron transition probability densities that appear in the Au L III-edge. From XPS investigations we find electronic states corresponding to gold as well as to the oxide supports.

  10. Local Structure, Electronic Behavior, and Electrocatalytic Reactivity of CO-Reduced Platinum-Iron Oxide Nanoparticles

    SciTech Connect

    Duchesne, Paul N.; Chen, Guangxu; Zheng, Nanfeng; Zhang, Peng

    2014-02-18

    A series of platinum–iron oxide nanoparticles was synthesized using a “clean” CO-reduction method that employed different ratios of Pt-Fe precursor salts in oleylamine at elevated temperatures. High-resolution transmission electron microscopy (HRTEM) and energy-dispersive X-ray spectroscopy (EDS) studies revealed that nearly monodisperse (i.e., with relative standard deviations of less than 15%) nanoparticles with mean diameters of 3.5–4.4 nm and varied elemental compositions (Pt54Fe46 Pt70Fe30, and Pt87Fe13) were obtained. X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) measurements at the Pt L3- and Fe K-edges revealed that these nanoparticles all consisted of a Pt core with amorphous iron oxide on the surface. Furthermore, it was observed that the local structure (e.g., Pt–Pt bond distance and coordination number) and electronic behavior of the Pt–FeO nanoparticles (e.g., Pt d electron density and Fe valence state) are dependent on the Pt-Fe precursor ratios used in their synthesis. Quantum mechanical ab initio calculations were employed to interpret the results from X-ray spectroscopy and help elucidate the relationships between local structure and electronic properties in the nanoparticle samples. Finally, the surface reactivity of these nanoparticles in the oxygen reduction reaction (ORR) was explored, demonstrating higher electrocatalytic activity for all three platinum–iron oxide samples in comparison with a commercial Pt catalyst. The surface reactivity was also found to be sensitive to the Pt-Fe ratios of the nanoparticles and could be correlated with their local structure and electronic behavior.

  11. The Kohn-Sham kinetic energy density as indicator of the electron localization: atomic shell structure.

    PubMed

    Navarrete-López, Alejandra M; Garza, Jorge; Vargas, Rubicelia

    2008-03-14

    In this report, it is shown that the Kohn-Sham (KS) kinetic energy density (KED) contains the average local electrostatic potential (ALEP) and the average local ionization energy (ALIE); the shell structure in atomic systems is presented as one application of the KS-KED. By writing the KS-KED from the KS equations, this quantity was divided in three contributions: orbital, Coulomb, and exchange correlation. By studying several closed and open shell atoms, the shell structure was established by the maxima presented by the Coulomb contribution and the minima in the orbital contribution of the KS-KED. The exchange-correlation contribution to the KS-KED does not show maxima or minima, but this quantity shows bumps where the division between shells is expected. The results obtained in this work were compared with other shell structure indicators such as the electron localization function, the ALEP, the ALIE, and the radial distribution function. The most important result in this work is related to the fact that even when the ALEP and the ALIE functions were built with different arguments to each other, they are contained in the KS-KED. In this way, the KS-KED shows its importance to reveal the electron localization in atomic systems. PMID:18345880

  12. Scale-adaptive tensor algebra for local many-body methods of electronic structure theory

    SciTech Connect

    Liakh, Dmitry I

    2014-01-01

    While the formalism of multiresolution analysis (MRA), based on wavelets and adaptive integral representations of operators, is actively progressing in electronic structure theory (mostly on the independent-particle level and, recently, second-order perturbation theory), the concepts of multiresolution and adaptivity can also be utilized within the traditional formulation of correlated (many-particle) theory which is based on second quantization and the corresponding (generally nonorthogonal) tensor algebra. In this paper, we present a formalism called scale-adaptive tensor algebra (SATA) which exploits an adaptive representation of tensors of many-body operators via the local adjustment of the basis set quality. Given a series of locally supported fragment bases of a progressively lower quality, we formulate the explicit rules for tensor algebra operations dealing with adaptively resolved tensor operands. The formalism suggested is expected to enhance the applicability and reliability of local correlated many-body methods of electronic structure theory, especially those directly based on atomic orbitals (or any other localized basis functions).

  13. Local atomic and electronic structure of boron chemical doping in monolayer graphene.

    PubMed

    Zhao, Liuyan; Levendorf, Mark; Goncher, Scott; Schiros, Theanne; Pálová, Lucia; Zabet-Khosousi, Amir; Rim, Kwang Taeg; Gutiérrez, Christopher; Nordlund, Dennis; Jaye, Cherno; Hybertsen, Mark; Reichman, David; Flynn, George W; Park, Jiwoong; Pasupathy, Abhay N

    2013-10-01

    We use scanning tunneling microscopy and X-ray spectroscopy to characterize the atomic and electronic structure of boron-doped and nitrogen-doped graphene created by chemical vapor deposition on copper substrates. Microscopic measurements show that boron, like nitrogen, incorporates into the carbon lattice primarily in the graphitic form and contributes ~0.5 carriers into the graphene sheet per dopant. Density functional theory calculations indicate that boron dopants interact strongly with the underlying copper substrate while nitrogen dopants do not. The local bonding differences between graphitic boron and nitrogen dopants lead to large scale differences in dopant distribution. The distribution of dopants is observed to be completely random in the case of boron, while nitrogen displays strong sublattice clustering. Structurally, nitrogen-doped graphene is relatively defect-free while boron-doped graphene films show a large number of Stone-Wales defects. These defects create local electronic resonances and cause electronic scattering, but do not electronically dope the graphene film. PMID:24032458

  14. Local electronic structure in MgB2 from B12 β -NMR

    NASA Astrophysics Data System (ADS)

    Indris, Sylvio; Heitjans, Paul; Hattendorf, Jens; Zeitz, Wolf-Dietrich; Bredow, Thomas

    2007-01-01

    We performed β -NMR spectroscopic studies on B12 which was implanted into MgB2 to get insight into the local electronic structure of this high-temperature superconducting material. By measuring electric field gradients we probed the electronic charge distribution anisotropy around boron in this solid and thus obtained experimental information about the bonding by p electrons. Besides the absolute value, the sign of the electric field gradient was also experimentally determined. By comparison with quantum chemical calculations, some of which were performed in the present work, and with results from conventional NMR spectroscopy on B11 we were able to identify regular boron lattice sites as well as interstitial sites.

  15. TiO2 nanotube arrays for photocatalysis: Effects of crystallinity, local order, and electronic structure

    DOE PAGESBeta

    Liu, Jing; Hosseinpour, Pegah M.; Luo, Si; Heiman, Don; Menon, Latika; Arena, Dario A.; Lewis, Laura H.

    2014-11-19

    To furnish insight into correlations of electronic and local structure and photoactivity, arrays of short and long TiO₂ nanotubes were synthesized by electrochemical anodization of Ti foil, followed by thermal treatment in O₂ (oxidizing), Ar (inert), and H₂ (reducing) environments. The physical and electronic structures of these nanotubes were probed with x-ray diffraction, scanning electron microscopy, and synchrotron-based x-ray absorption spectroscopy, and correlated with their photocatalytic properties. The photocatalytic activity of the nanotubes was evaluated by monitoring the degradation of methyl orange under UV-VIS light irradiation. Results show that upon annealing at 350 °C all as-anodized amorphous TiO₂ nanotube samplesmore » partially transform to the anatase structure, with variations in the degree of crystallinity and in the concentration of local defects near the nanotubes' surface (~5 nm) depending on the annealing conditions. Degradation of methyl orange was not detectable for the as-anodized TiO₂ nanotubes regardless of their length. The annealed long nanotubes demonstrated detectable catalytic activity, which was more significant with the H₂-annealed nanotubes than with the Ar- and O₂-annealed nanotube samples. This enhanced photocatalytic response of the H₂-annealed long nanotubes relative to the other samples is positively correlated with the presence of a larger concentration of lattice defects (such as Ti3+ and anticipated oxygen vacancies) and a slightly lower degree of crystallinity near the nanotube surface. These physical and electronic structural attributes impact the efficacy of visible light absorption; moreover, the increased concentration of surface defects is postulated to promote the generation of hydroxyl radicals and thus accelerate the photodegradation of the methyl orange. The information obtained from this study provides unique insight into the role of the near-surface electronic and defect structure

  16. The effects of local correlations on the electronic structure of FeSe

    NASA Astrophysics Data System (ADS)

    Watson, Matthew; Kim, Timur; Haghighirad, Amir; Coldea, Amalia

    FeSe is structurally the simplest of Fe-based superconductors, but its complex and unique properties pose important theoretical questions. One important aspect of the physics of FeSe is the understanding of the strength and effects of electronic correlations. In order to explore this, we have performed angle-resolved photo-emission spectroscopy (ARPES) measurements on high quality bulk single crystals of FeSe over a wide range of binding energies, in different scattering geometries and with varying incident photon energies, analysing the quasiparticle renormalisations, scattering rates and degree of coherence. We find that FeSe exhibits moderately strong, orbital-dependent correlation effects which are understood to arise primarily due to local electron-electron interactions on the Fe sites. We conclude that electronic correlations constitute a key ingredient in understanding the electronic structure of FeSe. Part of this work was supported by EPSRC, UK (EP/I004475/1, EP/I017836/1). We thank Diamond Light Source for access to Beamline I05.

  17. Electronic transport in graphene structure: from weak to strong localization regimes

    NASA Astrophysics Data System (ADS)

    Lherbier, Aurelien

    2015-03-01

    Graphene, often named the wonder material for its many fascinating properties, has sparked out intense research activities over the last decade. Electronic transport in graphene became rapidly an important research field because of the early reported extremely high charge carrier mobility which triggered large expectations for nanoelectronic devices. Besides mobilities, graphene samples can exhibit particularly long electronic coherence lengths which allow for phase-related quantum transport phenomena such as the weak and strong localization transport regimes. This makes graphene a remarkable playground for fundamental studies of localization theory in low-dimensional systems. In this presentation, using tight-binding models enriched by first principle calculations, and a real-space Kubo-Greenwood method, multiscale simulations of the electronic transport in various graphene-based systems will be discussed. Such an approach allows for computing transport properties of systems containing millions of atoms reaching therefore the experimental sample size. In order to tailor graphene properties, chemical and/or structural modifications are widely used. However, such modifications act as scattering defects and usually deteriorate transport properties. Open a band gap while maintaining good mobility is a typical illustration of this dual problem. The influence of various chemical and structural defects will be analyzed. In particular, the consequences of unbalanced sublattice nitrogen doping in graphene and the case of highly defective graphene structures exhibiting strong Anderson insulator behaviors will be examined. Defects being even more detrimental for transport in 1D structures, a synthesis method that is free of defects is highly desirable. A solution is provided by a bottom-up chemistry approach where precursor monomers are self-assembled. The electronic transport and the potential for nanoelectronics of such defect-free carbon ribbons will also be discussed.

  18. Structural and electronic properties of trans-polyacetylene under local strain

    NASA Astrophysics Data System (ADS)

    Ketabi, S. A.

    2016-06-01

    A theoretical study is presented to investigate the structural and electronic properties of trans-polyacetylene (trans-PA) molecule under local strain. The influence of a local bending or compression of the space between neighboring carbon atoms on the band gap of the molecule was studied. Making use of an effective difference equation based on tight-binding procedure the band structure of trans-PA has been calculated. Our results indicate that the energy gap of the strained molecule modified significantly which affects the electronic properties of the molecule. We found that the size of the molecular gap is proportional to the bending angle so that for the bending perpendicular to π-orbitals plane the band gap reduced drastically and for the parallel one the band gap gradually increased. Furthermore, the current-voltage characteristics of the strained trans-PA molecule are studied. We found that under the local strain the threshold voltage for the current flow through the bent molecule decreased (increased) depending on the bending is perpendicular (parallel) to the molecule plane.

  19. Localization of fluorescently labeled structures in frozen-hydrated samples using integrated light electron microscopy.

    PubMed

    Faas, F G A; Bárcena, M; Agronskaia, A V; Gerritsen, H C; Moscicka, K B; Diebolder, C A; van Driel, L F; Limpens, R W A L; Bos, E; Ravelli, R B G; Koning, R I; Koster, A J

    2013-03-01

    Correlative light and electron microscopy is an increasingly popular technique to study complex biological systems at various levels of resolution. Fluorescence microscopy can be employed to scan large areas to localize regions of interest which are then analyzed by electron microscopy to obtain morphological and structural information from a selected field of view at nm-scale resolution. Previously, an integrated approach to room temperature correlative microscopy was described. Combined use of light and electron microscopy within one instrument greatly simplifies sample handling, avoids cumbersome experimental overheads, simplifies navigation between the two modalities, and improves the success rate of image correlation. Here, an integrated approach for correlative microscopy under cryogenic conditions is presented. Its advantages over the room temperature approach include safeguarding the native hydrated state of the biological specimen, preservation of the fluorescence signal without risk of quenching due to heavy atom stains, and reduced photo bleaching. The potential of cryo integrated light and electron microscopy is demonstrated for the detection of viable bacteria, the study of in vitro polymerized microtubules, the localization of mitochondria in mouse embryonic fibroblasts, and for a search into virus-induced intracellular membrane modifications within mammalian cells. PMID:23261400

  20. Local conditions for the Pauli potential in order to yield self-consistent electron densities exhibiting proper atomic shell structure

    NASA Astrophysics Data System (ADS)

    Finzel, Kati

    2016-01-01

    The local conditions for the Pauli potential that are necessary in order to yield self-consistent electron densities from orbital-free calculations are investigated for approximations that are expressed with the help of a local position variable. It is shown that those local conditions also apply when the Pauli potential is given in terms of the electron density. An explicit formula for the Ne atom is given, preserving the local conditions during the iterative procedure. The resulting orbital-free electron density exhibits proper shell structure behavior and is in close agreement with the Kohn-Sham electron density. This study demonstrates that it is possible to obtain self-consistent orbital-free electron densities with proper atomic shell structure from simple one-point approximations for the Pauli potential at local density level.

  1. Gas phase structures and charge localization in small aluminum oxide anions: Infrared photodissociation spectroscopy and electronic structure calculations.

    PubMed

    Song, Xiaowei; Fagiani, Matias R; Gewinner, Sandy; Schöllkopf, Wieland; Asmis, Knut R; Bischoff, Florian A; Berger, Fabian; Sauer, Joachim

    2016-06-28

    We use cryogenic ion trap vibrational spectroscopy in combination with quantum chemical calculations to study the structure of mono- and dialuminum oxide anions. The infrared photodissociation spectra of D2-tagged AlO1-4 (-) and Al2O3-6 (-) are measured in the region from 400 to 1200 cm(-1). Structures are assigned based on a comparison to simulated harmonic and anharmonic IR spectra derived from electronic structure calculations. The monoaluminum anions contain an even number of electrons and exhibit an electronic closed-shell ground state. The Al2O3-6 (-) anions are oxygen-centered radicals. As a result of a delicate balance between localization and delocalization of the unpaired electron, only the BHLYP functional is able to qualitatively describe the observed IR spectra of all species with the exception of AlO3 (-). Terminal Al-O stretching modes are found between 1140 and 960 cm(-1). Superoxo and peroxo stretching modes are found at higher (1120-1010 cm(-1)) and lower energies (850-570 cm(-1)), respectively. Four modes in-between 910 and 530 cm(-1) represent the IR fingerprint of the common structural motif of dialuminum oxide anions, an asymmetric four-member Al-(O)2-Al ring. PMID:27369513

  2. Gas phase structures and charge localization in small aluminum oxide anions: Infrared photodissociation spectroscopy and electronic structure calculations

    NASA Astrophysics Data System (ADS)

    Song, Xiaowei; Fagiani, Matias R.; Gewinner, Sandy; Schöllkopf, Wieland; Asmis, Knut R.; Bischoff, Florian A.; Berger, Fabian; Sauer, Joachim

    2016-06-01

    We use cryogenic ion trap vibrational spectroscopy in combination with quantum chemical calculations to study the structure of mono- and dialuminum oxide anions. The infrared photodissociation spectra of D2-tagged AlO1-4- and Al2O3-6- are measured in the region from 400 to 1200 cm-1. Structures are assigned based on a comparison to simulated harmonic and anharmonic IR spectra derived from electronic structure calculations. The monoaluminum anions contain an even number of electrons and exhibit an electronic closed-shell ground state. The Al2O3-6- anions are oxygen-centered radicals. As a result of a delicate balance between localization and delocalization of the unpaired electron, only the BHLYP functional is able to qualitatively describe the observed IR spectra of all species with the exception of AlO3-. Terminal Al-O stretching modes are found between 1140 and 960 cm-1. Superoxo and peroxo stretching modes are found at higher (1120-1010 cm-1) and lower energies (850-570 cm-1), respectively. Four modes in-between 910 and 530 cm-1 represent the IR fingerprint of the common structural motif of dialuminum oxide anions, an asymmetric four-member Al-(O)2-Al ring.

  3. Bonding in elemental boron: a view from electronic structure calculations using maximally localized Wannier functions

    NASA Astrophysics Data System (ADS)

    Ogitsu, Tadashi; Gygi, Francois; Reed, John; Schwegler, Eric; Galli, Giulia

    2007-03-01

    Boron exhibits the most complex structure of all elemental solids, with more than 300 atoms per unit cell arranged in interconnecting icosahedra, and some crystallographic positions occupied with a probability of less than one. The precise determination of the ground state geometry of boron---the so-called β-boron structure--has been elusive and its electronic and bonding properties have been difficult to rationalize. Using lattice model Monte Carlo optimization techniques and ab-initio simulations, we have shown that a defective, quasi-ordered β solid is the most stable structure at zero as well as finite T. In the absence of partially occupied sites (POS), the perfect β-boron crystal is unstable; the presence of POS lower its internal energy below that of an ordered α-phase, not mere an entropic effect. We present a picture of the intricate and unique bonding in boron based on maximally localized Wannier (MLWF) functions, which indicates that the presence of POS provides a subtle, yet essential spatial balance between electron deficient and fully saturated bonds. This work was performed under the auspices of the U.S. Dept. of Energy at the University of California/ LLNL under contract no. W-7405-Eng-48.

  4. The effect of electron localization on the electronic structure and migration barrier of oxygen vacancies in rutile.

    PubMed

    Zhu, Linggang; Hu, Qing-Miao; Yang, Rui

    2014-02-01

    By applying the on-site Coulomb interaction (Hubbard term U) to the Ti d orbital, the influence of electron localization on the electronic structure as well as the transport of oxygen vacancies (VO) in rutile was investigated. With U = 4.5 eV, the positions of defect states in the bandgap were correctly reproduced. The unbonded electrons generated by taking out one neutral oxygen atom are spin parallel and mainly localized on the Ti atoms near VO, giving rise to a magnetic moment of 2 μB, in agreement with the experimental finding. With regard to the migration barrier of VO, surprisingly, we found that U = 4.5 eV only changed the value of the energy barrier by ±0.15 eV, depending on the diffusion path. The most probable diffusion path (along [110]) is the same as that calculated by using the traditional GGA functional. To validate the GGA + U method itself, a hybrid functional with a smaller supercell was used, and the trend of the more probable diffusion path was not changed. In this regard, the traditional GGA functional might still be reliable in the study of intrinsic-defect transportation in rutile. Analyzing the atomic distortion and density of states of the transition states for different diffusion paths, we found that the anisotropy of the diffusion could be rationalized according to the various atomic relaxations and the different positions of the valence bands relative to the Fermi level of the transition states. PMID:24441015

  5. Structural phase transition and 5f-electrons localization of PuSe explored by ab initio calculations

    SciTech Connect

    Cui Shouxin; Feng Wenxia; Hu Haiquan; Gong Zizheng; Liu Hong

    2010-04-15

    An investigation into the structural phase transformation, electronic and optical properties of PuSe under high pressure was conducted by using the full potential linearized augmented plane wave plus local orbitals (FP-LAPW+lo) method, in the presence and in the absence of spin-orbit coupling (SOC). Our results demonstrate that there exists a structural phase transition from rocksalt (B 1) structure to CsCl-type (B 2) structure at the transition pressure of 36.3 GPa (without SOC) and 51.3 GPa (with SOC). The electronic density of states (DOS) for PuSe show that the f-electrons of Pu are more localized and concentrated in a narrow peak near the Fermi level, which is consistent with the experimental studies. The band structure shows that B 1-PuSe is metallic. A pseudogap appears around the Fermi level of the total density of states of B 1 phase PuSe, which may contribute to its stability. The calculated reflectivity R(omega) shows agreement with the available experimental results. Furthermore, the absorption spectrum, refractive index, extinction coefficient, energy-loss spectrum and dielectric function were calculated. The origin of the spectral peaks was interpreted based on the electronic structures. - Abstract: Graphical Abstract Legend (TOC Figure): 5f-electrons are more localized by the analysis of the density of states (SOC). The origin spectra peaks was interpreted based on electronic structures.

  6. Propagation of localized structures in relativistic magnetized electron-positron plasmas using particle-in-cell simulations

    SciTech Connect

    López, Rodrigo A.; Muñoz, Víctor; Viñas, Adolfo F.; Valdivia, Juan A.

    2015-09-15

    We use a particle-in-cell simulation to study the propagation of localized structures in a magnetized electron-positron plasma with relativistic finite temperature. We use as initial condition for the simulation an envelope soliton solution of the nonlinear Schrödinger equation, derived from the relativistic two fluid equations in the strongly magnetized limit. This envelope soliton turns out not to be a stable solution for the simulation and splits in two localized structures propagating in opposite directions. However, these two localized structures exhibit a soliton-like behavior, as they keep their profile after they collide with each other due to the periodic boundary conditions. We also observe the formation of localized structures in the evolution of a spatially uniform circularly polarized Alfvén wave. In both cases, the localized structures propagate with an amplitude independent velocity.

  7. Role of non-local exchange in the electronic structure of correlated oxides

    NASA Astrophysics Data System (ADS)

    Iori, Federico; Gatti, Matteo; Rubio Secades, Angel

    Transition-metal oxides (TMO) with partially filled d or f shells are a prototype of correlated materials. They exhibit very interesting properties, like metal-insulator phase transitions (MIT). In this work we consider several TMO insulators in which Kohn-Sham LDA band structures are metallic: VO2, V2O3, Ti2O3, LaTiO3 and YTiO3. In the past, this failure of LDA has been explained in terms of its inadequacy to capture the strong interactions taking place between correlated electrons. In the spirit of the Hubbard model, possible corrections to improve onsite correlation are the LDA +U and LDA +DMFT approaches. Here we make use of the HSE06 hybrid functional. We show that, without invoking strong-correlation effects, the contribution of the non-local Fock exchange is essential to correct the LDA results, by curing its delocalization error. In fact, HSE06 provides insulating band structures and correctly describes the MIT in all the considered compounds. We further discuss the advantages and the limitations of the HSE06 hybrid functional in correlated TMO

  8. Local atomic and electronic structure in LaMnO{sub 3} across the orbital ordering transition

    SciTech Connect

    Souza, Raquel A.; Souza-Neto, Narcizo M.; Ramos, Aline Y.; Tolentino, Helio C.N.; Granado, Eduardo

    2004-12-01

    The local atomic disorder and electronic structure in the environment of manganese atoms in LaMnO{sub 3} has been studied by x-ray absorption spectroscopy over a temperature range (300-870 K) covering the orbital ordering transition ({approx}710 K). The Mn-O distance splitting into short and long bonds (1.95 and 2.15 A) is kept across the transition temperature, so that the MnO{sub 6} octahedra remain locally Jahn-Teller distorted. Discontinuities in the Mn local structure are identified in the extended x-ray fine structure spectra at this temperature, associated with a reduction of the disorder in the superexchange angle and to the removal of the anisotropy in the radial disorder within the coordination shell. Subtle changes in the electronic local structure also take place at the Mn site at the transition temperature. The near-edge spectra show a small drop of the Mn 4p hole count and a small enhancement in the pre-edge structures at the transition temperature. These features are associated with an increase of the covalence of the Mn-O bonds. Our results shed light on the local electronic and structural phenomena in a model of order-disorder transition, where the cooperative distortion is overcome by the thermal disorder.

  9. Local electronic structure and photoelectrochemical activity of partial chemically etched Ti-doped hematite

    NASA Astrophysics Data System (ADS)

    Rioult, Maxime; Belkhou, Rachid; Magnan, Hélène; Stanescu, Dana; Stanescu, Stefan; Maccherozzi, Francesco; Rountree, Cindy; Barbier, Antoine

    2015-11-01

    The direct conversion of solar light into chemical energy or fuel through photoelectrochemical water splitting is promising as a clean hydrogen production solution. Ti-doped hematite (Ti:α-Fe2O3) is a potential key photoanode material, which despite its optimal band gap, excellent chemical stability, abundance, non-toxicity and low cost, still has to be improved. Here we give evidence of a drastic improvement of the water splitting performances of Ti-doped hematite photoanodes upon a HCl wet-etching. In addition to the topography investigation by atomic force microscopy, a detailed determination of the local electronic structure has been carried out in order to understand the phenomenon and to provide new insights in the understanding of solar water splitting. Using synchrotron radiation based spectromicroscopy (X-PEEM), we investigated the X-ray absorption spectral features at the L3 Fe edge of the as grown surface and of the wet-etched surface on the very same sample thanks to patterning. We show that HCl wet etching leads to substantial surface modifications of the oxide layer including increased roughness and chemical reduction (presence of Fe2 +) without changing the band gap. We demonstrate that these changes are profitable and correlated to the drastic changes of the photocatalytic activity.

  10. Edge states and local electronic structure around an adsorbed impurity in a topological superconductor

    NASA Astrophysics Data System (ADS)

    Tai, Yuan-Yen; Choi, Hongchul; Ahmed, Towfiq; Ting, C. S.; Zhu, Jian-Xin

    2015-11-01

    Recently, topological superconducting states have attracted much interest. In this paper, we consider a topological superconductor with Z2 topological mirror order [Y.-Y. Tai et al., Phys. Rev. B 91, 041111(R) (2015), 10.1103/PhysRevB.91.041111] and s±-wave superconducting pairing symmetry, within a two-orbital model originally designed for iron-based superconductivity [Y.-Y. Tai et al., Europhys. Lett. 103, 67001 (2013), 10.1209/0295-5075/103/67001]. We predict the existence of gapless edge states. We also study the local electronic structure around an adsorbed interstitial magnetic impurity in the system, and find the existence of low-energy in-gap bound states even with a weak spin polarization on the impurity. We also discuss the relevance of our results to a recent scanning tunneling microscopy experiment on a Fe(Te,Se) compound with an adsorbed Fe impurity [J.-X. Yin et al., Nat. Phys. 11, 543 (2015), 10.1038/nphys3371], for which our density functional calculations show the Fe impurity is spin polarized.

  11. Three-Dimensional Imaging of the Local Structure of Materials at Atomic Resolution by Electron Tomography

    NASA Astrophysics Data System (ADS)

    Zhu, Chun

    Electron tomography was originally developed in 1968, and has been primarily applied to determine the three-dimensional (3D) structure of biological systems. In the last decade, the application of electron tomography in materials science and nanoscience has revived due to the utilization of scanning transmission electron microscopy (STEM) in the high-angle annular dark-field (HAADF) mode, and a highest resolution of ˜1 nm3 has been achieved. However, improving the resolution from ˜1 nm 3 to the atomic level remains a challenging task, which requires new tomographic reconstruction algorithms, better projection alignment methods, state-of-the-art STEM instruments, and more accurate data-acquisition procedures. In this thesis, important progress has been made in all these four areas. First, a novel tomographic method, termed equally sloped tomography (EST), was developed and allows the 3D image reconstruction of tilt series with a limited number projections and a "missing wedge" (i.e. specimens cannot usually be tilted beyond +/-70°). Second, an alignment method which can be used to align the projections of a tilt series at atomic-level resolution was developed based on center of mass. Finally, by using a Titan 80-300 STEM instrument at the California NanoSystems Institute, UCLA, more accurate data acquisition procedures were developed and a number of tomographic tilt series of atomic resolution projections from different nanoparticles have been obtained. With all these combinations, the 3D structure of a 10 nm gold nanoparticle was determined at 2.4 A resolution, the highest resolution ever achieved in any general tomography method. More recently, this novel electron tomography method has been applied to observe nearly all the atoms in a Pt nanoparticle, and imaged for the first time the 3D core structure of edge and screw dislocations at atomic resolution. Furthermore, through numerical simulations the feasibility of determining the 3D atomic structure of

  12. TiO2 nanotube arrays for photocatalysis: Effects of crystallinity, local order, and electronic structure

    SciTech Connect

    Liu, Jing; Hosseinpour, Pegah M.; Luo, Si; Heiman, Don; Menon, Latika; Arena, Dario A.; Lewis, Laura H.

    2014-11-19

    To furnish insight into correlations of electronic and local structure and photoactivity, arrays of short and long TiO₂ nanotubes were synthesized by electrochemical anodization of Ti foil, followed by thermal treatment in O₂ (oxidizing), Ar (inert), and H₂ (reducing) environments. The physical and electronic structures of these nanotubes were probed with x-ray diffraction, scanning electron microscopy, and synchrotron-based x-ray absorption spectroscopy, and correlated with their photocatalytic properties. The photocatalytic activity of the nanotubes was evaluated by monitoring the degradation of methyl orange under UV-VIS light irradiation. Results show that upon annealing at 350 °C all as-anodized amorphous TiO₂ nanotube samples partially transform to the anatase structure, with variations in the degree of crystallinity and in the concentration of local defects near the nanotubes' surface (~5 nm) depending on the annealing conditions. Degradation of methyl orange was not detectable for the as-anodized TiO₂ nanotubes regardless of their length. The annealed long nanotubes demonstrated detectable catalytic activity, which was more significant with the H₂-annealed nanotubes than with the Ar- and O₂-annealed nanotube samples. This enhanced photocatalytic response of the H₂-annealed long nanotubes relative to the other samples is positively correlated with the presence of a larger concentration of lattice defects (such as Ti3+ and anticipated oxygen vacancies) and a slightly lower degree of crystallinity near the nanotube surface. These physical and electronic structural attributes impact the efficacy of visible light absorption; moreover, the increased concentration of surface defects is postulated to promote the generation of hydroxyl radicals and thus accelerate the photodegradation of the methyl orange. The information obtained from this study provides unique insight into the role of the near-surface electronic and defect structure

  13. Ion Streaming Instabilities in Pair Ion Plasma and Localized Structure with Non-Thermal Electrons

    NASA Astrophysics Data System (ADS)

    Nasir Khattak, M.; Mushtaq, A.; Qamar, A.

    2015-12-01

    Pair ion plasma with a fraction of non-thermal electrons is considered. We investigate the effects of the streaming motion of ions on linear and nonlinear properties of unmagnetized, collisionless plasma by using the fluid model. A dispersion relation is derived, and the growth rate of streaming instabilities with effect of streaming motion of ions and non-thermal electrons is calculated. A qausi-potential approach is adopted to study the characteristics of ion acoustic solitons. An energy integral equation involving Sagdeev potential is derived during this process. The presence of the streaming term in the energy integral equation affects the structure of the solitary waves significantly along with non-thermal electrons. Possible application of the work to the space and laboratory plasmas are highlighted.

  14. Global and local health monitoring of civil structures using smart ferroelectric sensors and electronically steerable antennas

    NASA Astrophysics Data System (ADS)

    Varadan, Vijay K.; Varadan, Vasundara V.

    1994-09-01

    In this paper, the global and local health monitoring of civil structures using RF antennas and ferroelectric sensors is presented. The sensors are fabricated with interdigital transducers printed on a piezoelectric polymer or ceramic type film. They in turn are mounted onto an ultra thin Penn State's novel RF antenna. The wave form measurements may be monitored at a remote location via the antennas in the sensors and an outside antenna.

  15. Exciton Localization in Extended π-Electron Systems: Comparison of Linear and Cyclic Structures.

    PubMed

    Thiessen, Alexander; Würsch, Dominik; Jester, Stefan-S; Aggarwal, A Vikas; Idelson, Alissa; Bange, Sebastian; Vogelsang, Jan; Höger, Sigurd; Lupton, John M

    2015-07-30

    We employ five π-conjugated model materials of different molecular shape-oligomers and cyclic structures-to investigate the extent of exciton self-trapping and torsional motion of the molecular framework following optical excitation. Our studies combine steady state and transient fluorescence spectroscopy in the ensemble with measurements of polarization anisotropy on single molecules, supported by Monte Carlo simulations. The dimer exhibits a significant spectral red shift within ∼100 ps after photoexcitation which is attributed to torsional relaxation. This relaxation mechanism is inhibited in the structurally rigid macrocyclic analogue. However, both systems show a high degree of exciton localization but with very different consequences: while, in the macrocycle, the exciton localizes randomly on different parts of the ring, scrambling polarization memory, in the dimer, localization leads to a deterministic exciton position with luminescence characteristics of a dipole. Monte Carlo simulations allow us to quantify the structural difference between the emitting and absorbing units of the π-conjugated system in terms of disorder parameters. PMID:26035080

  16. Plane-wave based electronic structure calculations for correlated materials using dynamical mean-field theory and projected local orbitals

    NASA Astrophysics Data System (ADS)

    Amadon, B.; Lechermann, F.; Georges, A.; Jollet, F.; Wehling, T. O.; Lichtenstein, A. I.

    2008-05-01

    The description of realistic strongly correlated systems has recently advanced through the combination of density functional theory in the local density approximation (LDA) and dynamical mean field theory (DMFT). This LDA+DMFT method is able to treat both strongly correlated insulators and metals. Several interfaces between LDA and DMFT have been used, such as ( Nth order) linear muffin-tin orbitals or maximally localized Wannier functions. Such schemes are, however, either complex in use or additional simplifications are often performed (i.e., the atomic sphere approximation). We present an alternative implementation of LDA+DMFT , which keeps the precision of the Wannier implementation, but which is lighter. It relies on the projection of localized orbitals onto a restricted set of Kohn-Sham states to define the correlated subspace. The method is implemented within the projector augmented wave and within the mixed-basis pseudopotential frameworks. This opens the way to electronic structure calculations within LDA+DMFT for more complex structures with the precision of an all-electron method. We present an application to two correlated systems, namely, SrVO3 and β -NiS (a charge-transfer material), including ligand states in the basis set. The results are compared to calculations done with maximally localized Wannier functions, and the physical features appearing in the orbitally resolved spectral functions are discussed.

  17. Fermi orbital self-interaction corrected electronic structure of molecules beyond local density approximation

    NASA Astrophysics Data System (ADS)

    Hahn, Torsten; Liebing, Simon; Kortus, Jens; Pederson, Mark

    The correction of the self-interaction error that is inherent to all standard density functional theory (DFT) calculations is an object of increasing interest. We present our results on the application of the recently developed Fermi-orbital based approach for the self-interaction correction (FO-SIC) to a set of different molecular systems. Our study covers systems ranging from simple diatomic to large organic molecules. Our focus lies on the direct estimation of the ionization potential from orbital eigenvalues and on the ordering of electronic levels in metal-organic molecules. Further, we show that the Fermi orbital positions in structurally similar molecules appear to be transferable. Support by DFG FOR1154 is greatly acknowledged.

  18. Probing the structural and dynamical properties of liquid water with models including non-local electron correlation

    NASA Astrophysics Data System (ADS)

    Del Ben, Mauro; Hutter, Jürg; VandeVondele, Joost

    2015-08-01

    Water is a ubiquitous liquid that displays a wide range of anomalous properties and has a delicate structure that challenges experiment and simulation alike. The various intermolecular interactions that play an important role, such as repulsion, polarization, hydrogen bonding, and van der Waals interactions, are often difficult to reproduce faithfully in atomistic models. Here, electronic structure theories including all these interactions at equal footing, which requires the inclusion of non-local electron correlation, are used to describe structure and dynamics of bulk liquid water. Isobaric-isothermal (NpT) ensemble simulations based on the Random Phase Approximation (RPA) yield excellent density (0.994 g/ml) and fair radial distribution functions, while various other density functional approximations produce scattered results (0.8-1.2 g/ml). Molecular dynamics simulation in the microcanonical (NVE) ensemble based on Møller-Plesset perturbation theory (MP2) yields dynamical properties in the condensed phase, namely, the infrared spectrum and diffusion constant. At the MP2 and RPA levels of theory, ice is correctly predicted to float on water, resolving one of the anomalies as resulting from a delicate balance between van der Waals and hydrogen bonding interactions. For several properties, obtaining quantitative agreement with experiment requires correction for nuclear quantum effects (NQEs), highlighting their importance, for structure, dynamics, and electronic properties. A computed NQE shift of 0.6 eV for the band gap and absorption spectrum illustrates the latter. Giving access to both structure and dynamics of condensed phase systems, non-local electron correlation will increasingly be used to study systems where weak interactions are of paramount importance.

  19. Probing the structural and dynamical properties of liquid water with models including non-local electron correlation.

    PubMed

    Del Ben, Mauro; Hutter, Jürg; VandeVondele, Joost

    2015-08-01

    Water is a ubiquitous liquid that displays a wide range of anomalous properties and has a delicate structure that challenges experiment and simulation alike. The various intermolecular interactions that play an important role, such as repulsion, polarization, hydrogen bonding, and van der Waals interactions, are often difficult to reproduce faithfully in atomistic models. Here, electronic structure theories including all these interactions at equal footing, which requires the inclusion of non-local electron correlation, are used to describe structure and dynamics of bulk liquid water. Isobaric-isothermal (NpT) ensemble simulations based on the Random Phase Approximation (RPA) yield excellent density (0.994 g/ml) and fair radial distribution functions, while various other density functional approximations produce scattered results (0.8-1.2 g/ml). Molecular dynamics simulation in the microcanonical (NVE) ensemble based on Møller-Plesset perturbation theory (MP2) yields dynamical properties in the condensed phase, namely, the infrared spectrum and diffusion constant. At the MP2 and RPA levels of theory, ice is correctly predicted to float on water, resolving one of the anomalies as resulting from a delicate balance between van der Waals and hydrogen bonding interactions. For several properties, obtaining quantitative agreement with experiment requires correction for nuclear quantum effects (NQEs), highlighting their importance, for structure, dynamics, and electronic properties. A computed NQE shift of 0.6 eV for the band gap and absorption spectrum illustrates the latter. Giving access to both structure and dynamics of condensed phase systems, non-local electron correlation will increasingly be used to study systems where weak interactions are of paramount importance. PMID:26254660

  20. Probing the structural and dynamical properties of liquid water with models including non-local electron correlation

    SciTech Connect

    Del Ben, Mauro Hutter, Jürg; VandeVondele, Joost

    2015-08-07

    Water is a ubiquitous liquid that displays a wide range of anomalous properties and has a delicate structure that challenges experiment and simulation alike. The various intermolecular interactions that play an important role, such as repulsion, polarization, hydrogen bonding, and van der Waals interactions, are often difficult to reproduce faithfully in atomistic models. Here, electronic structure theories including all these interactions at equal footing, which requires the inclusion of non-local electron correlation, are used to describe structure and dynamics of bulk liquid water. Isobaric-isothermal (NpT) ensemble simulations based on the Random Phase Approximation (RPA) yield excellent density (0.994 g/ml) and fair radial distribution functions, while various other density functional approximations produce scattered results (0.8-1.2 g/ml). Molecular dynamics simulation in the microcanonical (NVE) ensemble based on Møller-Plesset perturbation theory (MP2) yields dynamical properties in the condensed phase, namely, the infrared spectrum and diffusion constant. At the MP2 and RPA levels of theory, ice is correctly predicted to float on water, resolving one of the anomalies as resulting from a delicate balance between van der Waals and hydrogen bonding interactions. For several properties, obtaining quantitative agreement with experiment requires correction for nuclear quantum effects (NQEs), highlighting their importance, for structure, dynamics, and electronic properties. A computed NQE shift of 0.6 eV for the band gap and absorption spectrum illustrates the latter. Giving access to both structure and dynamics of condensed phase systems, non-local electron correlation will increasingly be used to study systems where weak interactions are of paramount importance.

  1. TiO{sub 2} nanotube arrays for photocatalysis: Effects of crystallinity, local order, and electronic structure

    SciTech Connect

    Liu, Jing; Hosseinpour, Pegah M.; Lewis, Laura H.; Luo, Si; Heiman, Don; Menon, Latika; Arena, Dario A.

    2015-03-15

    To furnish insight into correlations of electronic and local structure and photoactivity, arrays of short and long TiO{sub 2} nanotubes were synthesized by electrochemical anodization of Ti foil, followed by thermal treatment in O{sub 2} (oxidizing), Ar (inert), and H{sub 2} (reducing) environments. The physical and electronic structures of these nanotubes were probed with x-ray diffraction, scanning electron microscopy, and synchrotron-based x-ray absorption spectroscopy, and correlated with their photocatalytic properties. The photocatalytic activity of the nanotubes was evaluated by monitoring the degradation of methyl orange under UV-VIS light irradiation. Results show that upon annealing at 350 °C all as-anodized amorphous TiO{sub 2} nanotube samples partially transform to the anatase structure, with variations in the degree of crystallinity and in the concentration of local defects near the nanotubes' surface (∼5 nm) depending on the annealing conditions. Degradation of methyl orange was not detectable for the as-anodized TiO{sub 2} nanotubes regardless of their length. However, the annealed long nanotubes demonstrated detectable catalytic activity, which was more significant with the H{sub 2}-annealed nanotubes than with the Ar- and O{sub 2}-annealed nanotube samples. This enhanced photocatalytic response of the H{sub 2}-annealed long nanotubes relative to the other samples is positively correlated with the presence of a larger concentration of lattice defects (such as Ti{sup 3+} and anticipated oxygen vacancies) and a slightly lower degree of crystallinity near the nanotube surface. These physical and electronic structural attributes impact the efficacy of visible light absorption; moreover, the increased concentration of surface defects is postulated to promote the generation of hydroxyl radicals and thus accelerate the photodegradation of the methyl orange. The information obtained from this study provides unique insight into the role of the near

  2. The Local Electronic Structure of Dicarba-closo-dodecaboranes C2B10H12

    SciTech Connect

    Fister, Timothy T.; Vila, Fernando D.; Seidler, Gerald T.; Svec, Lukas; Linehan, John C.; Cross, Julie O.

    2008-01-16

    We report nonresonant inelastic x-ray scattering (NRIXS) measurement of core-shell excitations from both B 1s and C 1s initial states in all three isomers of the dicarba-closo-dodecaboranes C2B10H12. First, this data yields an experimental determination of the angular-momentum-projected final local density of states (l-DOS). We find low-energy resonances with distinctive local s- or p-type character, providing a more complete experimental characterization of bond hybridization than is available from dipole-transition limited techniques, such as x-ray absorption spectroscopies. This analysis is supported by independent density functional theory and real-space full multiple scattering calculation of the l-DOS which yield a clear distinction between tangential and radial contributions. Second, we investigate the isomer-sensitivity of the NRIXS signal, and compare and contrast these results with prior electron energy loss spectroscopy measurements. This work establishes NRIXS as a valuable tool for borane chemistry, not only for the unique spectroscopic capabilities of the technique, but also through its compatibility with future studies in solution or in high pressure environments. In addition, this work also establishes the real-space full multiple scattering approach as a useful alternative to traditional approaches for the excited states calculations for aromatic polyhedral boranes and related systems. This research was supported by DOE, Basic Energy Science, Office of Science, Contract Nos. DE-FGE03-97ER45628 and W-31-109-ENG-38, ONR Grant No. N00014-05-1-0843, Grant DE-FG03-97ER5623, NIH NCRR BTP Grant RR-01209, the Leonard X. Bosack and Bette M. Kruger Foundation, the Hydrogen Fuel Cell Initiative of DOE Office of Basic Energy Sciences, and the Summer Research Institute Program at the Pacific Northwest National Lab. Battelle operates the Pacific Northwest National Lab for DOE. The operation of Sector 20 PNC-CAT/XOR is supported by DOE Basic Energy Science

  3. Local structural distortion and electronic modifications in PrNiO3 across the metal-insulator transition

    SciTech Connect

    Piamonteze, C.; Tolentino, H.C.N.; Ramos, A.Y.; Massa, N. E.; Alonso, J.A.; Martinez-Lope, M.J.; Casais, M.T.

    2003-01-24

    Local electronic and structural properties of PrNiO3 perovskite were studied by means of X-ray Absorption Spectroscopy at Ni K and L edges. The EXAFS results at Ni K edge show a structural transition from three different Ni-O bond-lengths at the insulating phase to two Ni-O bond-lengths above TMI. These results were interpreted as being due to a transition from a structure with two different Ni sites at the insulating phase to one distorted Ni site at the metallic phase. The Ni L edge spectra show a remarkable difference between the spectra measured at the insulating and metallic phases that indicates a decreasing degree of hybridization between Ni3d and O2p bands from the metallic to the insulating phase.

  4. Non-local exchange correlation functionals impact on the structural, electronic and optical properties of III-V arsenides

    NASA Astrophysics Data System (ADS)

    Najwa Anua, N.; Ahmed, R.; Shaari, A.; Saeed, M. A.; Haq, Bakhtiar Ul; Goumri-Said, Souraya

    2013-10-01

    Exchange correlation (XC) energy functionals play a vital role in the efficiency of density functional theory (DFT) calculations, more soundly in the calculation of fundamental electronic energy bandgap. In the present DFT study of III-arsenides, we investigate the implications of XC-energy functional and corresponding potential on the structural, electronic and optical properties of XAs (X = B, Al, Ga, In). Firstly we report and discuss the optimized structural lattice parameters and the band gap calculations performed within different non-local XC functionals as implemented in the DFT-packages: WIEN2k, CASTEP and SIESTA. These packages are representative of the available code in ab initio studies. We employed the LDA, GGA-PBE, GGA-WC and mBJ-LDA using WIEN2k. In CASTEP, we employed the hybrid functional, sX-LDA. Furthermore LDA, GGA-PBE and meta-GGA were employed using SIESTA code. Our results point to GGA-WC as a more appropriate approximation for the calculations of structural parameters. However our electronic bandstructure calculations at the level of mBJ-LDA potential show considerable improvements over the other XC functionals, even the sX-LDA hybrid functional. We report also the optical properties within mBJ potential, which show a nice agreement with the experimental measurements in addition to other theoretical results.

  5. On the local electronic and atomic structure of Ce1-xPrxO2-δ epitaxial films on Si

    NASA Astrophysics Data System (ADS)

    Niu, Gang; Schubert, Markus Andreas; d'Acapito, Francesco; Zoellner, Marvin Hartwig; Schroeder, Thomas; Boscherini, Federico

    2014-09-01

    The local electronic and atomic structure of (111)-oriented, single crystalline mixed Ce1-xPrxO2-δ (x = 0, 0.1 and 0.6) epitaxial thin films on silicon substrates have been investigated in view of engineering redox properties of complex oxide films. Non-destructive X-ray absorption near edge structure reveals that Pr shows only +3 valence and Ce shows only nominal +4 valence in mixed oxides. Extended x-ray absorption fine structure (EXAFS) studies were performed at K edges of Ce and Pr using a specially designed monochromator system for high energy measurements. They demonstrate that the fluorite lattice of ceria (CeO2) is almost not perturbed for x = 0.1 sample, while higher Pr concentration (x = 0.6) not only generates a higher disorder level (thus more disordered oxygen) but also causes a significant reduction of Ce-O interatomic distances. The valence states of the cations were also examined by techniques operating in highly reducing environments: scanning transmission electron microscopy-electron energy loss spectroscopy and X-ray photoemission spectroscopy; in these reducing environments, evidence for the presence of Ce3+ was clearly found for the higher Pr concentration. Thus, the introduction of Pr3+ into CeO2 strongly enhances the oxygen exchange properties of CeO2. This improved oxygen mobility properties of CeO2 are attributed to the lattice disorder induced by Pr mixing in the CeO2 fluorite lattice, as demonstrated by EXAFS measurements. Thus, a comprehensive picture of the modifications of the atomic and electronic structure of Ce1-xPrxO2-δ epitaxial films and their relation is obtained.

  6. Extended electron energy loss fine structure simulation of the local boron environment in sodium aluminoborosilicate glasses containing gadolinium

    SciTech Connect

    Qian, Morris; Li, Hong; Li, Liyu ); Strachan, Denis M. )

    2003-10-15

    Gadolinium can be dissolved in sodium-alumino-borosilicate glasses up to 47 wt% in a baseline borosilicate glass (mol%) 20 B2O3, 5 Al2O3, 60 SiO2,and 20 Na2O. Understanding of Gd dissolution in borosilicate melts is important in glass formulation optimization. Electron energy loss fine structure (ELFS) spectroscopy is chosen, which provides well resolved local atomic structure information for both amorphous and crystalline materials with high sensitivity to low Z elements such as Al, B, Na, O, and Si where the x-ray absorption fine structure (XAFS) technique faces experimental difficulty. In this study, we report our results of boron K-edge ELFS study. Two borosilicate glass samples with 30 and 47 mass% Gd2O3, B20Gd30 and B20Gd47were chosen for B K-edge ELFS study. EEL spectra were acquired on a Philips 430 TEM equipped with Gatan PEELS system 666 and EL/P 2.1 software with Custom function AcqLong. The ELFS data analysis was performed using UWELFS, UWXAFS and FEFF software. From our Gd solubility study, the local structure of Gd in the borate environment possibly resembles double chain structure found in crystalline Gd(BO2)3 as proposed by Chakraborty et al. The B/Gd ratio's in both glasses are smaller then 3, which means the excess Gd atoms in the Si-sites would be 17 and 60 mol% of the total Gd atoms, respectively according to the model, yet the local environment of borate sites saturated with Gd should be remained. To verity above hypothesis, the double chain structure model was applied to fit boron K-edge. The model was shown to well fit experimental boron K-edge EELS spectra for both glasses with some degree of distance distortion which is understandable in amorphous structure. Therefore, it is very likely that Gd stabilized in borate sites has a local structure resembling the double chain Gd(BO2)3 structure as proposed by our solubility study and literature.

  7. Characterization of the electronic structure of crystalline compounds through their localized Wannier functions

    NASA Astrophysics Data System (ADS)

    Zicovich-Wilson, Claudio M.; Bert, Alberto; Roetti, Carla; Dovesi, Roberto; Saunders, Victor R.

    2002-01-01

    The crystalline orbitals of seven oxygen containing compounds with increasing degree of covalent character (MgO, MnO, ZnO, Al2O3, SiO2, AlPO4, and CaSO4) are localized according to a Wannier-Boys mixed scheme recently implemented. The resulting Wannier functions are analyzed in terms of various indices (centroids positions, second-order central moment tensor, its eigenvalues and principal axes, Mulliken population analysis, and atomic localization indices). Systematic trends are observed along the series.

  8. Electron acceleration at localized wave structures in the solar corona (German Title: Elektronenbeschleunigung an lokalen Wellenstrukturen in der Sonnenkorona)

    NASA Astrophysics Data System (ADS)

    Miteva, Rositsa Stoycheva

    2007-07-01

    Our dynamic Sun manifests its activity by different phenomena: from the 11-year cyclic sunspot pattern to the unpredictable and violent explosions in the case of solar flares. During flares, a huge amount of the stored magnetic energy is suddenly released and a substantial part of this energy is carried by the energetic electrons, considered to be the source of the nonthermal radio and X-ray radiation. One of the most important and still open question in solar physics is how the electrons are accelerated up to high energies within (the observed in the radio emission) short time scales. Because the acceleration site is extremely small in spatial extent as well (compared to the solar radius), the electron acceleration is regarded as a local process. The search for localized wave structures in the solar corona that are able to accelerate electrons together with the theoretical and numerical description of the conditions and requirements for this process, is the aim of the dissertation. Two models of electron acceleration in the solar corona are proposed in the dissertation: I. Electron acceleration due to the solar jet interaction with the background coronal plasma (the jet--plasma interaction) A jet is formed when the newly reconnected and highly curved magnetic field lines are relaxed by shooting plasma away from the reconnection site. Such jets, as observed in soft X-rays with the Yohkoh satellite, are spatially and temporally associated with beams of nonthermal electrons (in terms of the so-called type III metric radio bursts) propagating through the corona. A model that attempts to give an explanation for such observational facts is developed here. Initially, the interaction of such jets with the background plasma leads to an (ion-acoustic) instability associated with growing of electrostatic fluctuations in time for certain range of the jet initial velocity. During this process, any test electron that happen to feel this electrostatic wave field is drawn to co

  9. Electron acceleration at localized wave structures in the solar corona (German Title: Elektronenbeschleunigung an lokalen Wellenstrukturen in der Sonnenkorona)

    NASA Astrophysics Data System (ADS)

    Miteva, Rositsa Stoycheva

    2007-07-01

    Our dynamic Sun manifests its activity by different phenomena: from the 11-year cyclic sunspot pattern to the unpredictable and violent explosions in the case of solar flares. During flares, a huge amount of the stored magnetic energy is suddenly released and a substantial part of this energy is carried by the energetic electrons, considered to be the source of the nonthermal radio and X-ray radiation. One of the most important and still open question in solar physics is how the electrons are accelerated up to high energies within (the observed in the radio emission) short time scales. Because the acceleration site is extremely small in spatial extent as well (compared to the solar radius), the electron acceleration is regarded as a local process. The search for localized wave structures in the solar corona that are able to accelerate electrons together with the theoretical and numerical description of the conditions and requirements for this process, is the aim of the dissertation. Two models of electron acceleration in the solar corona are proposed in the dissertation: I. Electron acceleration due to the solar jet interaction with the background coronal plasma (the jet--plasma interaction) A jet is formed when the newly reconnected and highly curved magnetic field lines are relaxed by shooting plasma away from the reconnection site. Such jets, as observed in soft X-rays with the Yohkoh satellite, are spatially and temporally associated with beams of nonthermal electrons (in terms of the so-called type III metric radio bursts) propagating through the corona. A model that attempts to give an explanation for such observational facts is developed here. Initially, the interaction of such jets with the background plasma leads to an (ion-acoustic) instability associated with growing of electrostatic fluctuations in time for certain range of the jet initial velocity. During this process, any test electron that happen to feel this electrostatic wave field is drawn to co

  10. Dependence of Localized Electronic Structure on Ligand Configuration in the [2Fe] Hydrogenase Catalytic Core^*

    NASA Astrophysics Data System (ADS)

    Chang, Christopher H.; Kim, Kwiseon

    2007-03-01

    The [FeFe] hydrogenase enzyme is found in a variety of organisms, including Archaea, Eubacteria, and green algae^1,2, and crystallographically determined atomic position data is available for two examples. The biologically unusual catalytic H-cluster, responsible for proton reduction to H2 in vivo, is conserved in the known structures and includes two bis-thiolato bridged iron ions with extensive cyano- and carbonyl ligation. To address the configurational specificity of the diatomic ligand ligation, density functional theoretical calculations were done on [2Fe] core models of the active center, with varying CO and CN^- ligation patterns. Bonding in each complex has been characterized within the Natural Bond Orbital formalism. The effect of ligand configuration on bonding and charge distribution as well as Kohn-Sham orbital structure will be presented. [1] M. Forestier, P. King, L. Zhang, M. Posewitz, S. Schwarzer, T. Happe, M.L. Ghirardi, and M. Seibert, Eur. J. Biochem. 270, 2750 (2003). [2] Posewitz, M.C., P.W. King, S.L. Smolinski, R.D. Smith, II, A.R. Ginley, M.L. Ghirardi, and M. Seibert, Biochem. Soc. Trans. 33, 102 (2005). ^*This work was supported by the US DOE-SC-BES Hydrogen Fuels Initiative, and done in collaboration with the NREL Chemical and Biosciences Center.

  11. Fermi orbital self-interaction corrected electronic structure of molecules beyond local density approximation

    NASA Astrophysics Data System (ADS)

    Hahn, T.; Liebing, S.; Kortus, J.; Pederson, Mark R.

    2015-12-01

    The correction of the self-interaction error that is inherent to all standard density functional theory calculations is an object of increasing interest. In this article, we apply the very recently developed Fermi-orbital based approach for the self-interaction correction [M. R. Pederson et al., J. Chem. Phys. 140, 121103 (2014) and M. R. Pederson, J. Chem. Phys. 142, 064112 (2015)] to a set of different molecular systems. Our study covers systems ranging from simple diatomic to large organic molecules. We focus our analysis on the direct estimation of the ionization potential from orbital eigenvalues. Further, we show that the Fermi orbital positions in structurally similar molecules appear to be transferable.

  12. Fermi orbital self-interaction corrected electronic structure of molecules beyond local density approximation

    SciTech Connect

    Hahn, T. Liebing, S.; Kortus, J.; Pederson, Mark R.

    2015-12-14

    The correction of the self-interaction error that is inherent to all standard density functional theory calculations is an object of increasing interest. In this article, we apply the very recently developed Fermi-orbital based approach for the self-interaction correction [M. R. Pederson et al., J. Chem. Phys. 140, 121103 (2014) and M. R. Pederson, J. Chem. Phys. 142, 064112 (2015)] to a set of different molecular systems. Our study covers systems ranging from simple diatomic to large organic molecules. We focus our analysis on the direct estimation of the ionization potential from orbital eigenvalues. Further, we show that the Fermi orbital positions in structurally similar molecules appear to be transferable.

  13. Extended electron energy loss fine structure simulation of the local boron environment in sodium aluminoborosilicate glasses containing gadolinium

    SciTech Connect

    Qian, Morris; Li, Hong; Li, Liyu ); Strachan, Denis M. )

    2003-12-01

    Phase separation in sodium-aluminoborosilicate glasses was systematically studied as a function of Gd2O3 concentration with transmission electron microscopy (TEM), energy dispersive x-ray spectroscopy (EDS), and electron energy loss spectroscopy (EELS) methods. Gadolinium-induced phase separation in the three systems can be consistently explained by proposing that Gd cations partition to the borate-rich environments and subsequent agglomeration of the Gd-borate moieties, or short-range ordered structural groups, in the glass. Agglomeration of the Gd-borate rich environments is further discussed within the context of excess metal oxides,[Na2O]ex or[Al2O3]ex=|Na2O - Al2O3|, and excess B2O3,[B2O3]ex, available for incorporating Gd cations. Results showed that agglomeration of the Gd-borate rich environments occurred at a much lower Gd2O3 concentration in the glass without[Na2O]ex or[Al2O3]ex and at a significantly higher Gd2O3 concentration in the glass with either[Na2O]ex or[Al2O3]ex. Assuming 1BO4 : 1Gd : 2BO3 (based on literature-reported Gd-metaborate structure) as a local Gd-borate environment in glass, we introduced the saturation index of boron, SI[B]= Gd2O3/(1/3[B2O3]ex), to examine the glass susceptibility to Gd-induced phase separation for all three alkali-aluminoborosilicate systems. While our results have provided some insight to the glass structure, they also provide insight to the mechanism by which the metal oxide is dissolved into the melt. This appears to occur predominantly through boron complexation of the metal oxide.

  14. Electron Structure of Francium

    NASA Astrophysics Data System (ADS)

    Koufos, Alexander

    2012-02-01

    This talk presents the first calculations of the electronic structure of francium for the bcc, fcc and hcp structures, using the Augmented Plane Wave (APW) method in its muffin-tin and linearized general potential forms. Both the Local Density Approximation (LDA) and Generalized Gradient Approximation (GGA), were used to calculate the electronic structure and total energy of francium (Fr). The GGA and LDA both found the total energy of the hcp structure slightly below that of the fcc and bcc structure, respectively. This is in agreement with similar results for the other alkali metals using the same methodology. The equilibrium lattice constant, bulk modulus and superconductivity parameters were calculated. We found that under pressures, in the range of 1-5 GPa, Fr could be a superconductor at a critical temperature of about 4K.

  15. The Effect of Polarization on Local Electronic Structure in Ferroelectric Nano-Domains in BaTiO3

    NASA Astrophysics Data System (ADS)

    Morales, Erie; Perez, Carlos; Bonnell, Dawn; MSE Team

    Novel ferroelectric BaTiO3 applications ranging from sensors to nanogenerators require a detailed understanding of atomic interactions at surfaces. Single crystals provide a platform that allows the exploitation of surface physical and chemical properties that can be readily transferred to other ABO3 perovskites. The processes that result in the atomic and electronic structures of surfaces in tandem with polarization of domains are necessary steps towards understanding BaTiO3. Here we treat BaTiO3 surface using sputtering-annealing cycles that yield the (6x1) reconstruction. We demonstrate that it is possible to pole a thin BaTiO3 single crystal in ultra high vacuum using scanning tunneling microscopy (STM). We determine that we can prepare BaTiO3 using in-situ annealing that allows us to control the size of poled region to 40nm. We pole in constant-current mode in STM by applying a bias of less than 10 V between tip and sample for 100ms. STM and scanning tunneling spectroscopy characterization allow us to map topography and local density of states, respectively. For a given unique pulse, the poled domains show a fluctuating electronic occupation of conduction bands and shifting of valence band. We will also discuss the effect of polarization on molecular adsorption.

  16. The 5f localization/delocalization in square and hexagonal americium monolayers: a FP-LAPW electronic structure study

    NASA Astrophysics Data System (ADS)

    Gao, D.; Ray, A. K.

    2006-04-01

    The electronic and geometrical properties of bulk americium and square and hexagonal americium monolayers have been studied with the full-potential linearized augmented plane wave (FP-LAPW) method. The effects of several common approximations are examined: (1) non-spin polarization (NSP) vs. spin polarization (SP); (2) scalar-relativity (no spin-orbit coupling (NSO)) vs. full-relativity (i.e., with spin-orbit (SO) coupling included); (3) local-density approximation (LDA) vs. generalized-gradient approximation (GGA). Our results indicate that both spin polarization and spin orbit coupling play important roles in determining the geometrical and electronic properties of americium bulk and monolayers. A compression of both americium square and hexagonal monolayers compared to the americium bulk is also observed. In general, the LDA is found to underestimate the equilibrium lattice constant and give a larger total energy compared to the GGA calculations. While spin orbit coupling shows a similar effect on both square and hexagonal monolayer calculations regardless of the model, GGA versus LDA, an unusual spin polarization effect on both square and hexagonal monolayers is found in the LDA results as compared with the GGA results. The 5f delocalization transition of americium is employed to explain our observed unusual spin polarization effect. In addition, our results at the LDA level of theory indicate a possible 5f delocalization could happen in the americium surface within the same Am II (fcc crystal structure) phase, unlike the usually reported americium 5f delocalization which is associated with crystal structure change. The similarities and dissimilarities between the properties of an Am monolayer and a Pu monolayer are discussed in detail.

  17. Probing local and electronic structure in Warm Dense Matter: single pulse synchrotron x-ray absorption spectroscopy on shocked Fe

    PubMed Central

    Torchio, Raffaella; Occelli, Florent; Mathon, Olivier; Sollier, Arnaud; Lescoute, Emilien; Videau, Laurent; Vinci, Tommaso; Benuzzi-Mounaix, Alessandra; Headspith, Jon; Helsby, William; Bland, Simon; Eakins, Daniel; Chapman, David; Pascarelli, Sakura; Loubeyre, Paul

    2016-01-01

    Understanding Warm Dense Matter (WDM), the state of planetary interiors, is a new frontier in scientific research. There exists very little experimental data probing WDM states at the atomic level to test current models and those performed up to now are limited in quality. Here, we report a proof-of-principle experiment that makes microscopic investigations of materials under dynamic compression easily accessible to users and with data quality close to that achievable at ambient. Using a single 100 ps synchrotron x-ray pulse, we have measured, by K-edge absorption spectroscopy, ns-lived equilibrium states of WDM Fe. Structural and electronic changes in Fe are clearly observed for the first time at such extreme conditions. The amplitude of the EXAFS oscillations persists up to 500 GPa and 17000 K, suggesting an enduring local order. Moreover, a discrepancy exists with respect to theoretical calculations in the value of the energy shift of the absorption onset and so this comparison should help to refine the approximations used in models. PMID:27246145

  18. Probing local and electronic structure in Warm Dense Matter: single pulse synchrotron x-ray absorption spectroscopy on shocked Fe

    NASA Astrophysics Data System (ADS)

    Torchio, Raffaella; Occelli, Florent; Mathon, Olivier; Sollier, Arnaud; Lescoute, Emilien; Videau, Laurent; Vinci, Tommaso; Benuzzi-Mounaix, Alessandra; Headspith, Jon; Helsby, William; Bland, Simon; Eakins, Daniel; Chapman, David; Pascarelli, Sakura; Loubeyre, Paul

    2016-06-01

    Understanding Warm Dense Matter (WDM), the state of planetary interiors, is a new frontier in scientific research. There exists very little experimental data probing WDM states at the atomic level to test current models and those performed up to now are limited in quality. Here, we report a proof-of-principle experiment that makes microscopic investigations of materials under dynamic compression easily accessible to users and with data quality close to that achievable at ambient. Using a single 100 ps synchrotron x-ray pulse, we have measured, by K-edge absorption spectroscopy, ns-lived equilibrium states of WDM Fe. Structural and electronic changes in Fe are clearly observed for the first time at such extreme conditions. The amplitude of the EXAFS oscillations persists up to 500 GPa and 17000 K, suggesting an enduring local order. Moreover, a discrepancy exists with respect to theoretical calculations in the value of the energy shift of the absorption onset and so this comparison should help to refine the approximations used in models.

  19. Probing local and electronic structure in Warm Dense Matter: single pulse synchrotron x-ray absorption spectroscopy on shocked Fe.

    PubMed

    Torchio, Raffaella; Occelli, Florent; Mathon, Olivier; Sollier, Arnaud; Lescoute, Emilien; Videau, Laurent; Vinci, Tommaso; Benuzzi-Mounaix, Alessandra; Headspith, Jon; Helsby, William; Bland, Simon; Eakins, Daniel; Chapman, David; Pascarelli, Sakura; Loubeyre, Paul

    2016-01-01

    Understanding Warm Dense Matter (WDM), the state of planetary interiors, is a new frontier in scientific research. There exists very little experimental data probing WDM states at the atomic level to test current models and those performed up to now are limited in quality. Here, we report a proof-of-principle experiment that makes microscopic investigations of materials under dynamic compression easily accessible to users and with data quality close to that achievable at ambient. Using a single 100 ps synchrotron x-ray pulse, we have measured, by K-edge absorption spectroscopy, ns-lived equilibrium states of WDM Fe. Structural and electronic changes in Fe are clearly observed for the first time at such extreme conditions. The amplitude of the EXAFS oscillations persists up to 500 GPa and 17000 K, suggesting an enduring local order. Moreover, a discrepancy exists with respect to theoretical calculations in the value of the energy shift of the absorption onset and so this comparison should help to refine the approximations used in models. PMID:27246145

  20. Laser induced local structural and property modifications in semiconductors for electronic and photonic superstructures - Silicon carbide to graphene conversion

    NASA Astrophysics Data System (ADS)

    Yue, Naili

    Graphene is a single atomic layer two-dimensional (2D) hexagonal crystal of carbon atoms with sp2-bonding. Because of its various special or unique properties, graphene has attracted huge attention and considerable interest in recent years. This PhD research work focuses on the development of a novel approach to fabricating graphene micro- and nano-structures using a 532 nm Nd:YAG laser, a technique based on local conversion of 3C-SiC thin film into graphene. Different from other reported laser-induced graphene on single crystalline 4H- or 6H- SiC, this study focus on 3C-SiC polycrystal film grown using MBE. Because the SiC thin film is grown on silicon wafer, this approach may potentially lead to various new technologies that are compatible with those of Si microelectronics for fabricating graphene-based electronic, optoelectronic, and photonic devices. The growth conditions for depositing 3C-SiC using MBE on Si wafers with three orientations, (100), (110), and (111), were evaluated and explored. The surface morphology and crystalline structure of 3C-SiC epilayer were investigated with SEM, AFM, XRD, μ-Raman, and TEM. The laser modification process to convert 3C-SiC into graphene layers has been developed and optimized by studying the quality dependence of the graphene layers on incident power, irradiation time, and surface morphology of the SiC film. The laser and power density used in this study which focused on thin film SiC was compared with those used in other related research works which focused on bulk SiC. The laser-induced graphene was characterized with μ-Raman, SEM/EDS, TEM, AFM, and, I-V curve tracer. Selective deposition of 3C-SiC thin film on patterned Si substrate with SiO2 as deposition mask has been demonstrated, which may allow the realization of graphene nanostructures (e.g., dots and ribbons) smaller than the diffraction limit spot size of the laser beam, down to the order of 100 nm. The electrical conductance of directly written graphene

  1. Role of defects in BiFeO₃ multiferroic films and their local electronic structure by x-ray absorption spectroscopy

    SciTech Connect

    Ravalia, Ashish; Vagadia, Megha; Solanki, P. S.; Shah, N. A.; Kuberkar, D. G.; Gautam, S.; Chae, K. H.; Asokan, K.

    2014-10-21

    Present study reports the role of defects in the electrical transport in BiFeO₃ (BFO) multiferroic films and its local electronic structure investigated by near-edge X-ray absorption fine structure. Defects created by high energy 200 MeV Ag⁺¹⁵ ion irradiation with a fluence of ∼5 × 10¹¹ ions/cm² results in the increase in structural strain and reduction in the mobility of charge carriers and enhancement in resistive (I-V) and polarization (P-E) switching behaviour. At higher fluence of ∼5 × 10¹² ions/cm², there is a release in the structural strain due to local annealing effect, resulting in an increase in the mobility of charge carriers, which are released from oxygen vacancies and hence suppression in resistive and polarization switching. Near-edge X-ray absorption fine structure studies at Fe L₃,₂- and O K-edges show a significant change in the spectral features suggesting the modifications in the local electronic structure responsible for changes in the intrinsic magnetic moment and electrical transport properties of BFO.

  2. Temperature dependent evolution of the electronic and local atomic structure in the cubic colossal magnetoresistive manganite La1-xSrxMnO3

    SciTech Connect

    Arenholz, Elke; Mannella, N.; Booth, C.H.; Rosenhahn, A.; Sell, B.C.; Nambu, A.; Marchesini, S.; Mun, B. S.; Yang, S.-H.; Watanabe, M.; Ibrahim, K.; Arenholz, E.; Young, A.; Guo, J.; Tomioka, Y.; Fadley, C.S.

    2007-12-06

    We have studied the temperature-dependent evolution of the electronic and local atomic structure in the cubic colossal magnetoresistive manganite La{sub 1-x}Sr{sub x}MnO{sub 3} (x= 0.3-0.4) with core and valence level photoemission (PE), x-ray absorption spectroscopy (XAS), x-ray emission spectroscopy (XES), resonant inelastic x-ray scattering (RIXS), extended x-ray absorption fine structure (EXAFS) spectroscopy and magnetometry. As the temperature is varied across the Curie temperature T{sub c}, our PE experiments reveal a dramatic change of the electronic structure involving an increase in the Mn spin moment from {approx} 3 {micro}B to {approx} 4 {micro}B, and a modification of the local chemical environment of the other constituent atoms indicative of electron localization on the Mn atom. These effects are reversible and exhibit a slow-timescale {approx}200 K-wide hysteresis centered at T{sub c}. Based upon the probing depths accessed in our PE measurements, these effects seem to survive for at least 35-50 {angstrom} inward from the surface, while other consistent signatures for this modification of the electronic structure are revealed by more bulk sensitive spectroscopies like XAS and XES/RIXS. We interpret these effects as spectroscopic fingerprints for polaron formation, consistent with the presence of local Jahn-Teller distortions of the MnO{sub 6} octahedra around the Mn atom, as revealed by the EXAFS data. Magnetic susceptibility measurements in addition show typical signatures of ferro-magnetic clusters formation well above the Curie temperature.

  3. Electronic structure localization and spin-state transition in Cu-substituted FeSe: Fe1-xCuxSe

    SciTech Connect

    Chadov, Stanislav; Scharf, Daniel; Fecher, Gerhard H; Felser, Claudia; Zhang, Lijun; Singh, David J

    2010-01-01

    We report density-functional studies of the Fe{sub 1-x}Cu{sub x}Se alloy done using supercell and coherent-potential approximation methods. Magnetic behavior was investigated using the disordered local moment approach. We find that Cu occurs in a nominal d{sup 10} configuration and is highly disruptive to the electronic structure of the Fe sheets. This would be consistent with a metal-insulator transition due to Anderson localization. We further find a strong crossover from a weak moment itinerant system to a local moment magnet at x{approx}0.12. We associate this with the experimentally observed jump near this concentration. our results are consistent with the characterization of this concentration-dependent jump as a transition to a spin glass.

  4. An insight into crystal, electronic, and local structures of lithium iron silicate (Li2FeSiO4) materials upon lithium extraction

    NASA Astrophysics Data System (ADS)

    Kamon-in, O.; Klysubun, W.; Limphirat, W.; Srilomsak, S.; Meethong, N.

    2013-05-01

    Recently, orthosilicate, Li2MSiO4 (where M=transition metal) materials have been attracting considerable attention for potential use as a new generation cathode for Li-ion batteries due to their safety, low toxicity, and low cost characteristics. In addition, the presence of two Li+ ions in the molecule offers a multiple electron-charge transfer (M2+/M3+ and M3+/M4+ redox couples), thus allowing a high achievable capacity of more than 320 mA h/g per M unit. Good electrochemical properties of Li2FeSiO4 have been reported through several approaches such as downsizing of the particles, carbon-coating, etc. However, in addition to electrochemical performance, fundamental understanding regarding crystal, electronic and local structure changes during charge/discharge processes is also important and needs more rigorous investigation. In this work, lithium iron silicates (Li2FeSiO4/C) in space group of Pnma: a=10.6671(3) Å, b=6.2689(2) Å, and c=5.0042(2) Å have been prepared by solid-state reaction. The synthesized as well as chemical delithiated samples have been characterized by XRD, HRTEM, AAS and XAS techniques. We will show the results focusing on Fe K-edge XANES, EXAFS, HRTEM and XRD of the Li2-xFeSiO4 samples and discuss how the crystal, electronic, and local structure changes upon Li+ de-intercalation.

  5. Natural geometric representation for electron local observables

    SciTech Connect

    Minogin, V.G.

    2014-03-15

    An existence of the quartic identities for the electron local observables that define orthogonality relations for the 3D quantities quadratic in the electron observables is found. It is shown that the joint solution of the quartic and bilinear identities for the electron observables defines a unique natural representation of the observables. In the natural representation the vector type electron local observables have well-defined fixed positions with respect to a local 3D orthogonal reference frame. It is shown that the natural representation of the electron local observables can be defined in six different forms depending on a choice of the orthogonal unit vectors. The natural representation is used to determine the functional dependence of the electron wave functions on the local observables valid for any shape of the electron wave packet. -- Highlights: •Quartic identities that define the orthogonality relations for the electron local observables are found. •Joint solution of quartic and bilinear identities defines a unique natural representation of the electron local observables. •Functional dependence of the electron wave functions on the electron local observables is determined.

  6. Local symmetry breaking of a thin crystal structure of β-Si3N4 as revealed by spherical aberration corrected high-resolution transmission electron microscopy images.

    PubMed

    Kim, Hwang Su; Zhang, Zaoli; Kaiser, Ute

    2012-06-01

    This report is an extension of the study for structural imaging of 5-6 nm thick β-Si(3)N(4) [0001] crystal with a spherical aberration corrected transmission electron microscope by Zhang and Kaiser [2009. Structure imaging of β-Si(3)N(4) by spherical aberration-corrected high-resolution transmission electron microscopy. Ultramicroscopy 109, 1114-1120]. In this work, a local symmetry breaking with an uneven resolution of dumbbells in the six-membered rings revealed in the reported images in the study of Zhang and Kaiser has been analyzed in detail. It is found that this local asymmetry in the image basically is not relevant to a slight mistilt of the specimen and/or a beam tilt (coma). Rather the certain variation of the tetrahedral bond length of Si-N(4) in the crystal structure is found to be responsible for the uneven resolution with a local structural variation from region to region. This characteristic of the variation is also supposed to give a distorted lattice of apparently 2°-2.5° deviations from the perfect hexagonal unit cell as observed in the reported image in the work of Zhang and Kaiser. It is discussed that this variation may prevail only in a thin specimen with a thickness ranging ~≤ 5-6 nm. At the same time, it is noted that the average of the bond length variation is close to the fixed length known in a bulk crystal of β-Si(3)N(4). PMID:22499470

  7. Structural and electronic control of the metal to insulator transition and local orderings in the θ-(BEDT-TTF)2X organic conductors.

    PubMed

    Alemany, Pere; Pouget, Jean-Paul; Canadell, Enric

    2015-11-25

    A first-principles density functional theory (DFT) study of [Formula: see text]-(BEDT-TTF)2X molecular conductors with X  =  I3, CsCo(SCN)4 (ambient pressure, 7.5 kbar and 10 kbar), CsZn(SCN)4, TlCo(SCN)4, RbCo(SCN)4 and RbZn(SCN)4 (220 K and 90 K) is reported. It is shown that these salts exhibit three different types of band structure each of them associated with a different physical behavior. In contrast with previous proposals it is found that the key electronic parameter behind the differences in the band structures is the intrastack transfer integral, t c . A new mechanism for the metal to insulator transition in the [Formula: see text]-(BEDT-TTF)2MM'(SCN)4 ([Formula: see text], Tl; [Formula: see text], Co) salts is proposed, where an order-disorder structural transition of the ethylenedithio groups doubling the periodicity along the stack direction drives the system into an electronically pseudo-1D system along the interstack direction that is subject to a 4k F charge localization of holes. The structural rearrangement is such that the holes are not distributed equally between the two donors; the larger hole density is associated with the B donors which establish the strongest hydrogen bonds with the anion layers. A detailed microscopic description of how disorder of the ethylenedithio groups, the θ dihedral angle and the electronic structure intermingle and lead to the unusual phase diagram of these salts is presented. In this framework the role of pressure and uniaxial strain in controlling the physical behavior of these salts is discussed. PMID:26510211

  8. Structural and electronic control of the metal to insulator transition and local orderings in the θ-(BEDT-TTF)2X organic conductors

    NASA Astrophysics Data System (ADS)

    Alemany, Pere; Pouget, Jean-Paul; Canadell, Enric

    2015-11-01

    A first-principles density functional theory (DFT) study of θ -(BEDT-TTF)2X molecular conductors with X  =  I3, CsCo(SCN)4 (ambient pressure, 7.5 kbar and 10 kbar), CsZn(SCN)4, TlCo(SCN)4, RbCo(SCN)4 and RbZn(SCN)4 (220 K and 90 K) is reported. It is shown that these salts exhibit three different types of band structure each of them associated with a different physical behavior. In contrast with previous proposals it is found that the key electronic parameter behind the differences in the band structures is the intrastack transfer integral, t c . A new mechanism for the metal to insulator transition in the θ -(BEDT-TTF)2MM‧(SCN)4 (\\text{M}=\\text{Rb} , Tl; {{\\text{M}}\\prime}=\\text{Zn} , Co) salts is proposed, where an order-disorder structural transition of the ethylenedithio groups doubling the periodicity along the stack direction drives the system into an electronically pseudo-1D system along the interstack direction that is subject to a 4k F charge localization of holes. The structural rearrangement is such that the holes are not distributed equally between the two donors; the larger hole density is associated with the B donors which establish the strongest hydrogen bonds with the anion layers. A detailed microscopic description of how disorder of the ethylenedithio groups, the θ dihedral angle and the electronic structure intermingle and lead to the unusual phase diagram of these salts is presented. In this framework the role of pressure and uniaxial strain in controlling the physical behavior of these salts is discussed.

  9. Oxygen vacancy formation in CeO2 and Ce(1-x)Zr(x)O2 solid solutions: electron localization, electrostatic potential and structural relaxation.

    PubMed

    Wang, Hai-Feng; Li, Hui-Ying; Gong, Xue-Qing; Guo, Yang-Long; Lu, Guan-Zhong; Hu, P

    2012-12-28

    Ceria (CeO(2)) and ceria-based composite materials, especially Ce(1-x)Zr(x)O(2) solid solutions, possess a wide range of applications in many important catalytic processes, such as three-way catalysts, owing to their excellent oxygen storage capacity (OSC) through the oxygen vacancy formation and refilling. Much of this activity has focused on the understanding of the electronic and structural properties of defective CeO(2) with and without doping, and comprehending the determining factor for oxygen vacancy formation and the rule to tune the formation energy by doping has constituted a central issue in material chemistry related to ceria. However, the calculation on electronic structures and the corresponding relaxation patterns in defective CeO(2-x) oxides remains at present a challenge in the DFT framework. A pragmatic approach based on density functional theory with the inclusion of on-site Coulomb correction, i.e. the so-called DFT + U technique, has been extensively applied in the majority of recent theoretical investigations. Firstly, we review briefly the latest electronic structure calculations of defective CeO(2)(111), focusing on the phenomenon of multiple configurations of the localized 4f electrons, as well as the discussions of its formation mechanism and the catalytic role in activating the O(2) molecule. Secondly, aiming at shedding light on the doping effect on tuning the oxygen vacancy formation in ceria-based solid solutions, we summarize the recent theoretical results of Ce(1-x)Zr(x)O(2) solid solutions in terms of the effect of dopant concentrations and crystal phases. A general model on O vacancy formation is also discussed; it consists of electrostatic and structural relaxation terms, and the vital role of the later is emphasized. Particularly, we discuss the crucial role of the localized structural relaxation patterns in determining the superb oxygen storage capacity in kappa-phase Ce(1-x)Zr(1-x)O(2). Thirdly, we briefly discuss some

  10. Parameterised local spin density exchange-correlation energies and potentials for electronic structure calculations I. Zero temperature formalism

    NASA Astrophysics Data System (ADS)

    MacLaren, J. M.; Clougherty, D. P.; McHenry, M. E.; Donovan, M. M.

    1991-09-01

    Commonly used approximate forms for the exchange-correlation energy and potential within the local density approximation are summarised, and FORTRAN code is included for the evaluation of these various forms. Included are the following: Xα, Kohn-Sham-Gaspàr, Hedin-Lundqvist-Wilkins, Janak-Moruzzi-Williams, Von Barth-Hedin, Ceperley-Alder (Perdew-Zunger), and Ceperley-Alder (Vosko-Wilk-Nusair). Both the Vosko-Wilk-Nusair and the Von Barth-Hedin expressions for spin interpolation between paramagnetic and ferromagnetic limits are also provided.

  11. Local geometric and electronic structures and origin of magnetism in Co-doped BaTiO{sub 3} multiferroics

    SciTech Connect

    Phan, The-Long; Ho, T. A.; Manh, T. V.; Yu, S. C.; Thang, P. D.; Thanh, Tran Dang; Lam, V. D.; Dang, N. T.

    2015-05-07

    We have prepared polycrystalline samples BaTi{sub 1−x}Co{sub x}O{sub 3} (x = 0–0.1) by solid-state reaction. X-ray diffraction and Raman-scattering studies reveal the phase separation in crystal structure as changing Co-doping content (x). The samples with x = 0–0.01 are single phase in a tetragonal structure. At higher doping contents (x > 0.01), there is the formation and development of a secondary hexagonal phase. Magnetization measurements at room temperature indicate a coexistence of paramagnetic and weak-ferromagnetic behaviors in BaTi{sub 1−x}Co{sub x}O{sub 3} samples with x > 0, while pure BaTiO{sub 3} is diamagnetic. Both these properties increase with increasing x. Analyses of X-ray absorption spectra recorded from BaTi{sub 1−x}Co{sub x}O{sub 3} for the Co and Ti K-edges indicate the presence of Co{sup 2+} and Co{sup 3+} ions. They locate in the Ti{sup 4+} site of the tetragonal and hexagonal BaTiO{sub 3} structures. Particularly, there is a shift of oxidation state from Co{sup 2+} to Co{sup 3+} when Co-doping content increases. We believe that the paramagnetic nature in BaTi{sub 1−x}Co{sub x}O{sub 3} samples is due to isolated Co{sup 2+} and Co{sup 3+} centers. The addition of Co{sup 3+} ions enhances the paramagnetic behavior. Meanwhile, the origin of ferromagnetism is due to lattice defects, which is less influenced by the changes caused by the variation in concentration of Co{sup 2+} and Co{sup 3+} ions.

  12. How do electron localization functions describe π-electron delocalization?

    PubMed

    Steinmann, Stephan N; Mo, Yirong; Corminboeuf, Clemence

    2011-12-14

    Scalar fields provide an intuitive picture of chemical bonding. In particular, the electron localization function (ELF) has proven to be highly valuable in interpreting a broad range of bonding patterns. The discrimination between enhanced or reduced electron (de)localization within cyclic π-conjugated systems remains, however, challenging for ELF. In order to clearly distinguish between the local properties of ten highly and weakly π-(de)localized prototype systems, we compare the ELFs of both the canonical wave functions and electron-localized states (diabatic) with those of two closely related scalar fields: the electron localizability indicator (ELI-D) and the localized orbital locator (LOL). The simplest LOL function distinguishes enhanced from weak π-(de)localization in an insightful and reliable manner. LOL offers the finest contrast between annulenes with 4n/4n + 2 π electrons and their inorganic analogues as well as between hyperconjugated cyclopentadiene derivatives. LOL(π) also gives an appealing and intuitive picture of the π-bond. In contrast, the most popular ELF fails to capture subtle contrasting local electronic properties and suffers from the arbitrariness of the σ/π dissection. The orbital separation of the most recent ELI-D is clear-cut but the interpretations sometime less straightforward in the present context. PMID:21660323

  13. Electronic structure of black sodalite

    NASA Astrophysics Data System (ADS)

    Sankey, Otto F.; Demkov, Alexander A.; Lenosky, Thomas

    1998-06-01

    The electronic structure of black sodalite, Na8(AlSiO4)6, is determined in the local-spin-density approximation (LSDA). This structure has six Na atoms to compensate the six Al atoms, leaving two excess Na atoms. A band-gap electronic state is induced in the wide oxide gap by the excess sodium, and has ``particle in a box'' behavior. Magnetic orderings of these gap states are studied. Analytic models show that an antiferromagnetic ordering is lowest in energy in the LSDA. A self-consistent LSDA calculation shows the system to change from a metal to an antiferromagnetic insulator when spin orderings are allowed. Hopping and Hubbard-U parameters are estimated, and the many-body correlated Hubbard model is solved using a constrained path Monte Carlo technique, which again predicts the system to be antiferromagnetic with a Tc of order 50 K.

  14. Electronic structure of Calcium hexaborides

    SciTech Connect

    Lee, Byounghak; Wang, Lin-Wang

    2005-06-15

    We present a theoretical study of crystal and electronic structures of CaB6 within a screened-exchange local density approximation (sX-LDA). Our ab initio total energy calculations show that CaB6 is a semiconductor with a gap of >1.2 eV, in agreement with recent experimental observations. We show a very sensitive band gap dependence on the crystal internal parameter, which might partially explain the scatter of previous theoretical results. Our calculation demonstrates that it is essential to study this system simultaneously for both crystal structures and electronic properties, and that the sX-LDA provides an ideal method for this problem.

  15. Local electronic structure of a single nonmagnetic impurity as a test of the pairing symmetry of electrons in (K,Tl)FexSe2 superconductors.

    PubMed

    Zhu, Jian-Xin; Yu, Rong; Balatsky, A V; Si, Qimiao

    2011-10-14

    We study the effect of a single nonmagnetic impurity on the recently discovered (K,Tl)Fe(x)Se(2) superconductors, within both a toy two-band model and a more realistic five-band model. We find that, out of five types of pairing symmetry under consideration, only the d(x(2)-y(2))-wave pairing gives rise to impurity resonance states. The intragap states have energies far away from the Fermi energy. The existence of these intragap states is robust against the presence or absence of interband scattering. However, the interband scattering does tune the relative distribution of local density of states at the resonance states. All these features can readily be accessed by STM experiments, and are proposed as a means to test the pairing symmetry of the new superconductors. PMID:22107421

  16. Direct observation of the symmetry breaking of the nanometer-scale local structure in the paraelectric cubic phase of BaTiO3 using convergent-beam electron diffraction

    NASA Astrophysics Data System (ADS)

    Tsuda, Kenji; Tanaka, Michiyoshi

    2016-07-01

    Nanometer-scale local structures of the cubic phase of barium titanate (BaTiO3) are investigated by convergent-beam electron diffraction (CBED) using a nanometer-size electron probe. Breaking of the cubic symmetry has been discovered in the nanometer-scale areas of the cubic phase. This indicates the existence of local polarization clusters as a precursor of the phase transition. Symmetry-breaking index maps for the fourfold rotation symmetry are given at different temperatures with the combined use of scanning transmission electron microscopy and CBED methods (STEM-CBED). A spatially hierarchical structure of the cubic phase is proposed, which may explain different local symmetries reported using different experimental probes.

  17. Excess Electron Localization in Solvated DNA Bases

    SciTech Connect

    Smyth, Maeve; Kohanoff, Jorge

    2011-06-10

    We present a first-principles molecular dynamics study of an excess electron in condensed phase models of solvated DNA bases. Calculations on increasingly large microsolvated clusters taken from liquid phase simulations show that adiabatic electron affinities increase systematically upon solvation, as for optimized gas-phase geometries. Dynamical simulations after vertical attachment indicate that the excess electron, which is initially found delocalized, localizes around the nucleobases within a 15 fs time scale. This transition requires small rearrangements in the geometry of the bases.

  18. Electron localization of anions probed by nitrile vibrations

    SciTech Connect

    Mani, Tomoyasu; Grills, David C.; Newton, Marshall D.; Miller, John R.

    2015-08-02

    Localization and delocalization of electrons is a key concept in chemistry, and is one of the important factors determining the efficiency of electron transport through organic conjugated molecules, which have potential to act as “molecular wires”. This, in turn, substantially influences the efficiencies of organic solar cells and other molecular electronic devices. It is also necessary to understand the electronic energy landscape and the dynamics of electrons through molecular chain that govern their transport capabilities in one-dimensional conjugated chains so that we can better define the design principles of conjugated molecules for their applications. We show that nitrile ν(C≡N) vibrations respond to the degree of electron localization in nitrile-substituted organic anions by utilizing time-resolved infrared (TRIR) detection combined with pulse radiolysis. Measurements of a series of aryl nitrile anions allow us to construct a semi-empirical calibration curve between the changes in the ν(C≡N) IR shifts and the changes in the electronic charges from the neutral to the anion states in the nitriles; more electron localization in the nitrile anion results in larger IR shifts. Furthermore, the IR linewidth in anions can report a structural change accompanying changes in the electronic density distribution. Probing the shift of the nitrile ν(C≡N) IR vibrational bands enables us to determine how the electron is localized in anions of nitrile-functionalized oligofluorenes, considered as organic mixed-valence compounds. We estimate the diabatic electron transfer distance, electronic coupling strengths, and energy barriers in these organic mixed-valence compounds. The analysis reveals a dynamic picture, showing that the electron is moving back and forth within the oligomers with a small activation energy of ≤ kBT, likely controlled by the movement of dihedral angles between monomer units. Thus, implications for the electron transport

  19. Electron localization of anions probed by nitrile vibrations

    DOE PAGESBeta

    Mani, Tomoyasu; Grills, David C.; Newton, Marshall D.; Miller, John R.

    2015-08-02

    Localization and delocalization of electrons is a key concept in chemistry, and is one of the important factors determining the efficiency of electron transport through organic conjugated molecules, which have potential to act as “molecular wires”. This, in turn, substantially influences the efficiencies of organic solar cells and other molecular electronic devices. It is also necessary to understand the electronic energy landscape and the dynamics of electrons through molecular chain that govern their transport capabilities in one-dimensional conjugated chains so that we can better define the design principles of conjugated molecules for their applications. We show that nitrile ν(C≡N) vibrationsmore » respond to the degree of electron localization in nitrile-substituted organic anions by utilizing time-resolved infrared (TRIR) detection combined with pulse radiolysis. Measurements of a series of aryl nitrile anions allow us to construct a semi-empirical calibration curve between the changes in the ν(C≡N) IR shifts and the changes in the electronic charges from the neutral to the anion states in the nitriles; more electron localization in the nitrile anion results in larger IR shifts. Furthermore, the IR linewidth in anions can report a structural change accompanying changes in the electronic density distribution. Probing the shift of the nitrile ν(C≡N) IR vibrational bands enables us to determine how the electron is localized in anions of nitrile-functionalized oligofluorenes, considered as organic mixed-valence compounds. We estimate the diabatic electron transfer distance, electronic coupling strengths, and energy barriers in these organic mixed-valence compounds. The analysis reveals a dynamic picture, showing that the electron is moving back and forth within the oligomers with a small activation energy of ≤ kBT, likely controlled by the movement of dihedral angles between monomer units. Thus, implications for the electron transport capability

  20. Electronic structure of disordered conjugated polymers: Polythiophenes

    SciTech Connect

    Vukmirovic, Nenad; Wang, Lin-Wang

    2008-11-26

    Electronic structure of disordered semiconducting conjugated polymers was studied. Atomic structure was found from a classical molecular dynamics simulation and the charge patching method was used to calculate the electronic structure with the accuracy similar to the one of density functional theory in local density approximation. The total density of states, the local density of states at different points in the system and the wavefunctions of several states around the gap were calculated in the case of poly(3-hexylthiophene) (P3HT) and polythiophene (PT) systems to gain insight into the origin of disorder in the system, the degree of carrier localization and the role of chain interactions. The results indicated that disorder in the electronic structure of alkyl substituted polythiophenes comes from disorder in the conformation of individualchains, while in the case of polythiophene there is an additional contribution due to disorder in the electronic coupling between the chains. Each of the first several wavefunctions in the conduction and valence band of P3HT is localized over several rings of a single chain. It was shown that the localization can be caused in principle both by ring torsions and chain bending, however the effect of ring torsions is much stronger. PT wavefunctions are more complicated due to larger interchain electronic coupling and are not necessarily localized on a single chain.

  1. Electronic structure of lithium amide

    NASA Astrophysics Data System (ADS)

    Kamakura, N.; Takeda, Y.; Saitoh, Y.; Yamagami, H.; Tsubota, M.; Paik, B.; Ichikawa, T.; Kojima, Y.; Muro, T.; Kato, Y.; Kinoshita, T.

    2011-01-01

    The electronic structure of the insulator lithium amide (LiNH2), which is a lightweight complex hydride being considered as a high-capacity hydrogen storage material, is investigated by N 1s soft x-ray emission spectroscopy (XES) and absorption spectroscopy (XAS). The XES and XAS spectra show a band gap between the valence and conduction bands. The valence band in the XES spectrum consists of three peaks, which extend up to ~-8 eV from the valence band top. The band calculation within the local-density approximation (LDA) for LiNH2shows energetically separated three peaks in the occupied N 2p partial density of states (pDOS) and the band gap. The energy distribution of three peaks in the XES spectrum agrees with that in the calculated pDOS except for the peak at the highest binding energy, which is attributed to the strongly hybridized state between N 2p and H 1s. The XES experiment has clarified that the strongly hybridized state with H 1s in LiNH2is located at binding energy higher than that of the LDA calculation, while the overall feature of the electronic structure of LiNH2experimentally obtained by XES and XAS is consistent with the calculated result.

  2. Probing the local electronic structure of the cross-linked (1 × 2) reconstruction of rutile TiO2(110)

    NASA Astrophysics Data System (ADS)

    Yim, Chi Ming; Pang, Chi Lun; Thornton, Geoff

    2016-08-01

    The electronic structure of cross-linked TiO2(110)-(1 × 2) has been investigated using scanning tunneling spectroscopy (STS) and by monitoring changes in ultraviolet photoelectron spectroscopy (UPS) following exposure of the surface to O2. STS reveals two states located in the bandgap, at 0.7 and 1.5 eV below the Fermi level. The population of these two states varies over different parts of the (1 × 2)-reconstructed surface. An additional state at 1.1 eV above the Fermi level is observed at the double link part of the structure. All of the bandgap states are attenuated following exposure to O2, while the workfunction is increased. We attribute this to an electron transfer from the surface to the adsorbed oxygen.

  3. Guanine quadruplex structures localize to heterochromatin

    PubMed Central

    Hoffmann, Roland F.; Moshkin, Yuri M.; Mouton, Stijn; Grzeschik, Nicola A.; Kalicharan, Ruby D.; Kuipers, Jeroen; Wolters, Anouk H.G.; Nishida, Kazuki; Romashchenko, Aleksander V.; Postberg, Jan; Lipps, Hans; Berezikov, Eugene; Sibon, Ody C.M.; Giepmans, Ben N.G.; Lansdorp, Peter M.

    2016-01-01

    Increasing amounts of data support a role for guanine quadruplex (G4) DNA and RNA structures in various cellular processes. We stained different organisms with monoclonal antibody 1H6 specific for G4 DNA. Strikingly, immuno-electron microscopy showed exquisite specificity for heterochromatin. Polytene chromosomes from Drosophila salivary glands showed bands that co-localized with heterochromatin proteins HP1 and the SNF2 domain-containing protein SUUR. Staining was retained in SUUR knock-out mutants but lost upon overexpression of SUUR. Somatic cells in Macrostomum lignano were strongly labeled, but pluripotent stem cells labeled weakly. Similarly, germline stem cells in Drosophila ovaries were weakly labeled compared to most other cells. The unexpected presence of G4 structures in heterochromatin and the difference in G4 staining between somatic cells and stem cells with germline DNA in ciliates, flatworms, flies and mammals point to a conserved role for G4 structures in nuclear organization and cellular differentiation. PMID:26384414

  4. Guanine quadruplex structures localize to heterochromatin.

    PubMed

    Hoffmann, Roland F; Moshkin, Yuri M; Mouton, Stijn; Grzeschik, Nicola A; Kalicharan, Ruby D; Kuipers, Jeroen; Wolters, Anouk H G; Nishida, Kazuki; Romashchenko, Aleksander V; Postberg, Jan; Lipps, Hans; Berezikov, Eugene; Sibon, Ody C M; Giepmans, Ben N G; Lansdorp, Peter M

    2016-01-01

    Increasing amounts of data support a role for guanine quadruplex (G4) DNA and RNA structures in various cellular processes. We stained different organisms with monoclonal antibody 1H6 specific for G4 DNA. Strikingly, immuno-electron microscopy showed exquisite specificity for heterochromatin. Polytene chromosomes from Drosophila salivary glands showed bands that co-localized with heterochromatin proteins HP1 and the SNF2 domain-containing protein SUUR. Staining was retained in SUUR knock-out mutants but lost upon overexpression of SUUR. Somatic cells in Macrostomum lignano were strongly labeled, but pluripotent stem cells labeled weakly. Similarly, germline stem cells in Drosophila ovaries were weakly labeled compared to most other cells. The unexpected presence of G4 structures in heterochromatin and the difference in G4 staining between somatic cells and stem cells with germline DNA in ciliates, flatworms, flies and mammals point to a conserved role for G4 structures in nuclear organization and cellular differentiation. PMID:26384414

  5. Localized Electron States Near a Metal-SemiconductorNanocontact

    SciTech Connect

    Demchenko, Denis O.; Wang, Lin-Wang

    2007-04-25

    The electronic structure of nanowires in contact withmetallic electrodes of experimentally relevant sizes is calculated byincorporating the electrostatic polarization potential into the atomisticsingle particle Schrodinger equation. We show that the presence of anelectrode produces localized electron/hole states near the electrode, aphenomenon only exhibited in nanostructures and overlooked in the past.This phenomenon will have profound implications on electron transport insuch nanosystems. We calculate several electrode/nanowire geometries,with varying contact depths and nanowire radii. We demonstrate the changein the band gap of up to 0.5 eV in 3 nm diameter CdSe nanowires andcalculate the magnitude of the applied electric field necessary toovercome the localization.

  6. Local atomic and electronic structure of LaCoO3 /SrTiO3 thin films by HAADF STEM and EELS

    NASA Astrophysics Data System (ADS)

    Borisevich, Albina; Hyuck Jang, Jae; Kim, Young-Min; Qiao, Liang; Biegalski, Michael

    2013-03-01

    For perovskite films with several competing functionalities, magnetic and electronic properties can be affected both by structural order parameters and chemical factors. For example, in LaCoO3 (LCO) thin films, magnetic and transport properties are strongly dependent on strain state and oxygen content. For this study, LCO thin films were deposited by pulsed laser deposition method with different thicknesses (2, 5, 15 unit cell and 20 nm thickness) on SrTiO3 substrate. X-ray photoelectron spectroscopy studies of the grown films have demonstrated that Co 3p edges shift up to 2 eV for 15 u.c. and 20 nm films, indicating possible presence of 2D electron gas. The structure of the 5 u.c and 15 u.c LCO films was examined. Atomic position mapping from STEM HAADF and BF images can reveal lattice parameter and octahedral tilt behavior with atomic resolution. BF STEM imaging showed that octahedral tilts were active in the 15 u.c. film but not in the 5 u.c. film. A complex pattern of O K fine structure evolution at the interface was observed; results of the deconvolution of different contributions to this behavior using advanced simulations, as well as data on oxygen vacancy mapping, will be presented. Research supported by the US DOE-BES, Materials Sciences and Engineering Division, and through a user project supported by ORNL's ShaRE User Program.

  7. Electronics for Piezoelectric Smart Structures

    NASA Technical Reports Server (NTRS)

    Warkentin, D. J.; Tani, J.

    1997-01-01

    This paper briefly presents work addressing some of the basic considerations for the electronic components used in smart structures incorporating piezoelectric elements. After general remarks on the application of piezoelectric elements to the problem of structural vibration control, three main topics are described. Work to date on the development of techniques for embedding electronic components within structural parts is presented, followed by a description of the power flow and dissipation requirements of those components. Finally current work on the development of electronic circuits for use in an 'active wall' for acoustic noise is introduced.

  8. Evolution of electronic structure as a function of layer thickness in group-VIB transition metal dichalcogenides: emergence of localization prototypes.

    PubMed

    Zhang, Lijun; Zunger, Alex

    2015-02-11

    Layered group-VIB transition metal dichalcogenides (with the formula of MX2) are known to show a transition from an indirect band gap in the thick n-monolayer stack (MX2)n to a direct band gap at the n = 1 monolayer limit, thus converting the system into an optically active material suitable for a variety of optoelectronic applications. The origin of this transition has been attributed predominantly to quantum confinement effect at reduced n. Our analysis of the evolution of band-edge energies and wave functions as a function of n using ab initio density functional calculations including the long-range dispersion interaction reveals (i) the indirect-to-direct band gap transformation is triggered not only by (kinetic-energy controlled) quantum confinement but also by (potential-energy controlled) band repulsion and localization. On its own, neither of the two effects can explain by itself the energy evolution of the band-edge states relevant to the transformation; (ii) when n decreased, there emerge distinct regimes with characteristic localization prototypes of band-edge states deciding the optical response of the system. They are distinguished by the real-space direct/indirect in combination with momentum-space direct/indirect nature of electron and hole states and give rise to distinct types of charge distribution of the photoexcited carriers that control excitonic behaviors; (iii) the various regimes associated with different localization prototypes are predicted to change with modification of cations and anions in the complete MX2 (M = Cr, Mo, W and X = S, Se, Te) series. These results offer new insight into understanding the excitonic properties (e.g., binding energy, lifetime etc.) of multiple layered MX2 and their heterostructures. PMID:25562378

  9. Localized structures in gaseous combustion

    NASA Astrophysics Data System (ADS)

    Knobloch, Edgar; Lo Jacono, David; Bergeon, Alain

    2015-11-01

    We consider a flame between a pair of porous walls at x = +/- 1 that allow fuel and oxidizer to diffuse into the burn region from opposite sides. The burn process is described by a binary one-step process of Arrhenius type. The heat released is redistributed via radiation. Convection is ignored. In 1D the low and high temperature states are connected by an S-shaped branch with a fold at low Damköhler number below which extinction takes place. Various instabilities occur on the upper (flame) branch leading to different time-dependent but 1D flames. In 2D the situation is dramatically modified: near the extinction region the burn front breaks up into structures that are localized in the direction along the front, with multiple branches of such states bifurcating from the fold. These correspond to states with n = 1 , 2 , ⋯ identical and equispaced hotspots. Further bifurcations generate states in which the hotspots are nonidentical and separated by unequal distances. All these states are present in the same parameter interval, implying great sensitivity of the system to initial conditions.

  10. Localized structure of Euglena bioconvection

    NASA Astrophysics Data System (ADS)

    Iima, Makoto; Shoji, Erika; Awazu, Akinori; Nishimori, Hiraku; Izumi, Shunsuke; Hiroshima University Collaboration

    2013-11-01

    Bioconvection of a suspension of Euglena gracilis, a photosensitive flagellate whose body length is approximately 50 micrometers, was experimentally studied. Under strong light intensity, Euglena has a negative phototaxis; they tend to go away from the light source. When the bright illumination is given from the bottom, a large scale spatio-temporal pattern is generated as a result of interaction between Euglena and surrounding flow. Recently, localized convection pattern had been reported, however, the generation process and interaction of the localized convection cells has not been analyzed. We performed experimental study to understand the localization mechanism, in particular, the onset of bioconvection and lateral localization behavior due to phototaxis. Experiments started from different initial condition suggests a bistability near the onset of the convection as binary fluid convection that also shows localized convection cells. Dynamics of localized convections cells, which is similar to the binary fluid convection case although the basic equations are not the same, is also reported.

  11. DNA Electronic Fingerprints by Local Spectroscopy on Graphene

    NASA Astrophysics Data System (ADS)

    Balatsky, Alexander

    2013-03-01

    Working and scalable alternatives to the conventional chemical methods of DNA sequencing that are based on electronic/ionic signatures would revolutionize the field of sequencing. The approach of a single molecule imaging and spectroscopy with unprecedented resolution, achieved by Scanning Tunneling Spectroscopy (STS) and nanopore electronics could enable this revolution. We use the data from our group and others in applying this local scanning tunneling microscopy and illustrate possibilities of electronic sequencing of freeze dried deposits on graphene. We will present two types of calculated fingerprints: first in Local Density of States (LDOS) of DNA nucleotide bases (A,C,G,T) deposited on graphene. Significant base-dependent features in the LDOS in an energy range within few eV of the Fermi level were found in our calculations. These features can serve as electronic fingerprints for the identification of individual bases in STS. In the second approach we present calculated base dependent electronic transverse conductance as DNA translocates through the graphene nanopore. Thus we argue that the fingerprints of DNA-graphene hybrid structures may provide an alternative route to DNA sequencing using STS. Work supported by US DOE, NORDITA.

  12. The Electronic Structure of Amorphous Carbon Nanodots.

    PubMed

    Margraf, Johannes T; Strauss, Volker; Guldi, Dirk M; Clark, Timothy

    2015-06-18

    We have studied hydrogen-passivated amorphous carbon nanostructures with semiempirical molecular orbital theory in order to provide an understanding of the factors that affect their electronic properties. Amorphous structures were first constructed using periodic calculations in a melt/quench protocol. Pure periodic amorphous carbon structures and their counterparts doped with nitrogen and/or oxygen feature large electronic band gaps. Surprisingly, descriptors such as the elemental composition and the number of sp(3)-atoms only influence the electronic structure weakly. Instead, the exact topology of the sp(2)-network in terms of effective conjugation defines the band gap. Amorphous carbon nanodots of different structures and sizes were cut out of the periodic structures. Our calculations predict the occurrence of localized electronic surface states, which give rise to interesting effects such as amphoteric reactivity and predicted optical band gaps in the near-UV/visible range. Optical and electronic gaps display a dependence on particle size similar to that of inorganic colloidal quantum dots. PMID:25731776

  13. Theoretical electronic structure of structurally modified graphene

    NASA Astrophysics Data System (ADS)

    Dvorak, Marc David

    Graphene has emerged as a promising replacement for silicon in next-generation electronics and optoelectronic devices. If graphene is to be used in semiconductor devices, however, it must acquire an electronic band gap. Numerous approaches have been proposed to control the band gap of graphene, including the periodic patterning of defects. However, the mechanism for band gap opening and the associated physics in graphene patterned with defects remain unclear. Using both analytic theory and first-principles calculations, we show that periodic patterning of defects on graphene can open a large and tunable band gap, induce strong absorption peaks at optical wavelengths, and host a giant band gap quantum spin Hall phase. First, a geometric rule is analytically derived for the arrangements of defects that open a band gap in graphene, with one ninth of all possible patterns opening a band gap. Next, we perform ab-initio density functional calculations to compare the effects of structural vacancies, hexagonal BN dopants, and passivants on the electronic structure of graphene. Qualitatively, these three types of structural defects behave the same, with only slight differences in their resulting band structures. By adjusting the shape of structural defects, we show how to move the Dirac cones in reciprocal space in accordance with the tight-binding model for the anisotropic honeycomb lattice, while the fundamental mechanism for band gap opening remains the same. To quantitatively predict the band gap and optical properties of these materials, we employ many-body perturbation theory with Green's functions (GW/Bethe-Salpeter equation) to directly include electron-electron and electron-hole interactions. Structurally modified graphene shows a strong renormalization of the fundamental band gap over single particle descriptions, and a strong electron-hole interaction as indicated by strong exciton binding energies (> 0.5 eV). Finally, we show that structurally modified graphene

  14. Nano-fEM: Protein Localization Using Photo-activated Localization Microscopy and Electron Microscopy

    PubMed Central

    Watanabe, Shigeki; Richards, Jackson; Hollopeter, Gunther; Hobson, Robert J.; Davis, Wayne M.; Jorgensen, Erik M.

    2012-01-01

    Mapping the distribution of proteins is essential for understanding the function of proteins in a cell. Fluorescence microscopy is extensively used for protein localization, but subcellular context is often absent in fluorescence images. Immuno-electron microscopy, on the other hand, can localize proteins, but the technique is limited by a lack of compatible antibodies, poor preservation of morphology and because most antigens are not exposed to the specimen surface. Correlative approaches can acquire the fluorescence image from a whole cell first, either from immuno-fluorescence or genetically tagged proteins. The sample is then fixed and embedded for electron microscopy, and the images are correlated 1-3. However, the low-resolution fluorescence image and the lack of fiducial markers preclude the precise localization of proteins. Alternatively, fluorescence imaging can be done after preserving the specimen in plastic. In this approach, the block is sectioned, and fluorescence images and electron micrographs of the same section are correlated 4-7. However, the diffraction limit of light in the correlated image obscures the locations of individual molecules, and the fluorescence often extends beyond the boundary of the cell. Nano-resolution fluorescence electron microscopy (nano-fEM) is designed to localize proteins at nano-scale by imaging the same sections using photo-activated localization microscopy (PALM) and electron microscopy. PALM overcomes the diffraction limit by imaging individual fluorescent proteins and subsequently mapping the centroid of each fluorescent spot 8-10. We outline the nano-fEM technique in five steps. First, the sample is fixed and embedded using conditions that preserve the fluorescence of tagged proteins. Second, the resin blocks are sectioned into ultrathin segments (70-80 nm) that are mounted on a cover glass. Third, fluorescence is imaged in these sections using the Zeiss PALM microscope. Fourth, electron dense structures are imaged

  15. Local spin dynamics with the electron electric dipole moment

    NASA Astrophysics Data System (ADS)

    Fukuda, Masahiro; Soga, Kota; Senami, Masato; Tachibana, Akitomo

    2016-01-01

    The local spin dynamics of the electron is studied from the viewpoint of the electric dipole moment (EDM) of the electron in the framework of the quantum field theory. The improvements of the computational accuracy of the effective electric field (Eeff) for the EDM and the understanding of spin precession are important for the experimental determination of the upper bound of the EDM. Calculations of Eeff in YbF (2Σ1 /2 ), BaF (2Σ1 /2 ), ThO (3Δ1 ), and HF+ (2Π1 /2 ) are performed on the basis of the restricted active space configuration interaction approach by using the four-component relativistic electronic structure calculation. The spin precession is also discussed from the viewpoint of local spin torque dynamics. We show that a contribution to the torque density for the spin is brought into by the EDM. Distributions of the local spin angular momentum density and torque densities induced by external fields in the above molecules are calculated and a property related with large Eeff is discussed.

  16. Electronic structure and correlation effects in actinides

    SciTech Connect

    Albers, R.C.

    1998-12-01

    This report consists of the vugraphs given at a conference on electronic structure. Topics discussed are electronic structure, f-bonding, crystal structure, and crystal structure stability of the actinides and how they are inter-related.

  17. Electron Scattering and Nuclear Structure

    ERIC Educational Resources Information Center

    Trower, W. P.; Ficenec, J. R.

    1971-01-01

    Presents information about the nucleus gained by studies of electron scattering. Discusses what can be implied about the shape of the charge distribution, the nucleus positions, the vibrational modes of the nucleus, the momentum of the nucleus, and the granularity and core structures of the nucleus. (DS)

  18. Electronic Structure Principles and Aromaticity

    ERIC Educational Resources Information Center

    Chattaraj, P. K.; Sarkar, U.; Roy, D. R.

    2007-01-01

    The relationship between aromaticity and stability in molecules on the basis of quantities such as hardness and electrophilicity is explored. The findings reveal that aromatic molecules are less energetic, harder, less polarizable, and less electrophilic as compared to antiaromatic molecules, as expected from the electronic structure principles.

  19. Structural and electronic properties of thallium compounds

    NASA Astrophysics Data System (ADS)

    Paliwal, Neetu; Srivastava, Vipul

    2016-05-01

    The tight binding linear muffin-tin-orbital (TB-LMTO) method within the local density approximation (LDA has been used to calculate structural and electronic properties of thallium pnictides TlX (X=Sb, Bi) at high pressure. As a function of volume, the total energy is evaluated. Apart from this, the lattice parameter (a0), bulk modulus (B0), band structure (BS) and density of states (DOS) are calculated. From energy band diagram we observed metallic behaviour in TlSb and TlBi compounds. The values of equilibrium lattice constants and bulk modulus are agreed well with the available data.

  20. Electron-electron interaction, weak localization and spin valve effect in vertical-transport graphene devices

    SciTech Connect

    Long, Mingsheng; Gong, Youpin; Wei, Xiangfei; Zhu, Chao; Xu, Jianbao; Liu, Ping; Guo, Yufen; Li, Weiwei; Liu, Liwei; Liu, Guangtong

    2014-04-14

    We fabricated a vertical structure device, in which graphene is sandwiched between two asymmetric ferromagnetic electrodes. The measurements of electron and spin transport were performed across the combined channels containing the vertical and horizontal components. The presence of electron-electron interaction (EEI) was found not only at low temperatures but also at moderate temperatures up to ∼120 K, and EEI dominates over weak localization (WL) with and without applying magnetic fields perpendicular to the sample plane. Moreover, spin valve effect was observed when magnetic filed is swept at the direction parallel to the sample surface. We attribute the EEI and WL surviving at a relatively high temperature to the effective suppress of phonon scattering in the vertical device structure. The findings open a way for studying quantum correlation at relatively high temperature.

  1. On the local electronic and atomic structure of Ce1-xPrxO2-δ epitaxial films on Si

    SciTech Connect

    Niu, Gang Schubert, Markus Andreas; Zoellner, Marvin Hartwig; D'Acapito, Francesco; Boscherini, Federico

    2014-09-28

    The local electronic and atomic structure of (111)-oriented, single crystalline mixed Ce1-xPrxO2-δ (x = 0, 0.1 and 0.6) epitaxial thin films on silicon substrates have been investigated in view of engineering redox properties of complex oxide films. Non-destructive X-ray absorption near edge structure reveals that Pr shows only +3 valence and Ce shows only nominal +4 valence in mixed oxides. Extended x-ray absorption fine structure (EXAFS) studies were performed at K edges of Ce and Pr using a specially designed monochromator system for high energy measurements. They demonstrate that the fluorite lattice of ceria (CeO₂) is almost not perturbed for x = 0.1 sample, while higher Pr concentration (x = 0.6) not only generates a higher disorder level (thus more disordered oxygen) but also causes a significant reduction of Ce–O interatomic distances. The valence states of the cations were also examined by techniques operating in highly reducing environments: scanning transmission electron microscopy-electron energy loss spectroscopy and X-ray photoemission spectroscopy; in these reducing environments, evidence for the presence of Ce³⁺ was clearly found for the higher Pr concentration. Thus, the introduction of Pr³⁺ into CeO₂ strongly enhances the oxygen exchange properties of CeO₂. This improved oxygen mobility properties of CeO₂ are attributed to the lattice disorder induced by Pr mixing in the CeO₂ fluorite lattice, as demonstrated by EXAFS measurements. Thus, a comprehensive picture of the modifications of the atomic and electronic structure of Ce1-xPrxO2-δ epitaxial films and their relation is obtained.

  2. Combinatorics of locally optimal RNA secondary structures.

    PubMed

    Fusy, Eric; Clote, Peter

    2014-01-01

    It is a classical result of Stein and Waterman that the asymptotic number of RNA secondary structures is 1.104366∙n-3/2∙2.618034n. Motivated by the kinetics of RNA secondary structure formation, we are interested in determining the asymptotic number of secondary structures that are locally optimal, with respect to a particular energy model. In the Nussinov energy model, where each base pair contributes -1 towards the energy of the structure, locally optimal structures are exactly the saturated structures, for which we have previously shown that asymptotically, there are 1.07427∙n-3/2∙2.35467n many saturated structures for a sequence of length n. In this paper, we consider the base stacking energy model, a mild variant of the Nussinov model, where each stacked base pair contributes -1 toward the energy of the structure. Locally optimal structures with respect to the base stacking energy model are exactly those secondary structures, whose stems cannot be extended. Such structures were first considered by Evers and Giegerich, who described a dynamic programming algorithm to enumerate all locally optimal structures. In this paper, we apply methods from enumerative combinatorics to compute the asymptotic number of such structures. Additionally, we consider analogous combinatorial problems for secondary structures with annotated single-stranded, stacking nucleotides (dangles). PMID:23263300

  3. Electronic properties of polycrystalline graphene under large local strain

    SciTech Connect

    He, Xin; Tang, Ning E-mail: geweikun@mail.tsinghua.edu.cn Duan, Junxi; Mei, Fuhong; Meng, Hu; Lu, Fangchao; Xu, Fujun; Yang, Xuelin; Gao, Li; Wang, Xinqiang; Shen, Bo E-mail: geweikun@mail.tsinghua.edu.cn; Ge, Weikun E-mail: geweikun@mail.tsinghua.edu.cn

    2014-06-16

    To explore the transport properties of polycrystalline graphene under large tensile strain, a strain device has been fabricated using piezocrystal to load local strain onto graphene, up to 22.5%. Ionic liquid gate whose capability of tuning carrier density being much higher than that of a solid gate is used to survey the transfer characteristics of the deformed graphene. The conductance of the Dirac point and field effect mobility of electrons and holes is found to decrease with increasing strain, which is attributed to the scattering of the graphene grain boundaries, the strain induced change of band structure, and defects. However, the transport gap is still not opened. Our study is helpful to evaluate the application of graphene in stretchable electronics.

  4. Electronic structure of lithium tetraborate

    NASA Astrophysics Data System (ADS)

    Wooten, David J.

    Due to many of its attributes, Li2B4O7 provides a possible material for incorporation as either a primary or companion material in future solid state neutron detectors. There is however a lack of fundamental characterization information regarding this useful material, particularly its electronic configuration. To address this, an investigation of Li2B4O7(110) and Li2B 4O7(100) was undertaken, utilizing photoemission and inverse photoemission spectroscopic techniques. The measured band gap depended on crystallographic direction with the band gaps ranging from 8.9+/-0.5 eV to 10.1+/-0.5 eV. The measurement yielded a density of states that qualitatively agreed with the theoretical results from model bulk band structure calculations for Li2B4O7; albeit with a larger band gap than predicted, but consistent with the known deficiencies of Local Density Approximation and Density Functional Theory calculations. The occupied states of both surfaces were extremely flat; to the degree that resolving periodic dispersion of the occupied states was inconclusive, within the resolution of the system. However, both surfaces demonstrated clear periodic dispersion within the empty states very close to theoretical Brillouin zone values. These attributes also translated to a lighter charge carrier effective mass in the unoccupied states. Of the two surfaces, Li2B4O 7(110) yielded the more consistent values in orthogonal directions for energy states. The presence of a bulk band gap surface state and image potential state in Li2B4O7(110) was indicative of a defect-free surface. The absence of both in the more polar, more dielectric Li2B4O7(100) was attributed to the presence of defects determined to be O vacancies. The results from Li2B 4O7(110) were indicative of a more stable surface than Li 2B4O7(100). In addition, Li 1s bulk and surface core level components were determined at the binding energies of -56.5+0.4 and -53.7+0.5 eV. Resonance features were observed along the [001

  5. Electronic structure tuning of diamondoids through functionalization

    NASA Astrophysics Data System (ADS)

    Rander, Torbjörn; Staiger, Matthias; Richter, Robert; Zimmermann, Tobias; Landt, Lasse; Wolter, David; Dahl, Jeremy E.; Carlson, Robert M. K.; Tkachenko, Boryslav A.; Fokina, Natalie A.; Schreiner, Peter R.; Möller, Thomas; Bostedt, Christoph

    2013-01-01

    We investigated the changes in electronic structures induced by chemical functionalization of the five smallest diamondoids using valence photoelectron spectroscopy. Through the variation of three parameters, namely functional group (thiol, hydroxy, and amino), host cluster size (adamantane, diamantane, triamantane, [121]tetramantane, and [1(2,3)4]pentamantane), and functionalization site (apical and medial) we are able to determine to what degree these affect the electronic structures of the overall systems. We show that unlike, for example, in the case of halobenzenes, the ionization potential does not show a linear dependence on the electronegativity of the functional group. Instead, a linear correlation exists between the HOMO-1 ionization potential and the functional group electronegativity. This is due to localization of the HOMO on the functional group and the HOMO-1 on the diamondoid cage. Density functional theory supports our interpretations.

  6. Sparse maps—A systematic infrastructure for reduced-scaling electronic structure methods. I. An efficient and simple linear scaling local MP2 method that uses an intermediate basis of pair natural orbitals.

    PubMed

    Pinski, Peter; Riplinger, Christoph; Valeev, Edward F; Neese, Frank

    2015-07-21

    In this work, a systematic infrastructure is described that formalizes concepts implicit in previous work and greatly simplifies computer implementation of reduced-scaling electronic structure methods. The key concept is sparse representation of tensors using chains of sparse maps between two index sets. Sparse map representation can be viewed as a generalization of compressed sparse row, a common representation of a sparse matrix, to tensor data. By combining few elementary operations on sparse maps (inversion, chaining, intersection, etc.), complex algorithms can be developed, illustrated here by a linear-scaling transformation of three-center Coulomb integrals based on our compact code library that implements sparse maps and operations on them. The sparsity of the three-center integrals arises from spatial locality of the basis functions and domain density fitting approximation. A novel feature of our approach is the use of differential overlap integrals computed in linear-scaling fashion for screening products of basis functions. Finally, a robust linear scaling domain based local pair natural orbital second-order Möller-Plesset (DLPNO-MP2) method is described based on the sparse map infrastructure that only depends on a minimal number of cutoff parameters that can be systematically tightened to approach 100% of the canonical MP2 correlation energy. With default truncation thresholds, DLPNO-MP2 recovers more than 99.9% of the canonical resolution of the identity MP2 (RI-MP2) energy while still showing a very early crossover with respect to the computational effort. Based on extensive benchmark calculations, relative energies are reproduced with an error of typically <0.2 kcal/mol. The efficiency of the local MP2 (LMP2) method can be drastically improved by carrying out the LMP2 iterations in a basis of pair natural orbitals. While the present work focuses on local electron correlation, it is of much broader applicability to computation with sparse tensors in

  7. Sparse maps—A systematic infrastructure for reduced-scaling electronic structure methods. I. An efficient and simple linear scaling local MP2 method that uses an intermediate basis of pair natural orbitals

    SciTech Connect

    Pinski, Peter; Riplinger, Christoph; Neese, Frank E-mail: frank.neese@cec.mpg.de; Valeev, Edward F. E-mail: frank.neese@cec.mpg.de

    2015-07-21

    In this work, a systematic infrastructure is described that formalizes concepts implicit in previous work and greatly simplifies computer implementation of reduced-scaling electronic structure methods. The key concept is sparse representation of tensors using chains of sparse maps between two index sets. Sparse map representation can be viewed as a generalization of compressed sparse row, a common representation of a sparse matrix, to tensor data. By combining few elementary operations on sparse maps (inversion, chaining, intersection, etc.), complex algorithms can be developed, illustrated here by a linear-scaling transformation of three-center Coulomb integrals based on our compact code library that implements sparse maps and operations on them. The sparsity of the three-center integrals arises from spatial locality of the basis functions and domain density fitting approximation. A novel feature of our approach is the use of differential overlap integrals computed in linear-scaling fashion for screening products of basis functions. Finally, a robust linear scaling domain based local pair natural orbital second-order Möller-Plesset (DLPNO-MP2) method is described based on the sparse map infrastructure that only depends on a minimal number of cutoff parameters that can be systematically tightened to approach 100% of the canonical MP2 correlation energy. With default truncation thresholds, DLPNO-MP2 recovers more than 99.9% of the canonical resolution of the identity MP2 (RI-MP2) energy while still showing a very early crossover with respect to the computational effort. Based on extensive benchmark calculations, relative energies are reproduced with an error of typically <0.2 kcal/mol. The efficiency of the local MP2 (LMP2) method can be drastically improved by carrying out the LMP2 iterations in a basis of pair natural orbitals. While the present work focuses on local electron correlation, it is of much broader applicability to computation with sparse tensors in

  8. Imaging Local Electronic Corrugations and Doped Regions in Graphene

    SciTech Connect

    B Schultz; C Patridge; V Lee; C Jaye; P Lysaght; C Smith; J Barnett; D Fischer; D Prendergast; S Banerjee

    2011-12-31

    Electronic structure heterogeneities are ubiquitous in two-dimensional graphene and profoundly impact the transport properties of this material. Here we show the mapping of discrete electronic domains within a single graphene sheet using scanning transmission X-ray microscopy in conjunction with ab initio density functional theory calculations. Scanning transmission X-ray microscopy imaging provides a wealth of detail regarding the extent to which the unoccupied levels of graphene are modified by corrugation, doping and adventitious impurities, as a result of synthesis and processing. Local electronic corrugations, visualized as distortions of the {pi}*cloud, have been imaged alongside inhomogeneously doped regions characterized by distinctive spectral signatures of altered unoccupied density of states. The combination of density functional theory calculations, scanning transmission X-ray microscopy imaging, and in situ near-edge X-ray absorption fine structure spectroscopy experiments also provide resolution of a longstanding debate in the literature regarding the spectral assignments of pre-edge and interlayer states.

  9. The Local Physical Structure of Amorphous Boron Carbide Thin Films

    NASA Astrophysics Data System (ADS)

    Paquette, M. M.; Li, Wenjing; Driver, M. S.; Oyler, N. A.; Caruso, A. N.

    2011-03-01

    Thin-film amorphous hydrogenated boron carbide (a-B5 C:Hx) and technical boron carbide (B4 C:Cy) are important materials in next-generation solid-state neutron detectors and refractory electronics. Optimizing the electrical carrier transport and electronic structure of these films for the stated applications has been severely hindered by: (1) their lack of long-range periodicity; (2) the ability of boron-rich solids to form complex polyhedra; and, (3) the possibility that carbon atoms incorporate into the polyhedral structures in an intraicosahedral fashion or that they bridge polyhedral structures in an intericosahedral fashion. The use of traditional spectroscopies that are sensitive to local coordination environment have been inadequate in the determination of the local physical structure because of either poor resolution or very low interaction cross sections. However, magic spinning angle (MAS) solid-state nuclear magnetic resonance (SSNMR), does have the signal-to-noise and rigor to extract the local physical coordination structure of these materials, despite the challenges associated with deltahedra-based structures. This poster will describe the progress and challenges in structure determination through a comparison of unknown samples to known calibration standards using MAS techniques, in the context of furthering the general understanding of the electronic structure of a-B5 C:Hx and B4 C:Cy thin films.

  10. Local atomic and electronic structure of oxide/GaAs and SiO2/Si interfaces using high-resolution XPS

    NASA Technical Reports Server (NTRS)

    Grunthaner, F. J.; Grunthaner, P. J.; Vasquez, R. P.; Lewis, B. F.; Maserjian, J.; Madhukar, A.

    1979-01-01

    The chemical structures of thin SiO2 films, thin native oxides of GaAs (20-30 A), and the respective oxide-semiconductor interfaces, have been investigated using high-resolution X-ray photoelectron spectroscopy. Depth profiles of these structures have been obtained using argon ion bombardment and wet chemical etching techniques. The chemical destruction induced by the ion profiling method is shown by direct comparison of these methods for identical samples. Fourier transform data-reduction methods based on linear prediction with maximum entropy constraints are used to analyze the discrete structure in oxides and substrates. This discrete structure is interpreted by means of a structure-induced charge-transfer model.

  11. Electronic and structural properties of metallic microclusters

    SciTech Connect

    Maiti, A.

    1992-04-01

    The first part of this thesis presents a first-order pseudopotential calculation at T=O of the total energy of small sodium clusters of size N<800. The calculation is based on a local-pseudopotential scheme and local-density correlation and exchange. A temperature-size (T-N) phase-diagram is then derived using the T=O results and Lindemann`s criterion for melting. The phase-diagram contains three regions of stability: (1) a liquid (jellium) phase at temperatures above the melting line T{sub M}(N) where cluster-stability occurs at electronic magic numbers: (2) a phase related to complete geometrical shells of body-centered-cubic structure at temperatures below the melting line; and (3) a close-packed structure at very low temperatures and sufficiently large N. The melting line drops to T{sub M}(N)=O for N<65, where electronic magic numbers are stable even at T=O. The phase diagram reduces asymptotically to the known phases of sodium as N{yields}{infinity}, including the known martensitic transformation at T{approximately}5 K. The second and the last part of this thesis consists of a study of small-cluster many-body systems by means of an on-site ``local`` chemical potential which allows the continuous variation of local electron-density. This method yields a criterion to distinguish particular features of a small cluster that are likely to survive in the large-N thermodynamic limit from those discontinuities that arise only from finite-size effects.

  12. Electronic and structural properties of metallic microclusters

    SciTech Connect

    Maiti, A.

    1992-04-01

    The first part of this thesis presents a first-order pseudopotential calculation at T=O of the total energy of small sodium clusters of size N<800. The calculation is based on a local-pseudopotential scheme and local-density correlation and exchange. A temperature-size (T-N) phase-diagram is then derived using the T=O results and Lindemann's criterion for melting. The phase-diagram contains three regions of stability: (1) a liquid (jellium) phase at temperatures above the melting line T{sub M}(N) where cluster-stability occurs at electronic magic numbers: (2) a phase related to complete geometrical shells of body-centered-cubic structure at temperatures below the melting line; and (3) a close-packed structure at very low temperatures and sufficiently large N. The melting line drops to T{sub M}(N)=O for N<65, where electronic magic numbers are stable even at T=O. The phase diagram reduces asymptotically to the known phases of sodium as N{yields}{infinity}, including the known martensitic transformation at T{approximately}5 K. The second and the last part of this thesis consists of a study of small-cluster many-body systems by means of an on-site local'' chemical potential which allows the continuous variation of local electron-density. This method yields a criterion to distinguish particular features of a small cluster that are likely to survive in the large-N thermodynamic limit from those discontinuities that arise only from finite-size effects.

  13. Structural Dynamics of Electronic Systems

    NASA Astrophysics Data System (ADS)

    Suhir, E.

    2013-03-01

    The published work on analytical ("mathematical") and computer-aided, primarily finite-element-analysis (FEA) based, predictive modeling of the dynamic response of electronic systems to shocks and vibrations is reviewed. While understanding the physics of and the ability to predict the response of an electronic structure to dynamic loading has been always of significant importance in military, avionic, aeronautic, automotive and maritime electronics, during the last decade this problem has become especially important also in commercial, and, particularly, in portable electronics in connection with accelerated testing of various surface mount technology (SMT) systems on the board level. The emphasis of the review is on the nonlinear shock-excited vibrations of flexible printed circuit boards (PCBs) experiencing shock loading applied to their support contours during drop tests. At the end of the review we provide, as a suitable and useful illustration, the exact solution to a highly nonlinear problem of the dynamic response of a "flexible-and-heavy" PCB to an impact load applied to its support contour during drop testing.

  14. Local Electronic And Dielectric Properties at Nanosized Interfaces

    SciTech Connect

    Bonnell, Dawn A.

    2015-02-23

    Final Report to the Department of Energy for period 6/1/2000 to 11/30/2014 for Grant # DE-FG02-00ER45813-A000 to the University of Pennsylvania Local Electronic And Dielectric Properties at Nanosized Interfaces PI: Dawn Bonnell The behavior of grain boundaries and interfaces has been a focus of fundamental research for decades because variations of structure and composition at interfaces dictate mechanical, electrical, optical and dielectric properties in solids. Similarly, the consequence of atomic and electronic structures of surfaces to chemical and physical interactions are critical due to their implications to catalysis and device fabrication. Increasing fundamental understanding of surfaces and interfaces has materially advanced technologies that directly bear on energy considerations. Currently, exciting developments in materials processing are enabling creative new electrical, optical and chemical device configurations. Controlled synthesis of nanoparticles, semiconducting nanowires and nanorods, optical quantum dots, etc. along with a range of strategies for assembling and patterning nanostructures portend the viability of new devices that have the potential to significantly impact the energy landscape. As devices become smaller the impact of interfaces and surfaces grows geometrically. As with other nanoscale phenomena, small interfaces do not exhibit the same properties as do large interfaces. The size dependence of interface properties had not been explored and understanding at the most fundamental level is necessary to the advancement of nanostructured devices. An equally important factor in the behavior of interfaces in devices is the ability to examine the interfaces under realistic conditions. For example, interfaces and boundaries dictate the behavior of oxide fuel cells which operate at extremely high temperatures in dynamic high pressure chemical environments. These conditions preclude the characterization of local properties during fuel cell

  15. Electronic structure of graphite oxide

    NASA Astrophysics Data System (ADS)

    Jeong, Hae Kyung; Yang, Cheolsoo; Kim, Bong Soo; Kim, Ki-Jeong

    2011-03-01

    We have investigated the electronic structure of graphite oxide by photoelectron spectroscopy at the Pohang Accelerator Laboratory, Korea. The typical sp 2 hybridization states found in graphite were also seen in graphite oxide. However, the π state disappeared near the Fermi level because of bonding between the π and oxygen-related states originating from graphite oxide, indicating electron transfer from graphite to oxygen and resulting in a downward shift of the highest occupied molecular orbital (HOMO) state to higher binding energies. The band gap opening increased to about 1.8 eV, and additional oxygen-related peaks were observed at 8.5 and 27 eV. This research was supported by the Basic Science Program through the National Research Foundation of Korea (NRF), funded by the Ministry of Education, Science and Technology (2010-0004592), and partly by the MEST (2009-0087138). Experiments at the PLS were supported in part by POSTECH and MEST.

  16. Electronic instrumentation for smart structures

    NASA Astrophysics Data System (ADS)

    Blanar, George J.

    1995-04-01

    The requirements of electronic instrumentation for smart structures are similar to those of data acquisition systems at our national particle physics laboratories. Modern high energy and heavy ion physics experiments may have tens of thousands of channels of data sources producing data that must be converted to digital form, compacted, stored and interpreted. In parallel, multiple sensors distributed in and around smart structures generate either binary or analog signals that are voltage, charge, or time like in their information content. In all cases, they must be transmitted, converted and preserved into a unified digital format for real-time processing. This paper will review the current status of practical large scale electronic measurement systems with special attention to architectures and physical organization. Brief surveys of the current state of the art will include preamplifiers and amplifiers, comparators and discriminators, voltage or charge analog-to-digital converters, time internal meters or time-to-digital converters, and finally, counting or scalar systems. The paper will conclude by integrating all of these ideas in a concept for an all-digital readout of a smart structure using the latest techniques used in physics research today.

  17. Electronic structure of cobalt nanocrystals suspended inliquid

    SciTech Connect

    Liu, Hongjian; Guo, Jinghua; Yin, Yadong; Augustsson, Andreas; Dong, Chungli; Nordgren, Joseph; Chang, Chinglin; Alivisatos, Paul; Thornton, Geoff; Ogletree, D. Frank; Requejo, Felix G.; de Groot, Frank; Salmeron, Miquel

    2007-07-16

    The electronic structure of cobalt nanocrystals suspended in liquid as a function of size has been investigated using in-situ x-ray absorption and emission spectroscopy. A sharp absorption peak associated with the ligand molecules is found that increases in intensity upon reducing the nanocrystal size. X-ray Raman features due to d-d and to charge-transfer excitations of ligand molecules are identified. The study reveals the local symmetry of the surface of {var_epsilon}-Co phase nanocrystals, which originates from a dynamic interaction between Co nanocrystals and surfactant + solvent molecules.

  18. Local structural origins of the distinct electronic properties of Nb-substituted SrTiO3 and BaTiO3

    SciTech Connect

    Proffen, Thomas E; Page, Katharine L; Kolodiazhnyi, Taras; Cheetham, Anthony K; Seshadri, R

    2008-01-01

    Relating the minute details of crystal and defect structures to the properties of transition metal oxides is a central preoccupation in condensed matter science. Aiding in these efforts have been the many significant advances in high resolution and high momentum transfer neutron diffraction, which today provide unprecedented precision in describing the location of atoms in functional materials.

  19. Local density functional calculations of the electronic structures of the intermetallic systems U{sub 2}Fe{sub 2}Sn and UFe{sub 2}Ge{sub 2}

    SciTech Connect

    Matar, S.F.; Chevalier, B.; Etourneau, J.; Eyert, V.

    1997-02-05

    The electronic structures of U{sub 2}Fe{sub 2}Sn and UFe{sub 2}Ge{sub 2} are self-consistently calculated within the local density functional theory using the augmented spherical wave (ASW) method. Calculations are scalar relativistic. The experimentally observed Pauli paramagnetic behavior of the two systems is accounted for and the influence of hybridization between the different l-states on the chemical bonding is discussed from the site-projected densities of states (DOS) as well as from the modulation of the DOS by the sign and magnitude of the overlap integral, i.e., with the so-called COOP. From this, we propose a mechanism for the evolution of bonding within the series to which the two compounds belong. 12 refs., 3 figs.

  20. Introduction: Dissipative localized structures in extended systems

    NASA Astrophysics Data System (ADS)

    Tlidi, Mustapha; Taki, Majid; Kolokolnikov, Theodore

    2007-09-01

    Localized structures belong to the class of dissipative structures found far from equilibrium. Contributions from the most representative groups working on a various fields of natural science such as biology, chemistry, plant ecology, mathematics, optics, and laser physics are presented. The aim of this issue is to gather specialists from these fields towards a cross-fertilization among these active areas of research and thereby to present an overview of the state of art in the formation and the characterization of dissipative localized structures. Nonlinear optics and laser physics have an important part in this issue because of potential applications in information technology. In particular, localized structures could be used as "bits" for parallel information storage and processing.

  1. High-resolution Mn K -edge x-ray emission and absorption spectroscopy study of the electronic and local structure of the three different phases in N d0.5S r0.5Mn O3

    NASA Astrophysics Data System (ADS)

    Lafuerza, S.; García, J.; Subías, G.; Blasco, J.; Glatzel, P.

    2016-05-01

    N d0.5S r0.5Mn O3 is particularly representative of mixed-valent manganites since their three characteristic macroscopic phases (charge-ordered insulator, ferromagnetic-metallic, and paramagnetic insulator) appear at different temperatures. We here report a complete x-ray emission and absorption spectroscopy (XES-XAS) study of N d0.5S r0.5Mn O3 as a function of temperature to investigate the electronic and local structure changes of the Mn atom in these three phases. Compared with the differences in the XES-XAS spectra between N d0.5S r0.5Mn O3 and the single-valent reference compounds NdMn O3 (M n3 + ) and Sr/CaMn O3 (M n4 + ), only modest changes have been obtained across the magnetoelectrical transitions. The XES spectra, including both the Mn Kα and Kβ emission lines, have mainly shown a subtle decrease in the local spin density accompanying the passage to the ferromagnetic-metallic phase. For the same phase, the small intensity variations in the pre-edge region of the high-resolution XAS spectra reflect an increase of the p -d mixing. The analysis of these XAS spectra imply a charge segregation between the two different Mn sites far from one electron, being in intermediate valences M n+3.5 ±δ /2(δ <0.2 e -) for all the phases. Our results indicate that the spin, charge, and geometrical structure of the Mn atom hardly change among the three macroscopic phases demonstrating the strong competition between the ferromagnetic conductor and the charge-ordered insulator behaviors in the manganites.

  2. The study of local atomic and electronic structure with magnetic properties of Bi(Fe0.95Co0.05)O3 ceramics

    NASA Astrophysics Data System (ADS)

    Li, Yongtao; Zhang, Hongguang; Liu, Hao; Li, Qi; Li, Xing'ao; Mao, Weiwei; Wang, Xingfu; Xu, Qingyu; Wei, Shiqiang

    2013-01-01

    The origin of the room-temperature ferromagnetism of Bi(Fe1-xCox)O3 (x=0, 0.05) has been investigated by X-ray Absorption Fine Structure (XAFS) and Soft X-ray Absorption Spectroscopy (SXAS). The results of XAFS data indicate that partial Fe cations occupy Bi-sites of lattices and the dopant Co cations occupy Fe-sites. The existence of divalent Fe2+ ions in this system is detected. The O1s core level SXAS spectra indicate the crystal field split energy for x=0.05 sample is larger than that for x=0 sample, which means a structural distortion. The origin of ferromagnetism in both samples is related to the existence of Fe2+ ions, crystal lattice distortion and occupation of Fe ions. To the enhancement of saturated magnetizations in the Co-doped sample, the existence of Fe2+ ions is not the dominant factor, while the crystal lattice distortion due to partial Fe ions occupying at Bi-sites plays an important role.

  3. Protein localization in electron micrographs using fluorescence nanoscopy

    PubMed Central

    Watanabe, Shigeki; Punge, Annedore; Hollopeter, Gunther; Willig, Katrin I.; Hobson, Robert John; Davis, M. Wayne; Hell, Stefan W.; Jorgensen, Erik M.

    2010-01-01

    A complete portrait of a cell requires a detailed description of its molecular topography: proteins must be linked to particular organelles. Immuno-electron microscopy can reveal locations of proteins with nanometer resolution but is limited by the quality of fixation, the paucity of antibodies, and the inaccessibility of the antigens. Here, we describe correlative fluorescence electron microscopy for the nanoscopic localization of proteins in electron micrographs. Proteins tagged with Citrine or tdEos were expressed in Caenorhabditis elegans, fixed and embedded. Tagged proteins were imaged from ultrathin sections using stimulated emission depletion microscopy (STED) or photoactivated localization microscopy (PALM). Fluorescence was correlated with organelles imaged in electron micrographs from the same sections. These methods were used to successfully localize histones, a mitochondrial protein, and a presynaptic dense projection protein in electron micrographs. PMID:21102453

  4. Patterns and localized structures in population dynamics

    NASA Astrophysics Data System (ADS)

    Clerc, M. G.; Escaff, D.; Kenkre, V. M.

    2005-11-01

    Patterns, fronts, and localized structures of a prototypical model for population dynamics interaction are studied. The physical content of the model is the coexistence of a simple random walk for the motion of the individuals with a nonlinearity in the competitive struggle for resources which simultaneously stresses the Allee effect and interaction at a distance. Mathematically, the model is variational and exhibits coexistence between different stable extended states. Solutions are obtained, the phase diagram is constructed, and the emergence of localized structures is investigated.

  5. Think Locally: A Prudent Approach to Electronic Resource Management Systems

    ERIC Educational Resources Information Center

    Gustafson-Sundell, Nat

    2011-01-01

    A few articles have drawn some amount of attention specifically to the local causes of the success or failure of electronic resource management system (ERMS) implementations. In fact, it seems clear that local conditions will largely determine whether any given ERMS implementation will succeed or fail. This statement might seem obvious, but the…

  6. Local backbone structure prediction of proteins.

    PubMed

    de Brevern, Alexandre G; Benros, Cristina; Gautier, Romain; Valadié, Héléne; Hazout, Serge; Etchebest, Catherine

    2004-01-01

    A statistical analysis of the PDB structures has led us to define a new set of small 3D structural prototypes called Protein Blocks (PBs). This structural alphabet includes 16 PBs, each one is defined by the (phi, psi) dihedral angles of 5 consecutive residues. The amino acid distributions observed in sequence windows encompassing these PBs are used to predict by a Bayesian approach the local 3D structure of proteins from the sole knowledge of their sequences. LocPred is a software which allows the users to submit a protein sequence and performs a prediction in terms of PBs. The prediction results are given both textually and graphically. PMID:15724288

  7. Electronic structure theory of weakly interacting bilayers

    NASA Astrophysics Data System (ADS)

    Fang, Shiang; Kaxiras, Efthimios

    2016-06-01

    We derive electronic structure models for weakly interacting bilayers such as graphene-graphene and graphene-hexagonal boron nitride, based on density functional theory calculations followed by Wannier transformation of electronic states. These transferable interlayer coupling models can be applied to investigate the physics of bilayers with arbitrary translations and twists. The functional form, in addition to the dependence on the distance, includes the angular dependence that results from higher angular momentum components in the Wannier pz orbitals. We demonstrate the capabilities of the method by applying it to a rotated graphene bilayer, which produces the analytically predicted renormalization of the Fermi velocity, Van Hove singularities in the density of states, and moiré pattern of the electronic localization at small twist angles. We further extend the theory to obtain the effective couplings by integrating out neighboring layers. This approach is instrumental for the design of van der Walls heterostructures with desirable electronic features and transport properties and for the derivation of low-energy theories for graphene stacks, including proximity effects from other layers.

  8. The electron localization as the information content of the conditional pair density

    NASA Astrophysics Data System (ADS)

    Urbina, Andres S.; Torres, F. Javier; Rincon, Luis

    2016-06-01

    In the present work, the information gained by an electron for "knowing" about the position of another electron with the same spin is calculated using the Kullback-Leibler divergence (DKL) between the same-spin conditional pair probability density and the marginal probability. DKL is proposed as an electron localization measurement, based on the observation that regions of the space with high information gain can be associated with strong correlated localized electrons. Taking into consideration the scaling of DKL with the number of σ-spin electrons of a system (Nσ), the quantity χ = (Nσ - 1) DKLfcut is introduced as a general descriptor that allows the quantification of the electron localization in the space. fcut is defined such that it goes smoothly to zero for negligible densities. χ is computed for a selection of atomic and molecular systems in order to test its capability to determine the region in space where electrons are localized. As a general conclusion, χ is able to explain the electron structure of molecules on the basis of chemical grounds with a high degree of success and to produce a clear differentiation of the localization of electrons that can be traced to the fluctuation in the average number of electrons in these regions.

  9. The electron localization as the information content of the conditional pair density.

    PubMed

    Urbina, Andres S; Torres, F Javier; Rincon, Luis

    2016-06-28

    In the present work, the information gained by an electron for "knowing" about the position of another electron with the same spin is calculated using the Kullback-Leibler divergence (DKL) between the same-spin conditional pair probability density and the marginal probability. DKL is proposed as an electron localization measurement, based on the observation that regions of the space with high information gain can be associated with strong correlated localized electrons. Taking into consideration the scaling of DKL with the number of σ-spin electrons of a system (N(σ)), the quantity χ = (N(σ) - 1) DKLfcut is introduced as a general descriptor that allows the quantification of the electron localization in the space. fcut is defined such that it goes smoothly to zero for negligible densities. χ is computed for a selection of atomic and molecular systems in order to test its capability to determine the region in space where electrons are localized. As a general conclusion, χ is able to explain the electron structure of molecules on the basis of chemical grounds with a high degree of success and to produce a clear differentiation of the localization of electrons that can be traced to the fluctuation in the average number of electrons in these regions. PMID:27369494

  10. Fast probe of local electronic states in nanostructures utilizing a single-lead quantum dot

    PubMed Central

    Otsuka, Tomohiro; Amaha, Shinichi; Nakajima, Takashi; Delbecq, Matthieu R.; Yoneda, Jun; Takeda, Kenta; Sugawara, Retsu; Allison, Giles; Ludwig, Arne; Wieck, Andreas D.; Tarucha, Seigo

    2015-01-01

    Transport measurements are powerful tools to probe electronic properties of solid-state materials. To access properties of local electronic states in nanostructures, such as local density of states, electronic distribution and so on, micro-probes utilizing artificial nanostructures have been invented to perform measurements in addition to those with conventional macroscopic electronic reservoirs. Here we demonstrate a new kind of micro-probe: a fast single-lead quantum dot probe, which utilizes a quantum dot coupled only to the target structure through a tunneling barrier and fast charge readout by RF reflectometry. The probe can directly access the local electronic states with wide bandwidth. The probe can also access more electronic states, not just those around the Fermi level, and the operations are robust against bias voltages and temperatures. PMID:26416582

  11. Fast probe of local electronic states in nanostructures utilizing a single-lead quantum dot

    NASA Astrophysics Data System (ADS)

    Otsuka, Tomohiro; Amaha, Shinichi; Nakajima, Takashi; Delbecq, Matthieu R.; Yoneda, Jun; Takeda, Kenta; Sugawara, Retsu; Allison, Giles; Ludwig, Arne; Wieck, Andreas D.; Tarucha, Seigo

    2015-09-01

    Transport measurements are powerful tools to probe electronic properties of solid-state materials. To access properties of local electronic states in nanostructures, such as local density of states, electronic distribution and so on, micro-probes utilizing artificial nanostructures have been invented to perform measurements in addition to those with conventional macroscopic electronic reservoirs. Here we demonstrate a new kind of micro-probe: a fast single-lead quantum dot probe, which utilizes a quantum dot coupled only to the target structure through a tunneling barrier and fast charge readout by RF reflectometry. The probe can directly access the local electronic states with wide bandwidth. The probe can also access more electronic states, not just those around the Fermi level, and the operations are robust against bias voltages and temperatures.

  12. Basis functions for electronic structure calculations on spheres.

    PubMed

    Gill, Peter M W; Loos, Pierre-François; Agboola, Davids

    2014-12-28

    We introduce a new basis function (the spherical Gaussian) for electronic structure calculations on spheres of any dimension D. We find general expressions for the one- and two-electron integrals and propose an efficient computational algorithm incorporating the Cauchy-Schwarz bound. Using numerical calculations for the D = 2 case, we show that spherical Gaussians are more efficient than spherical harmonics when the electrons are strongly localized. PMID:25554128

  13. Structure Process, Weak Values and Local Momentum

    NASA Astrophysics Data System (ADS)

    Hiley, B. J.

    2016-03-01

    We explain how weak values and the local momentum can be better understood in terms of Bohm's notion of structure process. The basic ideas of this approach can be expressed in a fully algebraic way, generalising Heisenberg's original matrix mechanics. This approach leads to questions that are now being experimentally investigated by our group at University College London.

  14. Detecting structure of haplotypes and local ancestry

    Technology Transfer Automated Retrieval System (TEKTRAN)

    We present a two-layer hidden Markov model to detect the structure of haplotypes for unrelated individuals. This allows us to model two scales of linkage disequilibrium (one within a group of haplotypes and one between groups), thereby taking advantage of rich haplotype information to infer local an...

  15. Localized electron heating by strong guide-field magnetic reconnection

    NASA Astrophysics Data System (ADS)

    Guo, Xuehan; Inomoto, Michiaki; Sugawara, Takumichi; Yamasaki, Kotaro; Ushiki, Tomohiko; Ono, Yasushi

    2015-10-01

    Localized electron heating of magnetic reconnection was studied under strong guide-field using two merging spherical tokamak plasmas in the University of Tokyo Spherical Tokamak experiment. Our new slide-type two-dimensional Thomson scattering system is documented for the first time the electron heating localized around the X-point. Shape of the high electron temperature area does not agree with that of energy dissipation term Et.jt . If we include a guide-field effect term Bt/(Bp+αBt) for Et.jt , the energy dissipation area becomes localized around the X-point, suggesting that the electrons are accelerated by the reconnection electric field parallel to the magnetic field and thermalized around the X-point.

  16. Electronic Structure of B12 coenzymes

    NASA Astrophysics Data System (ADS)

    Ouyang, Lizhi; Ching, W. Y.; Randaccio, Lucio

    2001-06-01

    We have carried out an ab-initio local density functional calculations of the two most important B12 coenzymes, adoensyl-cobalamin (Ado-Cbl) and methyl-cobalamin (Me-Cbl). The crystal structures were determined by accurate X-ray synchrotron radiation measurements. Both crystals have space group P2121 with four molecules, or about 800 atoms, per unit cell. Our electronic structure calculation is based on one full molecule including the side chains. Results are analyzed in terms of atom and orbital resolved partial density of states (PDOS), Mulliken effective charges and bond orders. The PDOS analysis shows that the Co complexes of both B12 coenzymes had a HOMO/LUMO gap of about 1.5 eV. The Co-C bond order in Me-Cbl is smaller than that in Ado-Cbl. This appears to be in contradiction with the measured bond dissociated energies. However, this could also indicate the importance of the effects of solvents, which were not included in the calculation. We are investigating whether the effect of the solvents could dramatically modify the electronic structures of Ado-Cbl and Me-Cbl.

  17. Local structures of homogeneous Hall MHD turbulence

    NASA Astrophysics Data System (ADS)

    Miura, H.; Araki, K.

    2011-12-01

    Local structures of decaying homogeneous and isotropic Hall MHD turbulence are studied by means of direct numerical simulations. Regions of strong vorticity and strong current density in Hall MHD turbulence are compared to those of single-fluid MHD turbulence. An analysis by the use of a low-pass filter reveals that the introduction of the Hall term can modify not only small-scale structures of the current density but also structures of the vorticity field, especially at the scales smaller than the ion skin depth.

  18. Electron localization in self-assembled Si quantum dots grown on Ge(111)

    NASA Astrophysics Data System (ADS)

    Stepina, N. P.; Zinovieva, A. F.; Zinovyev, V. A.; Deryabin, A. S.; Kulik, L. V.; Dvurechenskii, A. V.

    2015-12-01

    Electron localization in a Si/Ge heterosystem with Si quantum dots (QDs) was studied by transport and electron spin resonance (ESR) measurements. For Si QD structures grown on Ge(111) substrates, the ESR signal with a g-factor g=2.0022+/- 0.0001 and ESR line width {{Δ }}H≈ 1.2 Oe was observed and attributed to the electrons localized in QDs. The g-factor value was explained taking into account the energy band modification due to both strain and quantum confinement. The transport behavior confirms the efficient electron localization in QDs for a Si/Ge(111) system. A strong Ge-Si intermixing in QD structures grown on Ge(001) is assumed to be the main reason for an unobserved ESR signal from the QDs.

  19. A structural alphabet for local protein structures: improved prediction methods.

    PubMed

    Etchebest, Catherine; Benros, Cristina; Hazout, Serge; de Brevern, Alexandre G

    2005-06-01

    Three-dimensional protein structures can be described with a library of 3D fragments that define a structural alphabet. We have previously proposed such an alphabet, composed of 16 patterns of five consecutive amino acids, called Protein Blocks (PBs). These PBs have been used to describe protein backbones and to predict local structures from protein sequences. The Q16 prediction rate reaches 40.7% with an optimization procedure. This article examines two aspects of PBs. First, we determine the effect of the enlargement of databanks on their definition. The results show that the geometrical features of the different PBs are preserved (local RMSD value equal to 0.41 A on average) and sequence-structure specificities reinforced when databanks are enlarged. Second, we improve the methods for optimizing PB predictions from sequences, revisiting the optimization procedure and exploring different local prediction strategies. Use of a statistical optimization procedure for the sequence-local structure relation improves prediction accuracy by 8% (Q16 = 48.7%). Better recognition of repetitive structures occurs without losing the prediction efficiency of the other local folds. Adding secondary structure prediction improved the accuracy of Q16 by only 1%. An entropy index (Neq), strongly related to the RMSD value of the difference between predicted PBs and true local structures, is proposed to estimate prediction quality. The Neq is linearly correlated with the Q16 prediction rate distributions, computed for a large set of proteins. An "expected" prediction rate QE16 is deduced with a mean error of 5%. PMID:15822101

  20. Towards scalable electronic structure calculations for alloys

    SciTech Connect

    Stocks, G.M.; Nicholson, D.M.C.; Wang, Y.; Shelton, W.A.; Szotek, Z.; Temmermann, W.M.

    1994-06-01

    A new approach to calculating the properties of large systems within the local density approximation (LDA) that offers the promise of scalability on massively parallel supercomputers is outlined. The electronic structure problem is formulated in real space using multiple scattering theory. The standard LDA algorithm is divided into two parts. Firstly, finding the self-consistent field (SCF) electron density, Secondly, calculating the energy corresponding to the SCF density. We show, at least for metals and alloys, that the former problem is easily solved using real space methods. For the second we take advantage of the variational properties of a generalized Harris-Foulkes free energy functional, a new conduction band Fermi function, and a fictitious finite electron temperature that again allow us to use real-space methods. Using a compute-node {R_arrow} atom equivalence the new method is naturally highly parallel and leads to O(N) scaling where N is the number of atoms making up the system. We show scaling data gathered on the Intel XP/S 35 Paragon for systems up to 512-atoms/simulation cell. To demonstrate that we can achieve metallurgical-precision, we apply the new method to the calculation the energies of disordered CuO{sub 0.5}Zn{sub 0.5} alloys using a large random sample.

  1. Local representation of the electronic dielectric response function

    DOE PAGESBeta

    Lu, Deyu; Ge, Xiaochuan

    2015-12-11

    We present a local representation of the electronic dielectric response function, based on a spatial partition of the dielectric response into contributions from each occupied Wannier orbital using a generalized density functional perturbation theory. This procedure is fully ab initio, and therefore allows us to rigorously define local metrics, such as “bond polarizability,” on Wannier centers. We show that the locality of the bare response function is determined by the locality of three quantities: Wannier functions of the occupied manifold, the density matrix, and the Hamiltonian matrix. Furthermore, in systems with a gap, the bare dielectric response is exponentially localized,more » which supports the physical picture of the dielectric response function as a collection of interacting local responses that can be captured by a tight-binding model.« less

  2. Local representation of the electronic dielectric response function

    SciTech Connect

    Lu, Deyu; Ge, Xiaochuan

    2015-12-11

    We present a local representation of the electronic dielectric response function, based on a spatial partition of the dielectric response into contributions from each occupied Wannier orbital using a generalized density functional perturbation theory. This procedure is fully ab initio, and therefore allows us to rigorously define local metrics, such as “bond polarizability,” on Wannier centers. We show that the locality of the bare response function is determined by the locality of three quantities: Wannier functions of the occupied manifold, the density matrix, and the Hamiltonian matrix. Furthermore, in systems with a gap, the bare dielectric response is exponentially localized, which supports the physical picture of the dielectric response function as a collection of interacting local responses that can be captured by a tight-binding model.

  3. Kinetic effects on robustness of electron magnetohydrodynamic structures

    SciTech Connect

    Hata, M.; Sakagami, H.; Das, A.

    2013-04-15

    Following recent remarkable progress in the development of high-power short-pulse lasers, exploration is ongoing into hitherto unknown phenomena at fast time scales of electrons, the understanding of which is becoming crucial. For a simplified description of such phenomena, the Electron Magnetohydrodynamics (EMHDs) fluid description is often adopted. For the possibility of electron transport in high-density plasma, exact solutions of the EMHD model in the form of electron vortex currents, together with their associated magnetic fields, have been considered. However, the fluid EMHD model does not incorporate kinetic effects. Here, the finite Larmor radius effects owing to a finite electron temperature on the robustness of the exact EMHD structures are investigated using two-dimensional particle-in-cell simulations. It is found that larger EMHD vortex structures can sustain themselves for long periods, even in high temperature plasma; however, sustaining structures at higher temperatures tends to be difficult. With increasing temperature, electrons with finite Larmor radii become disengaged from the localized region. It is also shown that structures localized in smaller regions are more difficult to sustain. A quantitative criterion in terms of the structure size and Larmor radius has been established by simulations over a wide range of parameters. Finally, we conclude that a structure, larger than about eight times the typical Larmor radius at r=R, could form and exist even under the effects of finite electron temperature.

  4. Electronic structure of herbicides: Atrazine and bromoxynil

    NASA Astrophysics Data System (ADS)

    Novak, Igor; Kovač, Branka

    2011-06-01

    The electronic structures of herbicides atrazine and bromoxynil have been investigated by UV photoelectron spectroscopy (UPS), quantum chemical calculations and comparison with X-ray diffraction, molecular docking and molecular dynamics studies. Their electronic and molecular structures are discussed in the context of their biological activity. This is the first report which correlates the molecular mechanism of biological activity of these herbicides with their experimentally determined electronic and molecular structures.

  5. Multilevel domain decomposition for electronic structure calculations

    SciTech Connect

    Barrault, M. . E-mail: maxime.barrault@edf.fr; Cances, E. . E-mail: cances@cermics.enpc.fr; Hager, W.W. . E-mail: hager@math.ufl.edu; Le Bris, C. . E-mail: lebris@cermics.enpc.fr

    2007-03-01

    We introduce a new multilevel domain decomposition method (MDD) for electronic structure calculations within semi-empirical and density functional theory (DFT) frameworks. This method iterates between local fine solvers and global coarse solvers, in the spirit of domain decomposition methods. Using this approach, calculations have been successfully performed on several linear polymer chains containing up to 40,000 atoms and 200,000 atomic orbitals. Both the computational cost and the memory requirement scale linearly with the number of atoms. Additional speed-up can easily be obtained by parallelization. We show that this domain decomposition method outperforms the density matrix minimization (DMM) method for poor initial guesses. Our method provides an efficient preconditioner for DMM and other linear scaling methods, variational in nature, such as the orbital minimization (OM) procedure.

  6. Studying localized corrosion using liquid cell transmission electron microscopy

    SciTech Connect

    Chee, See Wee; Pratt, Sarah H.; Hattar, Khalid; Duquette, David; Ross, Frances M.; Hull, Robert

    2014-11-07

    Using liquid cell transmission electron microscopy (LCTEM), localized corrosion of Cu and Al thin films immersed in aqueous NaCl solutions was studied. We demonstrate that potentiostatic control can be used to initiate pitting and that local compositional changes, due to focused ion beam implantation of Au+ ions, can modify the corrosion susceptibility of Al films. Likewise, a discussion on strategies to control the onset of pitting is also presented.

  7. Studying localized corrosion using liquid cell transmission electron microscopy

    DOE PAGESBeta

    Chee, See Wee; Pratt, Sarah H.; Hattar, Khalid; Duquette, David; Ross, Frances M.; Hull, Robert

    2014-11-07

    Using liquid cell transmission electron microscopy (LCTEM), localized corrosion of Cu and Al thin films immersed in aqueous NaCl solutions was studied. We demonstrate that potentiostatic control can be used to initiate pitting and that local compositional changes, due to focused ion beam implantation of Au+ ions, can modify the corrosion susceptibility of Al films. Likewise, a discussion on strategies to control the onset of pitting is also presented.

  8. Structural phase transition and electronic properties of NdBi

    SciTech Connect

    Sahu, Ashvini K.; Patiya, Jagdish; Sanyal, Sankar P.

    2015-06-24

    The structural and electronic properties of NdBi from an electronic structure calculation have been presented. The calculation is performed using self-consistent tight binding linear muffin tin orbital (TB-LMTO) method within the local density approximation (LDA). The calculated equilibrium structural parameters are in good agreement with the available experimental results. It is found that this compound shows metallic behavior under ambient condition and undergoes a structural phase transition from the NaCl structure to the CsCl structure at the pressure 20.1 GPa. The electronic structures of NdBi under pressure are investigated. It is found that NdBi have metallization and the hybridizations of atoms in NdBi under pressure become stronger.

  9. Excitation of local magnetic moments by tunneling electrons

    NASA Astrophysics Data System (ADS)

    Gauyacq, Jean-Pierre; Lorente, Nicolás; Novaes, Frederico Dutilh

    2012-05-01

    The advent of milli-kelvin scanning tunneling microscopes (STM) with inbuilt magnetic fields has opened access to the study of magnetic phenomena with atomic resolution at surfaces. In the case of single atoms adsorbed on a surface, the existence of different magnetic energy levels localized on the adsorbate is due to the breaking of the rotational invariance of the adsorbate spin by the interaction with its environment, leading to energy terms in the meV range. These structures were revealed by STM experiments in IBM Almaden in the early 2000s for atomic adsorbates on CuN surfaces. The experiments consisted in the study of the changes in conductance caused by inelastic tunneling of electrons (IETS, inelastic electron tunneling spectroscopy). Manganese and Iron adatoms were shown to have different magnetic anisotropies induced by the substrate. More experiments by other groups followed up, showing that magnetic excitations could be detected in a variety of systems: e.g. complex organic molecules showed that their magnetic anisotropy was dependent on the molecular environment, piles of magnetic molecules showed that they interact via intermolecular exchange interaction, spin waves were excited on ferromagnetic surfaces and in Mn chains, and magnetic impurities have been analyzed on semiconductors. These experiments brought up some intriguing questions: the efficiency of magnetic excitations was very high, the excitations could or could not involve spin flip of the exciting electron and singular-like behavior was sometimes found at the excitation thresholds. These facts called for extended theoretical analysis; perturbation theories, sudden-approximation approaches and a strong coupling scheme successfully explained most of the magnetic inelastic processes. In addition, many-body approaches were also used to decipher the interplay between inelastic processes and the Kondo effect. Spin torque transfer has been shown to be effective in changing spin orientations of an

  10. Electronic structure of carbon-boron nitride nanotubes

    NASA Astrophysics Data System (ADS)

    Sanginés-Mendoza, Raúl; Martinez, Edgar

    2013-03-01

    Structures of carbon and boron nitride nanotubes (CNTs, BNNTs) are quite similar, conversely, electronic properties are radically different from each other. Carbon nanotubes, whose electronic properties can be either metallic or semiconducting depending on their chiral structure, boron nitride nanotubes are always semiconductors with bandgaps over 4 eV. We have looked to hybrid systems, to predict a new kind of nanostructures with novel electronic properties. In this way, we explore the electronic properties of C-BN nanotubes. In particular, we studied the electronic structure of armchair C-BN nanotubes. The calculations were performed using the pseudopotential LCAO method with a Generalized Gradient Approximation for the exchange-correlation energy functional. The band structure of most of these systems have semiconductor character with an indirect gap smaller than its analogous BNNTs. In addition, the most prominent feature of these systems is the existence of flat bands both at the valence band top and at the conduction band minimum. Such flat bands results in sharp and narrow peaks on the total density of states. The behavior of these flat bands mainly indicates that electrons are largely localized. Thus, a detailed analysis on the electronic band structure shows that hybridization between those orbitals on the interfaces is responsible to exhibit localization effects on the hybrid systems.This research was supported by Conacyt under Grant No. 133022.

  11. Parallel adaptive mesh refinement for electronic structure calculations

    SciTech Connect

    Kohn, S.; Weare, J.; Ong, E.; Baden, S.

    1996-12-01

    We have applied structured adaptive mesh refinement techniques to the solution of the LDA equations for electronic structure calculations. Local spatial refinement concentrates memory resources and numerical effort where it is most needed, near the atomic centers and in regions of rapidly varying charge density. The structured grid representation enables us to employ efficient iterative solver techniques such as conjugate gradients with multigrid preconditioning. We have parallelized our solver using an object-oriented adaptive mesh refinement framework.

  12. Electronic structure of Fe-based amorphous alloys studied using electron-energy-loss spectroscopy

    NASA Astrophysics Data System (ADS)

    Wang, H. J.; Gu, X. J.; Poon, S. J.; Shiflet, G. J.

    2008-01-01

    The local atomic electronic structures of Fe-Mo-C-B metallic glasses are investigated using electron energy-loss spectroscopy (EELS). The fracture behavior of this Fe-based amorphous alloy system undergoes the transition from being ductile to exhibiting brittleness when alloyed with Cr or Er atoms. In addition, the glass-forming ability is also enhanced. This plastic-to-brittle transition is suggested to correlate with the change of local atomic short-range order or bonding configurations. Therefore, the bonding configuration of Fe-Mo-C-B-Er(Cr) amorphous alloys is investigated by studying the electronic structure of Fe and C atoms using electron energy-loss spectroscopy. It is shown that the normalized EELS white line intensities of Fe-L2,3 edges decrease slightly with an increasing amount of Er additions, while no noticeable difference is obtained with Cr additions. As for the C K edge, a prominent change of edge shape is observed for both alloy systems, where the first peak corresponding to a 1s→1π* transition increases with increasing Er and Cr additions. Accordingly, it is concluded that changes in the local atomic and electronic structure occur around Fe and C atoms when Er and Cr are introduced into the alloys. Furthermore, it is pointed out that the formation of Er-C and Cr-C carbide like local order inferred from the observed C K edge spectra can provide a plausible explanation for the plastic-to-brittle transition observed in these Fe-based amorphous alloys. In spite of the complexity of electronic and atomic structure in this multicomponent Fe-based metallic glass system, this study could serve as a starting point for providing a qualitative interpretation between electronic structure and plasticity in the Fe-Mo-C-B amorphous alloy system. Complimentary techniques, such as x-ray diffraction and high-resolution transmission electron microscope are also employed, providing a more complete structural characterization.

  13. Electronic correlation contributions to structural energies

    NASA Astrophysics Data System (ADS)

    Haydock, Roger

    2015-03-01

    The recursion method is used to calculate electronic excitation spectra including electron-electron interactions within the Hubbard model. The effects of correlation on structural energies are then obtained from these spectra and applied to stacking faults. http://arxiv.org/abs/1405.2288 Supported by the Richmond F. Snyder Fund and Gifts.

  14. Localized Electron Heating by Strong Guide-Field Magnetic Reconnection

    NASA Astrophysics Data System (ADS)

    Guo, Xuehan; Sugawara, Takumichi; Inomoto, Michiaki; Yamasaki, Kotaro; Ono, Yasushi; UTST Team

    2015-11-01

    Localized electron heating of magnetic reconnection was studied under strong guide-field (typically Bt 15Bp) using two merging spherical tokamak plasmas in Univ. Tokyo Spherical Tokamak (UTST) experiment. Our new slide-type two-dimensional Thomson scattering system documented for the first time the electron heating localized around the X-point. The region of high electron temperature, which is perpendicular to the magnetic field, was found to have a round shape with radius of 2 [cm]. Also, it was localized around the X-point and does not agree with that of energy dissipation term Et .jt . When we include a guide-field effect term Bt / (Bp + αBt) for Et .jt where α =√{ (vin2 +vout2) /v∥2 } , the energy dissipation area becomes localized around the X-point, suggesting that the electrons are accelerated by the reconnection electric field parallel to the magnetic field and thermalized around the X-point. This work was supported by JSPS A3 Foresight Program ``Innovative Tokamak Plasma Startup and Current Drive in Spherical Torus,'' a Grant-in-Aid from the Japan Society for the Promotion of Science (JSPS) Fellows 15J03758.

  15. Local Acceleration of Radiation Belt Electrons: Where? When? and How?

    NASA Astrophysics Data System (ADS)

    Reeves, G. D.; Henderson, M. G.; Morley, S.; Larsen, B.; Friedel, R. H.; Claudepierre, S. G.; Fennell, J. F.; Blake, J. B.; Boyd, A. J.; Spence, H.; Kanekal, S. G.; Baker, D. N.; Skoug, R. M.; Funsten, H. O.

    2013-12-01

    Two broad classes of processes are capable of accelerating radiation belt electrons to ultra-relativistic energies: radial acceleration by inward diffusion from a high-altitude source population and local acceleration of an in situ source population by wave-particle interactions. Recently the Van Allen Probes mission provided unambiguous observations of local acceleration for one of the first radiation belt enhancement events of the mission on October 8-9, 2012 [Reeves et al., 2013]. Now, with over a year of Van Allen Probes observations, it is possible to conduct a larger survey of radiation belt enhancement events. Level 4 phase space densities recently been made available by the RBSP-ECT science operations center using data from the Magnetic Electron Ion Spectrometer (MagEIS) [Blake et al., 2013] and Van Allen Probes magnetic ephemeris files [Henderson et al., 2013]. In this presentation we survey the radial profiles of phase space density as a function of the magnetic invariants (mu, K, and L*) for characteristic signatures of local acceleration through wave particle interactions. We examine how many radiation belt enhancement events show signatures of local acceleration and determine where the peak acceleration occurred. We compare the observations with the expectations from theories of local acceleration in order to better understand the generation mechanisms and the relative roles of local acceleration and radial diffusion in controlling radiation belt dynamics.

  16. Electron tomography of dislocation structures

    SciTech Connect

    Liu, G.S.; House, S.D.; Kacher, J.; Tanaka, M.; Higashida, K.; Robertson, I.M.

    2014-01-15

    Recent developments in the application of electron tomography for characterizing microstructures in crystalline solids are described. The underlying principles for electron tomography are presented in the context of typical challenges in adapting the technique to crystalline systems and in using diffraction contrast imaging conditions. Methods for overcoming the limitations associated with the angular range, the number of acquired images, and uniformity of image contrast are introduced. In addition, a method for incorporating the real space coordinate system into the tomogram is presented. As the approach emphasizes development of experimental solutions to the challenges, the solutions developed and implemented are presented in the form of examples.

  17. The electronic structure of grain boundaries in Nb

    SciTech Connect

    Sowa, E.C.; Gonis, A. ); Zhang, X.G. )

    1990-11-01

    We present first-principles calculations of the electronic structure of Nb grain boundaries. These are the first such calculations for a bcc metal using the real-space multiple-scattering theory (RSMST). Local densities of states near a {Sigma}5 twist grain boundary are compared to those for bulk Nb. 5 refs., 1 fig.

  18. Electron gun controlled smart structure

    DOEpatents

    Martin, Jeffrey W.; Main, John Alan; Redmond, James M.; Henson, Tammy D.; Watson, Robert D.

    2001-01-01

    Disclosed is a method and system for actively controlling the shape of a sheet of electroactive material; the system comprising: one or more electrodes attached to the frontside of the electroactive sheet; a charged particle generator, disposed so as to direct a beam of charged particles (e.g. electrons) onto the electrode; a conductive substrate attached to the backside of the sheet; and a power supply electrically connected to the conductive substrate; whereby the sheet changes its shape in response to an electric field created across the sheet by an accumulation of electric charge within the electrode(s), relative to a potential applied to the conductive substrate. Use of multiple electrodes distributed across on the frontside ensures a uniform distribution of the charge with a single point of e-beam incidence, thereby greatly simplifying the beam scanning algorithm and raster control electronics, and reducing the problems associated with "blooming". By placing a distribution of electrodes over the front surface of a piezoelectric film (or other electroactive material), this arrangement enables improved control over the distribution of surface electric charges (e.g. electrons) by creating uniform (and possibly different) charge distributions within each individual electrode. Removal or deposition of net electric charge can be affected by controlling the secondary electron yield through manipulation of the backside electric potential with the power supply. The system can be used for actively controlling the shape of space-based deployable optics, such as adaptive mirrors and inflatable antennae.

  19. Radially Localized Measurements of Superthermal Electrons Using Obilique Ece

    NASA Astrophysics Data System (ADS)

    Preische, Sherrie Anne

    1995-01-01

    In the effort to design a tokamak which will make a more compact and economically attractive fusion energy reactor, tokamak regimes are envisioned in which radial profiles of the density, temperature, and current are controlled. Lower Hybrid Current Drive is one of the most flexible and proven means of controlling the plasma current profile. In order to develop a better understanding of how, to what extent, and under what conditions LHCD can be used to tailor the current profile, the radial profile and velocity distribution of the fast current-carrying electrons and their time evolution must be known. Spacially localized information about the fast electron distribution function is difficult to obtain. The electron calcitrant resonance, through its sensitivity to the magnetic field as well as to the frequency and angle of observation, provides a means of probing the fast electron distribution function in detail. A new and unique diagnostic has been developed, installed, and operated on the PBX -M tokamak to measure the Electron Cyclotron Emission from these fast electrons. An oblique horizontal view of upshifted cyclotron emission in the midplane gives radial as well as velocity space information about the fast electrons by utilizing the sensitivity of the electron cyclotron resonance. Emission in extraordinary (X)-mode at frequencies refracted by the right-hand cutoff is radially localized. An experiment has been performed in which quasi-X mode emission in the range 60-90 GHz is observed through a focusing gaussian lens antenna at a 57^ circ angle to the toroidal magnetic field. Using the sensitivity of the resonance condition to small changes in frequency and field, radially localized moments. E_ parallel, T_ |, n_{sth}, of the fast electron distribution function are found by a Bayesian analysis method. The evolution of the current profile obtained from these measurements is examined in detail. After the LHCD is turned off, the dynamics are found to be

  20. Structural change of graphite during electron irradiation

    SciTech Connect

    Koike, J. . Dept. of Mechanical Engineering); Pedraza, D.F. )

    1992-01-01

    Highly oriented pyrolytic graphite was irradiated at room temperature with 300-keV electrons. High resolution transmission electron microscopy and electron energy loss spectroscopy were employed to study the structure of electron-irradiated graphite. Results consistently indicated absence of long-range order periodicity in the basal plane, and loose retention of the c-axis periodicity. Structure was modeled based on a mixture of sixfold and non-sixfold atom rings. Formation of non-sixfold atom rings was related to the observed buckling and discontinuity of the original graphite basal plane.

  1. Structural change of graphite during electron irradiation

    SciTech Connect

    Koike, J.; Pedraza, D.F.

    1992-12-31

    Highly oriented pyrolytic graphite was irradiated at room temperature with 300-keV electrons. High resolution transmission electron microscopy and electron energy loss spectroscopy were employed to study the structure of electron-irradiated graphite. Results consistently indicated absence of long-range order periodicity in the basal plane, and loose retention of the c-axis periodicity. Structure was modeled based on a mixture of sixfold and non-sixfold atom rings. Formation of non-sixfold atom rings was related to the observed buckling and discontinuity of the original graphite basal plane.

  2. Localized electronic states at grain boundaries on the surface of graphene and graphite

    NASA Astrophysics Data System (ADS)

    Luican-Mayer, Adina; Barrios-Vargas, Jose E.; Toft Falkenberg, Jesper; Autès, Gabriel; Cummings, Aron W.; Soriano, David; Li, Guohong; Brandbyge, Mads; Yazyev, Oleg V.; Roche, Stephan; Andrei, Eva Y.

    2016-09-01

    Recent advances in large-scale synthesis of graphene and other 2D materials have underscored the importance of local defects such as dislocations and grain boundaries (GBs), and especially their tendency to alter the electronic properties of the material. Understanding how the polycrystalline morphology affects the electronic properties is crucial for the development of applications such as flexible electronics, energy harvesting devices or sensors. We here report on atomic scale characterization of several GBs and on the structural-dependence of the localized electronic states in their vicinity. Using low temperature scanning tunneling microscopy and spectroscopy, together with tight binding and ab initio numerical simulations we explore GBs on the surface of graphite and elucidate the interconnection between the local density of states and their atomic structure. We show that the electronic fingerprints of these GBs consist of pronounced resonances which, depending on the relative orientation of the adjacent crystallites, appear either on the electron side of the spectrum or as an electron-hole symmetric doublet close to the charge neutrality point. These two types of spectral features will impact very differently the transport properties allowing, in the asymmetric case to introduce transport anisotropy which could be utilized to design novel growth and fabrication strategies to control device performance.

  3. About zitterbewegung and electron structure

    NASA Astrophysics Data System (ADS)

    Rodrigues, Waldyr A.; Vaz, Jayme; Recami, Erasmo; Salesi, Giovanni

    1993-12-01

    We start from the spinning electron model by Barut and Zanghi, which has been recently translated into the Clifford algebra language. We ``complete'' such a translation, first of all, by expressing in the Clifford formalism a particular Barut-Zanghi (BZ) solution, which refers (at the classical limit) to an ``internal'' helical motion with a time-like speed (and is here shown to originate from the superposition of positive and negative frequency solutions of the Dirac equation). Then, we show how to construct solutions of the Dirac equation describing helical motions with light-like speed, which meet very well the standard interpretation of the velocity operator in the Dirac equation theory (and agree with the solution proposed by Hestenes, on the basis - however - of ad-hoc assumptions that are unnecessary in the present approach). The above results appear to support the conjecture that the zitterbewegung motion (a helical motion, at the classical limit) is responsible for the electron spin.

  4. Electronic structure of metallic glasses

    SciTech Connect

    Oelhafen, P.; Lapka, R.; Gubler, U.; Krieg, J.; DasGupta, A.; Guentherodt, H.J.; Mizoguchi, T.; Hague, C.; Kuebler, J.; Nagel, S.R.

    1981-01-01

    This paper is organized in six sections and deals with (1) the glassy transition metal alloys, their d-band structure, the d-band shifts on alloying and their relation to the alloy heat of formation (..delta..H) and the glass forming ability, (2) the glass to crystal phase transition viewed by valence band spectroscopy, (3) band structure calculations, (4) metallic glasses prepared by laser glazing, (5) glassy normal metal alloys, and (6) glassy hydrides.

  5. Structural physiology based on electron crystallography

    PubMed Central

    Fujiyoshi, Yoshinori

    2011-01-01

    There are many questions in brain science, which are extremely interesting but very difficult to answer. For example, how do education and other experiences during human development influence the ability and personality of the adult? The molecular mechanisms underlying such phenomena are still totally unclear. However, technological and instrumental advancements of electron microscopy have facilitated comprehension of the structures of biological components, cells, and organelles. Electron crystallography is especially good for studying the structure and function of membrane proteins, which are key molecules of signal transduction in neural and other cells. Electron crystallography is now an established technique to analyze the structures of membrane proteins in lipid bilayers, which are close to their natural biological environment. By utilizing cryo-electron microscopes with helium cooled specimen stages, which were developed through a personal motivation to understand functions of neural systems from a structural point of view, structures of membrane proteins were analyzed at a resolution higher than 3 Å. This review has four objectives. First, it is intended to introduce the new research field of structural physiology. Second, it introduces some of the personal struggles, which were involved in developing the cryo-electron microscope. Third, it discusses some of the technology for the structural analysis of membrane proteins based on cryo-electron microscopy. Finally, it reviews structural and functional analyses of membrane proteins. PMID:21416541

  6. Electron-phonon renormalization of the electronic structure of diamond

    NASA Astrophysics Data System (ADS)

    Giustino, Feliciano; Louie, Steven G.; Cohen, Marvin L.

    2011-03-01

    The calculation of band structures from first-principles has reached a high level of accuracy. Calculations combining density-functional theory with many-body perturbation theory often are in good agreement with measurements by photoemission, tunneling, and other spectroscopic probes. While significant efforts have been devoted to improving the description of electron-electron interactions in these calculations, the effect of lattice vibrations has largely been overlooked so far. In this work we study from first principles the electron-phonon renormalization of the band gap of diamond. The calculated temperature dependence of the gap and the broadening of the absorption edge are in excellent agreement with spectroscopic ellipsometry data. Interestingly we find a gap renormalization due to zero-point vibrations as large as 0.6 eV. We discuss the implications of our findings for the electronic structure of other carbon-based bulk materials and nanostructures.

  7. Impact of cation-based localized electronic states on the conduction and valence band structure of Al{sub 1−x}In{sub x}N alloys

    SciTech Connect

    Schulz, S.; Caro, M. A.; O'Reilly, E. P.

    2014-04-28

    We demonstrate that cation-related localized states strongly perturb the band structure of Al{sub 1−x}In{sub x}N leading to a strong band gap bowing at low In content. Our first-principles calculations show that In-related localized states are formed both in the conduction and the valence band in Al{sub 1−x}In{sub x}N for low In composition, x, and that these localized states dominate the evolution of the band structure with increasing x. Therefore, the commonly used assumption of a single composition-independent bowing parameter breaks down when describing the evolution both of the conduction and of the valence band edge in Al{sub 1−x}In{sub x}N.

  8. Effect of Structural Relaxation on the Electronic Structure of Graphene on Hexagonal Boron Nitride.

    PubMed

    Slotman, G J; van Wijk, M M; Zhao, Pei-Liang; Fasolino, A; Katsnelson, M I; Yuan, Shengjun

    2015-10-30

    We performed calculations of electronic, optical, and transport properties of graphene on hexagonal boron nitride with realistic moiré patterns. The latter are produced by structural relaxation using a fully atomistic model. This relaxation turns out to be crucially important for electronic properties. We describe experimentally observed features such as additional Dirac points and the "Hofstadter butterfly" structure of energy levels in a magnetic field. We find that the electronic structure is sensitive to many-body renormalization of the local energy gap. PMID:26565485

  9. Effect of Structural Relaxation on the Electronic Structure of Graphene on Hexagonal Boron Nitride

    NASA Astrophysics Data System (ADS)

    Slotman, G. J.; van Wijk, M. M.; Zhao, Pei-Liang; Fasolino, A.; Katsnelson, M. I.; Yuan, Shengjun

    2015-10-01

    We performed calculations of electronic, optical, and transport properties of graphene on hexagonal boron nitride with realistic moiré patterns. The latter are produced by structural relaxation using a fully atomistic model. This relaxation turns out to be crucially important for electronic properties. We describe experimentally observed features such as additional Dirac points and the "Hofstadter butterfly" structure of energy levels in a magnetic field. We find that the electronic structure is sensitive to many-body renormalization of the local energy gap.

  10. Wavelets in self-consistent electronic structure calculations

    SciTech Connect

    Wei, S.; Chou, M.Y.

    1996-04-01

    We report the first implementation of orthonormal wavelet bases in self-consistent electronic structure calculations within the local-density approximation. These local bases of different scales efficiently describe localized orbitals of interest. As an example, we studied two molecules, H{sub 2} and O{sub 2}, using pseudopotentials and supercells. Considerably fewer bases are needed compared with conventional plane-wave approaches, yet calculated binding properties are similar. Our implementation employs fast wavelet and Fourier transforms, avoiding evaluating any three-dimensional integral numerically. {copyright} {ital 1996 The American Physical Society.}

  11. Variations of the Local Electronic Surface Properties of TiO2(110) Induced By Intrinsic and Extrinsic Defects

    SciTech Connect

    Batzill, Matthias; Katsiev, Bulat; Gaspar, Dan J. ); Diebold, Ulrike

    2002-12-15

    Variation of the local electronic structure at rutile TiO2(110) surfaces was studied by scanning tunneling spectroscopy (STS). Structural surface features like step edges, (1 x 2) reconstructed strands, and their terminations were correlated to changes in tunneling spectra. In particular, band gap states, associated with a reduced surface, showed characteristic variations. In addition, electronic variations due extrinsic defects are discussed. Nanometer wide protrusions in constant current scanning tunneling microscopy images were identified in STS as local electronic alterations. These features are interpreted to be due to local band bending induced by individual, charged impurity atoms.

  12. Instructional Approach to Molecular Electronic Structure Theory

    ERIC Educational Resources Information Center

    Dykstra, Clifford E.; Schaefer, Henry F.

    1977-01-01

    Describes a graduate quantum mechanics projects in which students write a computer program that performs ab initio calculations on the electronic structure of a simple molecule. Theoretical potential energy curves are produced. (MLH)

  13. Computational Chemistry Using Modern Electronic Structure Methods

    ERIC Educational Resources Information Center

    Bell, Stephen; Dines, Trevor J.; Chowdhry, Babur Z.; Withnall, Robert

    2007-01-01

    Various modern electronic structure methods are now days used to teach computational chemistry to undergraduate students. Such quantum calculations can now be easily used even for large size molecules.

  14. Local Quark-Hadron Duality in Electron Scattering

    SciTech Connect

    Wally Melnitchouk

    2007-09-10

    We present some recent developments in the study of quark-hadron duality in structure functions in the resonance region. To understand the workings of local duality we introduce the concept of truncated moments, which are used to describe the Q^2 dependence of specific resonance regions within a QCD framework.

  15. Electronic structure and photophysical properties of polyimides

    SciTech Connect

    LaFemina, J.P.; Kafafi, S.A.

    1992-04-01

    The quantum mechanical AM1 and CNDO/S3 models were used to examine the effect of isoelectronic substitutions on the conformation, electronic structure, and optical absorption spectra for a series of aromatic polyimides. An analysis of the geometric changes at the substitution site and its effect on the electronic structure allowed for the prediction of changes in the ICT band of the optical absorption spectra.

  16. A Mapping of the Electron Localization Function for Earth Materials

    SciTech Connect

    Gibbs, Gerald V.; Cox, David F.; Ross, Nancy; Crawford, T Daniel; Burt, Jason; Rosso, Kevin M.

    2005-06-01

    The electron localization function, ELF, generated for a number of geometry-optimized earth materials, provides a graphical representation of the spatial localization of the probability electron density distribution as embodied in domains ascribed to localized bond and lone pair electrons. The lone pair domains, displayed by the silica polymorphs quartz, coesite and cristobalite, are typically banana-shaped and oriented perpendicular to the plane of the SiOSi angle at ~0.60 Å from the O atom on the reflex side of the angle. With decreasing angle, the domains increase in magnitude, indicating an increase in the nucleophilic character of the O atom, rendering it more susceptible to potential electrophilic attack. The Laplacian isosurface maps of the experimental and theoretical electron density distribution for coesite substantiates the increase in the size of the domain with decreasing angle. Bond pair domains are displayed along each of the SiO bond vectors as discrete concave hemispherically-shaped domains at ~0.70 Å from the O atom. For more closed-shell ionic bonded interactions, the bond and lone pair domains are often coalesced, resulting in concave hemispherical toroidal-shaped domains with local maxima centered along the bond vectors. As the shared covalent character of the bonded interactions increases, the bond and lone pair domains are better developed as discrete domains. ELF isosurface maps generated for the earth materials tremolite, diopside, talc and dickite display banana-shaped lone pair domains associated with the bridging O atoms of SiOSi angles and concave hemispherical toroidal bond pair domains associated with the nonbridging ones. The lone pair domains in dickite and talc provide a basis for understanding the bonded interactions between the adjacent neutral layers. Maps were also generated for beryl, cordierite, quartz, low albite, forsterite, wadeite, åkermanite, pectolite, periclase, hurlbutite, thortveitite and vanthoffite. Strategies

  17. MCSNA: Experimental Benchmarking of Pu Electronic Structure

    SciTech Connect

    Tobin, J G

    2007-01-29

    The objective of this work is to develop and/or apply advanced diagnostics to the understanding of aging of Pu. Advanced characterization techniques such as photoelectron and x-ray absorption spectroscopy will provide fundamental data on the electronic structure of Pu phases. These data are crucial for the validation of the electronic structure methods. The fundamental goal of this project is to narrow the parameter space for the theoretical modeling of Pu aging. The short-term goal is to perform experiments to validate electronic structure calculations of Pu. The long-term goal is to determine the effects of aging upon the electronic structure of Pu. Many of the input parameters for aging models are not directly measurable. These parameters will need to be calculated or estimated. Thus a First Principles-Approach Theory is needed, but it is unclear what terms are important in the Hamiltonian. (H{Psi} = E{Psi}) Therefore, experimental data concerning the 5f electronic structure are needed, to determine which terms in the Hamiltonian are important. The data obtained in this task are crucial for reducing the uncertainty of Task LL-01-developed models and predictions. The data impact the validation of electronic structure methods, the calculation of defect properties, the evaluation of helium diffusion, and the validation of void nucleation models. The importance of these activities increases if difficulties develop with the accelerating aging alloy approach.

  18. Localization of the valence electron of endohedrally confined hydrogen, lithium and sodium in fullerene cages

    NASA Astrophysics Data System (ADS)

    Cuestas, Eloisa; Serra, Pablo

    2016-03-01

    The localization of the valence electron of H, Li and Na atoms enclosed by three different fullerene molecules is studied. The structure of the fullerene molecules is used to calculate the equilibrium position of the endohedrally atom as the minimum of the classical (N + 1)-body Lennard-Jones potential. Once the position of the guest atom is determined, the fullerene cavity is modeled by a short range attractive shell according to molecule symmetry, and the enclosed atom is modeled by an effective one-electron potential. In order to examine whether the endohedral compound is formed by a neutral atom inside a neutral fullerene molecule X@CN or if the valence electron of the encapsulated atom localizes in the fullerene giving rise to a state with the form X+@CN‑, we analyze the electronic density, the projections onto free atomic states and the weights of partial angular waves.

  19. Foil support structure for large electron guns

    SciTech Connect

    Brucker, J.P.; Rose, E.A.

    1993-08-01

    This paper describes a novel support structure for a vacuum diode used to pump a gaseous laser with an electron beam. Conventional support structures are designed to hold a foil flat and rigid. This new structure takes advantage of the significantly greater strength of metals in pure tension, utilizing curved shapes for both foil and support structure. The shape of the foil is comparable to the skin of a balloon, and the shape of the support structures is comparable to the cables of a suspension bridge. This design allows a significant reduction in foil thickness and support structure mass, resulting in a lower electron-beam loss between diode and laser gas. In addition, the foil is pre-formed in the support structure at pressures higher than operating pressure. Therefore, the foil is operated far from the yield point. Increased reliability is anticipated.

  20. Electronic structure calculations in arbitrary electrostatic environments

    NASA Astrophysics Data System (ADS)

    Watson, Mark A.; Rappoport, Dmitrij; Lee, Elizabeth M. Y.; Olivares-Amaya, Roberto; Aspuru-Guzik, Alán

    2012-01-01

    Modeling of electronic structure of molecules in electrostatic environments is of considerable relevance for surface-enhanced spectroscopy and molecular electronics. We have developed and implemented a novel approach to the molecular electronic structure in arbitrary electrostatic environments that is compatible with standard quantum chemical methods and can be applied to medium-sized and large molecules. The scheme denoted CheESE (chemistry in electrostatic environments) is based on the description of molecular electronic structure subject to a boundary condition on the system/environment interface. Thus, it is particularly suited to study molecules on metallic surfaces. The proposed model is capable of describing both electrostatic effects near nanostructured metallic surfaces and image-charge effects. We present an implementation of the CheESE model as a library module and show example applications to neutral and negatively charged molecules.

  1. Structure and local structure of perovskite based materials

    NASA Astrophysics Data System (ADS)

    Rossell Abrodos, Marta Dacil

    Perovskites, with general formula ABX3, where A and B are cations and X is an anion, form a very important class of inorganic crystals whose physical properties are extensively used in many technological applications. The basic, so-called aristotype structure, consists of an infinite array of corner-linked anion octahedra, with the A cations in the spaces between the octahedra and a B cation at the center of each octahedron. Interesting physical properties are often related to the flexibility of the perovskite structure to deform or to form non-stoichiometric compositions. In this thesis, four perovskite-related systems are studied. Transmission electron microscopy (TEM) is of prime interest to analyze the influence of the structure and microstructure on the physical properties of these systems. (1) The anion-deficient Sr4Fe6O12+delta (delta < 1) derivatives. These materials are mixed conducting oxides with high oxygen and electronic conductivity. A complete characterization of the structure of these anion-deficient compounds is deduced from electron diffraction and high-resolution TEM. The presence of anion vacancies in the Sr4Fe6O12+delta (delta < 1) structure is suggested to have an influence on the transport properties. (2) The CaRMnSnO6 (R = La, Pr, Nd, Sm-Dy) double perovskites. A random distribution of the Ca and R cations over the A positions and Mn and Sn cations over the B positions is found. Due to a random distribution of the Mn 3+ and Sn4+ cations, a spin glass behavior was found for CaLaMnSnO6. (3) The K3AlF6 elpasolite-type (or ordered double perovskite) structure. This compound is of high technological importance since it is a basic component of the melts for low temperature electrolysis in aluminum smelting. A sequence of phase transitions at different temperatures in K3AlF6 along with the data on unit cell dimensions and space symmetry of three major polymorphs is reported. (4) Ca 2Fe2O5 brownmillerite-type thin films deposited on three different

  2. Software abstractions and computational issues in parallel structure adaptive mesh methods for electronic structure calculations

    SciTech Connect

    Kohn, S.; Weare, J.; Ong, E.; Baden, S.

    1997-05-01

    We have applied structured adaptive mesh refinement techniques to the solution of the LDA equations for electronic structure calculations. Local spatial refinement concentrates memory resources and numerical effort where it is most needed, near the atomic centers and in regions of rapidly varying charge density. The structured grid representation enables us to employ efficient iterative solver techniques such as conjugate gradient with FAC multigrid preconditioning. We have parallelized our solver using an object- oriented adaptive mesh refinement framework.

  3. Electron Spin Resonance Imaging Utilizing Localized Microwave Magnetic Field

    NASA Astrophysics Data System (ADS)

    Furusawa, Masahiro; Ikeya, Motoji

    1990-02-01

    A method for two-dimensional electron spin resonance (ESR) imaging utilizing a localized microwave field is presented with an application of the image processing technique. Microwaves are localized at the surface of a sample by placing a sample in contact with a pinholed cavity wall. A two-dimensional ESR image can be obtained by scanning the sample in contact with the cavity. Some ESR images which correspond to distribution of natural radiation damages and paramagnetic impurities in carbonate fossils of a crinoid and an ammonite are presented as applications in earth science. Resolution of a raw ESR image is restricted by the diameter of the hole (1 mm). Higher resolution of 0.2 mm is obtained by using a deconvolution algorithm and instrument function for the hole. Restored images of a test sample of DPPH and of a fossil crinoid are presented.

  4. Local charge measurement using off-axis electron holography

    NASA Astrophysics Data System (ADS)

    Beleggia, M.; Gontard, L. C.; Dunin-Borkowski, R. E.

    2016-07-01

    A model-independent approach based on Gauss’ theorem for measuring the local charge in a specimen from an electron-optical phase image recorded using off-axis electron holography was recently proposed. Here, we show that such a charge measurement is reliable when it is applied to determine the total charge enclosed within an object. However, the situation is more complicated for a partial charge measurement when the integration domain encloses only part of the object. We analyze in detail the effects on charge measurement of the mean inner potential of the object, of the presence of induced charges on nearby supports/electrodes and of noise. We perform calculations for spherical particles and highlight the differences when dealing with other object shapes. Our analysis is tested using numerical simulations and applied to the interpretation of an experimental dataset recorded from a sapphire particle.

  5. Inelastic electron tunneling spectroscopy of local "spin accumulation" devices

    NASA Astrophysics Data System (ADS)

    Tinkey, Holly N.; Li, Pengke; Appelbaum, Ian

    2014-06-01

    We investigate the origin of purported "spin accumulation" signals observed in local "three-terminal" (3T) measurements of ferromagnet/insulator/n-Si tunnel junctions using inelastic electron tunneling spectroscopy (IETS). Voltage bias and magnetic field dependences of the IET spectra were found to account for the dominant contribution to 3T magnetoresistance, thus indicating that it arises from inelastic tunneling through impurities and defects at junction interfaces and within the barrier, rather than from spin accumulation due to pure elastic tunneling into bulk Si as has been previously assumed.

  6. Dynamical localization of electrons in an aperiodic superlattice

    SciTech Connect

    Luban, M.; Luscombe, J.H.

    1998-04-01

    We derive the analytical form of the time-dependent wave function for a single-band tight-binding model of independent conduction electrons within an aperiodic semiconductor superlattice, created by modifications in the composition of a single layer of an otherwise periodic superlattice. While the wave function for long times is known to feature both diffusive and localized behavior, the latter originating in the superlattice aperiodicity, we provide quantitative results for these features for all values of the time. {copyright} {ital 1998} {ital The American Physical Society}

  7. Local Strain Evaluation of Strained-SOI Structures

    NASA Astrophysics Data System (ADS)

    Usuda, Koji; Mizuno, Tomohisa; Numata, Toshinori; Tezuka, Tsutomu; Sugiyama, Naoharu; Moriyama, Yoshihiko; Nakaharai, Shu; Takagi, Shin-Ichi

    The strain relaxation within a strained-Si on SiGe on insulator (SGOI) structure might be one of the key issues in development of strained-Si MOSFET devices for high-performance ULSIs. In order to investigate the strain relaxation within the thin strained-Si layers, a new characterization technique to directly evaluate a local strain variation in the layers is required. Hence, we have developed the nano-beam electron diffraction (NBD) method which has a lateral resolution of 10 nm and a strain resolution of 0.1%. In this paper, we discuss a detailed investigation of whether the NBD method could be utilized to clarify a strain in a strained-Si layer on the SGOI structures.

  8. Local structures of copper-doped ZnO films

    NASA Astrophysics Data System (ADS)

    Ma, Qing; Buchholz, D. Bruce; Chang, Robert P. H.

    2008-12-01

    We report the local structures of a series of copper-doped zinc oxide films using polarization-dependent x-ray-absorption spectroscopy. The films were grown by pulsed-laser ablation under various conditions. The results show that films where copper exists solely as clusters are not ferromagnetic. The results also show that some of the copper-doped zinc oxide films are not ferromagnetic despite the fact that the copper substitution for zinc in the ZnO lattice is in the Cu2+ state, which provides the necessary unpaired spins for ferromagnetism. Therefore, Cu2+/Zn2+ substitution is not the only imperative condition for ferromagnetism to occur. We present characteristics unique to the electronic and atomic structure of ferromagnetic films and argue that the increased covalence of the CuZn-O bond found in these films is a prerequisite for the spin alignments in a substitutionally copper-doped zinc oxide film.

  9. Electronic Structure and Phase Stability of PdPt Nanoparticles.

    PubMed

    Ishimoto, Takayoshi; Koyama, Michihisa

    2016-03-01

    To understand the origin of the physicochemical nature of bimetallic PdPt nanoparticles, we theoretically investigated the phase stability and electronic structure employing the PdPt nanoparticles models consisting of 711 atoms (ca. 3 nm). For the Pd-Pt core-shell nanoparticle, the PdPt solid-solution phase was found to be a thermodynamically stable phase in the nanoparticle as the result of difference in surface energy of Pd and Pt nanoparticles and configurational entropy effect, while it is well known that the Pd and Pt are the immiscible combination in the bulk phase. The electronic structure of nanoparticles is conducted to find that the electron transfer occurs locally within surface and subsurface layers. In addition, the electron transfer from Pd to Pt at the interfacial layers in core-shell nanoparticles is observed, which leads to unique geometrical and electronic structure changes. Our results show a clue for the tunability of the electronic structure of nanoparticles by controlling the arrangement in the nanoparticles. PMID:26862885

  10. On-site screened Coulomb interactions for localized electrons in transition metal oxides and defect systems

    NASA Astrophysics Data System (ADS)

    Shih, Bi-Ching; Zhang, Peihong; Department of Physics Team

    2011-03-01

    Electronic and structural properties of strongly correlated material systems are largely determined by the strength of the on-site Coulomb interaction. Theoretical models devised to capture the physics of strongly correlated materials usually involve screened Coulomb interactions as adjustable parameters. We present first-principles results for the screened on-site Coulomb and exchange energy for transition metal oxides. The dielectric screening is calculated within the random phase approximation and the localized electrons are represented by maximally localized Wannier functions. We further extend our study to calculate on-site Coulomb interactions for localized defect states in semiconductors. We acknowledge the computational support provided by the Center for Computational Research at the University at Buffalo, SUNY. This work is supported by the National Science Foundation under Grant No. DMR-0946404 and by the Department of Energy under Grant No. DE-SC0002623.

  11. Structure and Dynamics with Ultrafast Electron Microscopes

    NASA Astrophysics Data System (ADS)

    Siwick, Bradley

    In this talk I will describe how combining ultrafast lasers and electron microscopes in novel ways makes it possible to directly `watch' the time-evolving structure of condensed matter, both at the level of atomic-scale structural rearrangements in the unit cell and at the level of a material's nano- microstructure. First, I will briefly describe my group's efforts to develop ultrafast electron diffraction using radio- frequency compressed electron pulses in the 100keV range, a system that rivals the capabilities of xray free electron lasers for diffraction experiments. I will give several examples of the new kinds of information that can be gleaned from such experiments. In vanadium dioxide we have mapped the detailed reorganization of the unit cell during the much debated insulator-metal transition. In particular, we have been able to identify and separate lattice structural changes from valence charge density redistribution in the material on the ultrafast timescale. In doing so we uncovered a previously unreported optically accessible phase/state of vanadium dioxide that has monoclinic crystallography like the insulator, but electronic structure and properties that are more like the rutile metal. We have also combined these dynamic structural measurements with broadband ultrafast spectroscopy to make detailed connections between structure and properties for the photoinduced insulator to metal transition. Second, I will show how dynamic transmission electron microscopy (DTEM) can be used to make direct, real space images of nano-microstructural evolution during laser-induced crystallization of amorphous semiconductors at unprecedented spatio-temporal resolution. This is a remarkably complex process that involves several distinct modes of crystal growth and the development of intricate microstructural patterns on the nanosecond to ten microsecond timescales all of which can be imaged directly with DTEM.

  12. Creating and Probing Graphene Electron Optics with Local Scanning Probes

    NASA Astrophysics Data System (ADS)

    Stroscio, Joseph

    Ballistic propagation and the light-like dispersion of graphene charge carriers make graphene an attractive platform for optics-inspired graphene electronics where gate tunable potentials can control electron refraction and transmission. In analogy to optical wave propagation in lenses, mirrors and metamaterials, gate potentials can be used to create a negative index of refraction for Veselago lensing and Fabry-Pérot interferometers. In circular geometries, gate potentials can induce whispering gallery modes (WGM), similar to optical and acoustic whispering galleries albeit on a much smaller length scale. Klein scattering of Dirac carriers plays a central role in determining the coherent propagation of electron waves in these resonators. In this talk, I examine the probing of electron resonators in graphene confined by linear and circular gate potentials with the scanning tunneling microscope (STM). The tip in the STM tunnel junction serves both as a tunable local gate potential, and as a probe of the graphene states through tunneling spectroscopy. A combination of a back gate potential, Vg, and tip potential, Vb, creates and controls a circular pn junction that confines the WGM graphene states. The resonances are observed in two separate channels in the tunneling spectroscopy experiment: first, by directly tunneling into the state at the bias energy eVb, and, second, by tunneling from the resonance at the Fermi level as the state is gated by the tip potential. The second channel produces a fan-like set of WGM peaks, reminiscent of the fringes seen in planar geometries by transport measurements. The WGM resonances split in a small applied magnetic field, with a large energy splitting approaching the WGM spacing at 0.5 T. These results agree well with recent theory on Klein scattering in graphene electron resonators. This work is done in collaboration with Y. Zhao, J. Wyrick, F.D. Natterer, J. F. Rodriquez-Nieva, C. Lewandoswski, K. Watanabe, T. Taniguchi, N. B

  13. Defect Induced Electronic Structure of Uranofullerene

    PubMed Central

    Dai, Xing; Cheng, Cheng; Zhang, Wei; Xin, Minsi; Huai, Ping; Zhang, Ruiqin; Wang, Zhigang

    2013-01-01

    The interaction between the inner atoms/cluster and the outer fullerene cage is the source of various novel properties of endohedral metallofullerenes. Herein, we introduce an adatom-type spin polarization defect on the surface of a typical endohedral stable U2@C60 to predict the associated structure and electronic properties of U2@C61 based on the density functional theory method. We found that defect induces obvious changes in the electronic structure of this metallofullerene. More interestingly, the ground state of U2@C61 is nonet spin in contrast to the septet of U2@C60. Electronic structure analysis shows that the inner U atoms and the C ad-atom on the surface of the cage contribute together to this spin state, which is brought about by a ferromagnetic coupling between the spin of the unpaired electrons of the U atoms and the C ad-atom. This discovery may provide a possible approach to adapt the electronic structure properties of endohedral metallofullerenes. PMID:23439318

  14. Membrane protein structure determination by electron crystallography

    PubMed Central

    Ubarretxena-Belandia, Iban; Stokes, David L.

    2012-01-01

    During the past year, electron crystallography of membrane proteins has provided structural insights into the mechanism of several different transporters and into their interactions with lipid molecules within the bilayer. From a technical perspective there have been important advances in high-throughput screening of crystallization trials and in automated imaging of membrane crystals with the electron microscope. There have also been key developments in software, and in molecular replacement and phase extension methods designed to facilitate the process of structure determination. PMID:22572457

  15. The Electronic Structure of Heavy Element Complexes

    SciTech Connect

    Bursten, Bruce E.

    2000-07-25

    The area of study is the bonding in heavy element complexes, and the application of more sophisticated electronic structure theories. Progress is recounted in several areas: (a) technological advances and current methodologies - Relativistic effects are extremely important in gaining an understanding of the electronic structure of compounds of the actinides, transactinides, and other heavy elements. Therefore, a major part of the continual benchmarking was the proper inclusion of the appropriate relativistic effects for the properties under study. (b) specific applications - These include organoactinide sandwich complexes, CO activation by actinide atoms, and theoretical studies of molecules of the transactinide elements. Finally, specific directions in proposed research are described.

  16. Characterizing the Locality of Diabatic States for Electronic Excitation Transfer by Decomposing the Diabatic Coupling

    SciTech Connect

    Vura-Weis, Josh; Newton, M. D.; Wasielewski, Michael R; Subotnik, J.E.

    2010-12-09

    A common strategy to calculate electronic coupling matrix elements for charge or energy transfer is to take the adiabatic states generated by electronic structure computations and rotate them to form localized diabatic states. In this paper, we show that, for intermolecular transfer of singlet electronic excitation, usually we cannot fully localize the electronic excitations in this way. Instead, we calculate putative initial and final states with small excitation tails caused by weak interactions with high energy excited states in the electronic manifold. These tails do not lead to substantial changes in the total diabatic coupling between states, but they do lead to a different partitioning of the total coupling between Coulomb (Förster), exchange (Dexter), and one-electron components. The tails may be reduced by using a multistate diabatic model or eliminated entirely by truncation (denoted as “chopping”). Without more information, we are unable to conclude with certainty whether the observed diabatic tails are a physical reality or a computational artifact. This research suggests that decomposition of the diabatic coupling between chromophores into Coulomb, exchange, and one-electron components may depend strongly on the number of states considered, and such results should be treated with caution.

  17. Compositional dependence of the local structure of Se{sub x}Te{sub 1-x} alloys: Electron energy-loss spectra, real-space multiple-scattering calculations, and first-principles molecular dynamics

    SciTech Connect

    Katcho, N. A.; Lomba, E.; Urones-Garrote, E.; Otero-Diaz, L. C.; Landa-Canovas, A. R.

    2006-06-01

    In this work we present an investigation on the composition dependence of the local structure in Se{sub x}Te{sub 1-x} crystalline alloys analyzing their experimental energy-loss spectra with the aid of a real-space multiple-scattering modeling approach and first-principles molecular dynamics. The concourse of this latter technique is essential for a proper modeling of the alloy spectra. From our results, it can be inferred that Se{sub x}Te{sub 1-x} alloys exhibit a high degree of substitutional disorder ruling out the existence of fully ordered alternating copolymer chains of Se and Te atoms.

  18. Compositional dependence of the local structure of SexTe1-x alloys: Electron energy-loss spectra, real-space multiple-scattering calculations, and first-principles molecular dynamics

    NASA Astrophysics Data System (ADS)

    Katcho, N. A.; Lomba, E.; Urones-Garrote, E.; Landa-Cánovas, A. R.; Otero-Díaz, L. C.

    2006-06-01

    In this work we present an investigation on the composition dependence of the local structure in SexTe1-x crystalline alloys analyzing their experimental energy-loss spectra with the aid of a real-space multiple-scattering modeling approach and first-principles molecular dynamics. The concourse of this latter technique is essential for a proper modeling of the alloy spectra. From our results, it can be inferred that SexTe1-x alloys exhibit a high degree of substitutional disorder ruling out the existence of fully ordered alternating copolymer chains of Se and Te atoms.

  19. Electronic and magnetic structures of CeTe2

    NASA Astrophysics Data System (ADS)

    Shim, J. H.; Youn, S. J.; Park, Min Sik; Min, B. I.

    2005-05-01

    We have investigated electronic structures of CeTe2 to explore the correlation between the magnetic, charge density wave, and superconducting phases by using the local spin density approximation (LSDA) and LSDA +U (U =on-site Coulomb interaction) methods. We have found that the contribution near EF from Ce 4f states is negligible, suggesting that Ce 4f electrons are not the superconducting carriers. The total energy calculation indicates that the ABBA-type antiferromagnetic configuration is the most stable, while the stability is weakened by pressure. We have discussed the possible superconducting mechanism in the magnetic phase of CeTe1.82.

  20. Localized heating of electrons in ionization zones: Going beyond the Penning-Thornton paradigm in magnetron sputtering

    SciTech Connect

    Anders, André

    2014-12-15

    The fundamental question of how energy is supplied to a magnetron discharge is commonly answered by the Penning-Thornton paradigm invoking secondary electrons. Recently, Huo and coworkers (Plasma Sources Sci. Technol. 22, 045005 (2013)) used a global discharge model to show that electron heating in the electric field of the magnetic presheath is dominant over heating by secondary electrons. In this contribution, this concept is applied locally taking into account the electric potential structure of ionization zones. Images of ionization zones can and should be interpreted as diagrams of the localization of high electric potential and related electron energy.

  1. Electron localization in a mixed-valence diniobium benzene complex

    SciTech Connect

    Gianetti, Thomas L.; Nocton, Grégory; Minasian, Stefan G.; Kaltsoyannis, Nikolas; Kilcoyne, A. L. David; Kozimor, Stosh A.; Shuh, David K.; Tyliszczak, Tolek; Bergman, Robert G.; Arnold, John

    2014-11-11

    Reaction of the neutral diniobium benzene complex {[Nb(BDI)NtBu]2(μ-C6H6)} (BDI = N,N'-diisopropylbenzene-β-diketiminate) with Ag[B(C6F5)4] results in a single electron oxidation to produce a cationic diniobium arene complex, {[Nb(BDI)NtBu]2(μ-C6H6)}{B(C6F5)4}. Investigation of the solid state and solution phase structure using single-crystal X-ray diffraction, cyclic voltammetry, magnetic susceptibility, and multinuclear NMR spectroscopy indicates that the oxidation results in an asymmetric molecule with two chemically inequivalent Nb atoms. Further characterization using density functional theory (DFT) calculations, UV-visible, Nb L3,2-edge X-ray absorption near-edge structure (XANES), and EPR spectroscopies supports assignment of a diniobium complex, in which one Nb atom carries a single unpaired electron that is not largely delocalized on the second Nb atom. During the oxidative transformation, one electron is removed from the δ-bonding HOMO, which causes a destabilization of the molecule and formation of an asymmetric product. Subsequent reactivity studies indicate that the oxidized product allows access to metal-based chemistry with substrates that did not exhibit reactivity with the starting neutral complex.

  2. Electron localization in a mixed-valence diniobium benzene complex

    DOE PAGESBeta

    Gianetti, Thomas L.; Nocton, Grégory; Minasian, Stefan G.; Kaltsoyannis, Nikolas; Kilcoyne, A. L. David; Kozimor, Stosh A.; Shuh, David K.; Tyliszczak, Tolek; Bergman, Robert G.; Arnold, John

    2014-11-11

    Reaction of the neutral diniobium benzene complex {[Nb(BDI)NtBu]2(μ-C6H6)} (BDI = N,N'-diisopropylbenzene-β-diketiminate) with Ag[B(C6F5)4] results in a single electron oxidation to produce a cationic diniobium arene complex, {[Nb(BDI)NtBu]2(μ-C6H6)}{B(C6F5)4}. Investigation of the solid state and solution phase structure using single-crystal X-ray diffraction, cyclic voltammetry, magnetic susceptibility, and multinuclear NMR spectroscopy indicates that the oxidation results in an asymmetric molecule with two chemically inequivalent Nb atoms. Further characterization using density functional theory (DFT) calculations, UV-visible, Nb L3,2-edge X-ray absorption near-edge structure (XANES), and EPR spectroscopies supports assignment of a diniobium complex, in which one Nb atom carries a single unpaired electron that ismore » not largely delocalized on the second Nb atom. During the oxidative transformation, one electron is removed from the δ-bonding HOMO, which causes a destabilization of the molecule and formation of an asymmetric product. Subsequent reactivity studies indicate that the oxidized product allows access to metal-based chemistry with substrates that did not exhibit reactivity with the starting neutral complex.« less

  3. Electronic Structure and Properties of Organic Bulk-Heterojunction Interfaces.

    PubMed

    Street, Robert A

    2016-05-01

    The electronic structure and physical mechanisms of carrier generation and transport in the organic bulk heterojunction are reviewed. The electronic structure describes the bands and band-tail states, the band alignment at the bulk-heterojunction interface, and the overall density-of-states model. The different electronic character of excitons and mobile charge is discussed, the former being highly molecular and the latter more delocalized. Dissociation of the exciton via the charge-transfer (CT) states is attributed to weak binding of the CT state arising from charge delocalization. Carrier transport and charge collection is strongly influenced by the presence of localized band-tail states. Recombination is attributed primarily to transitions from mobile carriers to band-tail or deep trap states. PMID:26603977

  4. Electronic structure in the crossover regimes in lower dimensional structures

    NASA Astrophysics Data System (ADS)

    Batabyal, R.; Dev, B. N.

    2014-11-01

    Modern growth and fabrication techniques can produce lower dimensional structures in the crossover regimes. Such structures in the crossover regimes can provide tunability of various properties of materials. For example, a zero-dimensional (0-D) structure (quantum dot) evolving towards a 3-D structure (bulk) shows electronic structure, which is neither 0-D-like, nor 3-D-like in the dimensional crossover regime. Within the crossover regime the electronic density of states (DOS) at Fermi level (Ef) keeps on changing as the size of the system changes. DOS at Ef determines many properties of materials, such as electronic specific heat, spin susceptibility, etc. Such properties can be tuned by controlling the size of the system in the crossover regimes. Keeping the importance of DOS at Ef in mind, we determine their values and other details of electronic structure of lower dimensional structures, in the 0-D to 1-D, 1-D to 2-D, 2-D to 3-D, 0-D to 2-D, 0-D to 3-D and 1-D to 3-D crossover regimes, in a simple free electron model. We compare our results with analytical theory and experimental results, wherever available. We also present some results obtained by scanning tunneling spectroscopy measurements on Ag islands on Si(1 1 1) substrates evolving from a 0-D to a 2-D structure. This simple model is quite useful in understanding lower dimensional structures in the crossover regimes and, in general, in nanoscale science. Fabrication of such structures would provide control on materials properties.

  5. Structure refinement from precession electron diffraction data.

    PubMed

    Palatinus, Lukáš; Jacob, Damien; Cuvillier, Priscille; Klementová, Mariana; Sinkler, Wharton; Marks, Laurence D

    2013-03-01

    Electron diffraction is a unique tool for analysing the crystal structures of very small crystals. In particular, precession electron diffraction has been shown to be a useful method for ab initio structure solution. In this work it is demonstrated that precession electron diffraction data can also be successfully used for structure refinement, if the dynamical theory of diffraction is used for the calculation of diffracted intensities. The method is demonstrated on data from three materials - silicon, orthopyroxene (Mg,Fe)(2)Si(2)O(6) and gallium-indium tin oxide (Ga,In)(4)Sn(2)O(10). In particular, it is shown that atomic occupancies of mixed crystallographic sites can be refined to an accuracy approaching X-ray or neutron diffraction methods. In comparison with conventional electron diffraction data, the refinement against precession diffraction data yields significantly lower figures of merit, higher accuracy of refined parameters, much broader radii of convergence, especially for the thickness and orientation of the sample, and significantly reduced correlations between the structure parameters. The full dynamical refinement is compared with refinement using kinematical and two-beam approximations, and is shown to be superior to the latter two. PMID:23403968

  6. Evidence of local power deposition and electron heating by a standing electromagnetic wave in electron-cyclotron-resonance plasma.

    PubMed

    Durocher-Jean, A; Stafford, L; Dap, S; Makasheva, K; Clergereaux, R

    2014-09-01

    Microwave plasmas excited at electron-cyclotron resonance were studied in the 0.5-15 mTorr pressure range. In contrast with low-limit pressure conditions where the plasma emission highlights a fairly homogeneous spatial structure, a periodic spatial modulation (period ∼6.2 cm) appeared as pressure increased. This feature is ascribed to a local power deposition (related to the electron density) due to the presence of a standing electromagnetic wave created by the feed electromagnetic field (2.45 GHz) in the cavity formed by the reactor walls. Analysis of the electron energy probability function by Langmuir probe and optical emission spectroscopy further revealed the presence of a high-energy tail that showed strong periodic spatial modulation at higher pressure. The spatial evolution of the electron density and of the characteristic temperature of these high-energy electrons coincides with the nodes (maximum) and antinodes (minimum) of the standing wave. These spatially-modulated power deposition and electron heating mechanisms are then discussed. PMID:25314546

  7. Localize.pytom: a modern webserver for cryo-electron tomography.

    PubMed

    Hrabe, Thomas

    2015-07-01

    Localize.pytom, available through http://localize.pytom.org is a webserver for the localize module in the PyTom package. It is a free website and open to all users and there is no login requirement. The server accepts tomograms as they are imaged and reconstructed by Cryo-Electron Tomography (CET) and returns densities and coordinates of candidate-macromolecules in the tomogram. Localization of macromolecules in cryo-electron tomograms is one of the key procedures to unravel structural features of imaged macromolecules. Positions of localized molecules are further used for structural analysis by single particle procedures such as fine alignment, averaging and classification. Accurate localization can be furthermore used to generate molecular atlases of whole cells. Localization uses a cross-correlation-based score and requires a reference volume as input. A reference can either be a previously detected macromolecular structure or extrapolated on the server from a specific PDB chain. Users have the option to use either coarse or fine angular sampling strategies based on uniformly distributed rotations and to accurately compensate for the CET common 'Missing Wedge' artefact during sampling. After completion, all candidate macromolecules cut out from the tomogram are available for download. Their coordinates are stored and available in XML format, which can be easily integrated into successive analysis steps in other software. A pre-computed average of the first one hundred macromolecules is also available for immediate download, and the user has the option to further analyse the average, based on the detected score distribution in a novel web-density viewer. PMID:25934806

  8. Localize.pytom: a modern webserver for cryo-electron tomography

    PubMed Central

    Hrabe, Thomas

    2015-01-01

    Localize.pytom, available through http://localize.pytom.org is a webserver for the localize module in the PyTom package. It is a free website and open to all users and there is no login requirement. The server accepts tomograms as they are imaged and reconstructed by Cryo-Electron Tomography (CET) and returns densities and coordinates of candidate-macromolecules in the tomogram. Localization of macromolecules in cryo-electron tomograms is one of the key procedures to unravel structural features of imaged macromolecules. Positions of localized molecules are further used for structural analysis by single particle procedures such as fine alignment, averaging and classification. Accurate localization can be furthermore used to generate molecular atlases of whole cells. Localization uses a cross-correlation-based score and requires a reference volume as input. A reference can either be a previously detected macromolecular structure or extrapolated on the server from a specific PDB chain. Users have the option to use either coarse or fine angular sampling strategies based on uniformly distributed rotations and to accurately compensate for the CET common ‘Missing Wedge’ artefact during sampling. After completion, all candidate macromolecules cut out from the tomogram are available for download. Their coordinates are stored and available in XML format, which can be easily integrated into successive analysis steps in other software. A pre-computed average of the first one hundred macromolecules is also available for immediate download, and the user has the option to further analyse the average, based on the detected score distribution in a novel web-density viewer. PMID:25934806

  9. Local electron-electron interaction strength in ferromagnetic nickel determined by spin-polarized positron annihilation

    NASA Astrophysics Data System (ADS)

    Ceeh, Hubert; Weber, Josef Andreass; Böni, Peter; Leitner, Michael; Benea, Diana; Chioncel, Liviu; Ebert, Hubert; Minár, Jan; Vollhardt, Dieter; Hugenschmidt, Christoph

    2016-02-01

    We employ a positron annihilation technique, the spin-polarized two-dimensional angular correlation of annihilation radiation (2D-ACAR), to measure the spin-difference spectra of ferromagnetic nickel. The experimental data are compared with the theoretical results obtained within a combination of the local spin density approximation (LSDA) and the many-body dynamical mean-field theory (DMFT). We find that the self-energy defining the electronic correlations in Ni leads to anisotropic contributions to the momentum distribution. By direct comparison of the theoretical and experimental results we determine the strength of the local electronic interaction U in ferromagnetic Ni as 2.0 ± 0.1 eV.

  10. Local electron-electron interaction strength in ferromagnetic nickel determined by spin-polarized positron annihilation

    PubMed Central

    Ceeh, Hubert; Weber, Josef Andreass; Böni, Peter; Leitner, Michael; Benea, Diana; Chioncel, Liviu; Ebert, Hubert; Minár, Jan; Vollhardt, Dieter; Hugenschmidt, Christoph

    2016-01-01

    We employ a positron annihilation technique, the spin-polarized two-dimensional angular correlation of annihilation radiation (2D-ACAR), to measure the spin-difference spectra of ferromagnetic nickel. The experimental data are compared with the theoretical results obtained within a combination of the local spin density approximation (LSDA) and the many-body dynamical mean-field theory (DMFT). We find that the self-energy defining the electronic correlations in Ni leads to anisotropic contributions to the momentum distribution. By direct comparison of the theoretical and experimental results we determine the strength of the local electronic interaction U in ferromagnetic Ni as 2.0 ± 0.1 eV. PMID:26879249

  11. Local electron-electron interaction strength in ferromagnetic nickel determined by spin-polarized positron annihilation.

    PubMed

    Ceeh, Hubert; Weber, Josef Andreass; Böni, Peter; Leitner, Michael; Benea, Diana; Chioncel, Liviu; Ebert, Hubert; Minár, Jan; Vollhardt, Dieter; Hugenschmidt, Christoph

    2016-01-01

    We employ a positron annihilation technique, the spin-polarized two-dimensional angular correlation of annihilation radiation (2D-ACAR), to measure the spin-difference spectra of ferromagnetic nickel. The experimental data are compared with the theoretical results obtained within a combination of the local spin density approximation (LSDA) and the many-body dynamical mean-field theory (DMFT). We find that the self-energy defining the electronic correlations in Ni leads to anisotropic contributions to the momentum distribution. By direct comparison of the theoretical and experimental results we determine the strength of the local electronic interaction U in ferromagnetic Ni as 2.0 ± 0.1 eV. PMID:26879249

  12. Towards structural controllability of local-world networks

    NASA Astrophysics Data System (ADS)

    Sun, Shiwen; Ma, Yilin; Wu, Yafang; Wang, Li; Xia, Chengyi

    2016-05-01

    Controlling complex networks is of vital importance in science and engineering. Meanwhile, local-world effect is an important ingredient which should be taken into consideration in the complete description of real-world complex systems. In this letter, structural controllability of a class of local-world networks is investigated. Through extensive numerical simulations, firstly, effects of local world size M and network size N on structural controllability are examined. For local-world networks with sparse topological configuration, compared to network size, local-world size can induce stronger influence on controllability, however, for dense networks, controllability is greatly affected by network size and local-world effect can be neglected. Secondly, relationships between controllability and topological properties are analyzed. Lastly, the robustness of local-world networks under targeted attacks regarding structural controllability is discussed. These results can help to deepen the understanding of structural complexity and connectivity patterns of complex systems.

  13. Electronic structure engineering of various structural phases of phosphorene.

    PubMed

    Kaur, Sumandeep; Kumar, Ashok; Srivastava, Sunita; Tankeshwar, K

    2016-07-21

    We report the tailoring of the electronic structures of various structural phases of phosphorene (α-P, β-P, γ-P and δ-P) based homo- and hetero-bilayers through in-plane mechanical strains, vertical pressure and transverse electric field by employing density functional theory. In-plane biaxial strains have considerably modified the electronic bandgap of both homo- and hetero-bilayers while vertical pressure induces metallization in the considered structures. The γ-P homo-bilayer structure showed the highest ultimate tensile strength (UTS ∼ 6.21 GPa) upon in-plane stretching. Upon application of a transverse electric field, the variation in the bandgap of hetero-bilayers was found to be strongly dependent on the polarity of the applied field which is attributed to the counterbalance between the external electric field and the internal field induced by different structural phases and heterogeneity in the arrangements of atoms of each surface of the hetero-bilayer system. Our results demonstrate that the electronic structures of the considered hetero- and homo-bilayers of phosphorene could be modified by biaxial strain, pressure and electric field to achieve the desired properties for future nano-electronic devices. PMID:27334095

  14. Theoretical calculations of the electronic and vibrational structure of point defects in ionic crystals

    SciTech Connect

    Wood, R.F.; Wilson, T.M.

    1981-01-01

    The structure of the Hartree-Fock one-electron equations for simple point defects in ionic crystals are discussed. The importance of polarization effects due to the diffuse nature of the wavefunctions in the relaxed excited states are emphasized, and the usefulness of an effective mass approximation indicated. Several approaches to the calculation of the electronic structure are discussed and evaluated. The connection between electronic structure calculations and phonon perturbations are pointed out through a brief discussion of localized perturbation theory.

  15. Local atomic structure in disordered and nanocrystalline catalytic materials.

    SciTech Connect

    Dmowski, W.; Egami, T.; Swider-Lyons, K.; Dai, Sheng; Overbury, Steven {Steve} H

    2007-01-01

    The power of the atomic pair density function method to study the local atomic structure of dispersed materials is discussed for three examples (I) supercapacitor hydrous ruthenia, (II) electroctalyst platinum-iron phosphate and (III) nanoparticle gold catalyst. Hydrous ruthenia appears to be amorphous, but was found to be nanocomposite with RuO{sub 2} nanocrystals supporting electronic and hydrous boundaries protonic conductivity. A platinum-iron phosphate electrocatalyst, that exhibits activity for the oxygen reduction reaction has platinum in a non-metallic state. In catalysts comprised of gold nanoparticles supported on TiO{sub 2}, atomic correlations in the second atomic shell were observed suggesting interaction with the support that could modify gold chemical activity.

  16. Invariant current approach to wave propagation in locally symmetric structures

    NASA Astrophysics Data System (ADS)

    Zampetakis, V. E.; Diakonou, M. K.; Morfonios, C. V.; Kalozoumis, P. A.; Diakonos, F. K.; Schmelcher, P.

    2016-05-01

    A theory for wave mechanical systems with local inversion and translation symmetries is developed employing the two-dimensional solution space of the stationary Schrödinger equation. The local symmetries of the potential are encoded into corresponding local basis vectors in terms of symmetry-induced two-point invariant currents which map the basis amplitudes between symmetry-related points. A universal wavefunction structure in locally symmetric potentials is revealed, independently of the physical boundary conditions, by using special local bases which are adapted to the existing local symmetries. The local symmetry bases enable efficient computation of spatially resolved wave amplitudes in systems with arbitrary combinations of local inversion and translation symmetries. The approach opens the perspective of a flexible analysis and control of wave localization in structurally complex systems.

  17. Electronic structure and electron momentum density in TiSi

    NASA Astrophysics Data System (ADS)

    Ghaleb, A. M.; Mohammad, F. M.; Sahariya, Jagrati; Sharma, Mukesh; Ahuja, B. L.

    2013-03-01

    We report the electron momentum density in titanium monosilicide using 241Am Compton spectrometer. Experimental Compton profile has been compared with the theoretical profiles computed using linear combination of atomic orbitals (LCAO). The energy bands, density of states and Fermi surface structures of TiSi are reported using the LCAO and the full potential linearized augmented plane wave methods. Theoretical anisotropies in directional Compton profiles are interpreted in terms of energy bands. To confirm the conducting behavior, we also report the real space analysis of experimental Compton profile of TiSi.

  18. Electronic energy transfer: Localized operator partitioning of electronic energy in composite quantum systems

    NASA Astrophysics Data System (ADS)

    Khan, Yaser; Brumer, Paul

    2012-11-01

    A Hamiltonian based approach using spatially localized projection operators is introduced to give precise meaning to the chemically intuitive idea of the electronic energy on a quantum subsystem. This definition facilitates the study of electronic energy transfer in arbitrarily coupled quantum systems. In particular, the decomposition scheme can be applied to molecular components that are strongly interacting (with significant orbital overlap) as well as to isolated fragments. The result defines a consistent electronic energy at all internuclear distances, including the case of separated fragments, and reduces to the well-known Förster and Dexter results in their respective limits. Numerical calculations of coherent energy and charge transfer dynamics in simple model systems are presented and the effect of collisionally induced decoherence is examined.

  19. Electron density power spectrum in the local interstellar medium

    NASA Technical Reports Server (NTRS)

    Armstrong, J. W.; Rickett, B. J.; Spangler, S. R.

    1995-01-01

    Interstellar scintillation (ISS), fluctuations in the amplitude and phase of radio waves caused by scattering in the interstellar medium, is important as a diagnostic of interstellar plasma turbulence. ISS is also of interest because it is noise for other radio astronomical observations. The unifying concern is the power spectrum of the interstellar electron density. Here we use ISS observations through the nearby (less than or approximately =1 kpc) (ISM) to estimate the spectrum. From measurements of angular broadening of pulsars and extragalactic sources, decorrelation bandwidth of pulsars, refractive steering of features in pulsar dynamic spectra, dispersion measured fluctuations of pulsars, and refractive scintillation index measurements, we construct a composite structure function that is approximately power law over 2 x 10(exp 6) m less than scale less than 10(exp 13) m. The data are consistent with the structure function having a logarithmic slope versus baseline less than 2; thus there is a meaningful connection between scales in the radiowave fluctuation field and the scales in the electron density field causing the scattering. The data give an upper limit to the inner scale, l(sub o) less than or approximately 10(exp 8) m and are consistent with much smaller values. We construct a composite electron density spectrum that is approximately power law over at least the approximately = 5 decade wavenumber range 10(exp -13)/m less than wavenumber less than 10(exp -8)/m and that may extend to higher wavenumbers. The average spectral index of electron density over this wavenumber range is approximately = 3.7, very close to the value expected for a Kolmogorov process. The outer scale size, L(sub o), must be greater than or approximately = 10(exp 13) m (determined from dispersion measure fluctuations). When the ISS data are combined with measurements of differential Faraday rotation angle, and gradients in the average electron density, constraints can be put on the

  20. Electronic structure of bacterial surface protein layers

    SciTech Connect

    Maslyuk, Volodymyr V.; Mertig, Ingrid; Bredow, Thomas; Mertig, Michael; Vyalikh, Denis V.; Molodtsov, Serguei L.

    2008-01-15

    We report an approach for the calculation of the electronic density of states of the dried two-dimensional crystalline surface protein layer (S layer) of the bacterium Bacillus sphaericus NCTC 9602. The proposed model is based on the consideration of individual amino acids in the corresponding conformation of the peptide chain which additively contribute to the electronic structure of the entire protein complex. The derived results agree well with the experimental data obtained by means of photoemission (PE), resonant PE, and near-edge x-ray absorption spectroscopy.

  1. Structures of Local Rearrangements in Soft Colloidal Glasses

    NASA Astrophysics Data System (ADS)

    Yang, Xiunan; Liu, Rui; Yang, Mingcheng; Wang, Wei-Hua; Chen, Ke

    2016-06-01

    We image local structural rearrangements in soft colloidal glasses under small periodic perturbations induced by thermal cycling. Local structural entropy S2 positively correlates with observed rearrangements in colloidal glasses. The high S2 values of the rearranging clusters in glasses indicate that fragile regions in glasses are structurally less correlated, similar to structural defects in crystalline solids. Slow-evolving high S2 spots are capable of predicting local rearrangements long before the relaxations occur, while fluctuation-created high S2 spots best correlate with local deformations right before the rearrangement events. Local free volumes are also found to correlate with particle rearrangements at extreme values, although the ability to identify relaxation sites is substantially lower than S2. Our experiments provide an efficient structural identifier for the fragile regions in glasses and highlight the important role of structural correlations in the physics of glasses.

  2. Structures of Local Rearrangements in Soft Colloidal Glasses.

    PubMed

    Yang, Xiunan; Liu, Rui; Yang, Mingcheng; Wang, Wei-Hua; Chen, Ke

    2016-06-10

    We image local structural rearrangements in soft colloidal glasses under small periodic perturbations induced by thermal cycling. Local structural entropy S_{2} positively correlates with observed rearrangements in colloidal glasses. The high S_{2} values of the rearranging clusters in glasses indicate that fragile regions in glasses are structurally less correlated, similar to structural defects in crystalline solids. Slow-evolving high S_{2} spots are capable of predicting local rearrangements long before the relaxations occur, while fluctuation-created high S_{2} spots best correlate with local deformations right before the rearrangement events. Local free volumes are also found to correlate with particle rearrangements at extreme values, although the ability to identify relaxation sites is substantially lower than S_{2}. Our experiments provide an efficient structural identifier for the fragile regions in glasses and highlight the important role of structural correlations in the physics of glasses. PMID:27341261

  3. Rodlike localized structure in isotropic pattern-forming systems

    NASA Astrophysics Data System (ADS)

    Bordeu, Ignacio; Clerc, Marcel G.

    2015-10-01

    Stationary two-dimensional localized structures have been observed in a wide variety of dissipative systems. The existence, stability properties, dynamical evolution, and bifurcation diagram of an azimuthal symmetry breaking, rodlike localized structure in the isotropic prototype model of pattern formation, the Swift-Hohenberg model, is studied. These rodlike structures persist under the presence of nongradient perturbations. Interaction properties of the rodlike structures are studied. This allows us to envisage the possibility of different crystal-like configurations.

  4. Electronic structures of carbon nanotube peopods

    NASA Astrophysics Data System (ADS)

    Kuk, Young

    2003-03-01

    Carbon nanotubes have been successfully used for nanometer-sized devices such as diodes and transistors. These discrete devices utilize the spatially varying electronic structures of processed nanotubes by creating defect junctions or introducing substitutional or interstitial dopants. It was recently found that adsorption or insertion of molecules inside or outside of a nanotube modifies the electronic structure as observed with a low-temperature scanning tunneling microscope (LTSTM). We report a method to form spatial variation of the electronic structure by inserting various molecules such as fullerenes, metallo-fullerenes, metals or insulators. The results suggest that one can synthesize this band gap-engineered 1-dimensional wire by self-assembly instead of epitaxial growth. We propose a new type of device structure made by this processing technology. 1. J. Lee, H.J. Kim, G. Kim, Y.-W. Son, J. Ihm, S.J. Kahng, H. Kato, Z.W. Wang, T. Okazaki, H. Shinohara, and Y. Kuk, Nature, 415, 1005 (2002)

  5. Finding Common Ground: Creating Local Governance Structures.

    ERIC Educational Resources Information Center

    Mutchler, Sue E.; And Others

    As federal, state, and local policy makers attend to the economic, educational, social, and health-related needs of children, they are beginning to share a vision of a "seamless web" of high-quality, comprehensive, continuous services for children and their families. It remains a challenging goal because of the complexity of children's needs and…

  6. Electronic structure theory: Applications and geometrical aspects

    NASA Astrophysics Data System (ADS)

    Coh, Sinisa

    This thesis contains several applications of the first-principles electronic-structure theory with special emphasis in parts of the thesis on the geometrical aspects of the theory. We start by reviewing the basics of the first-principles electronic-structure methods which are then used throughout the thesis. The first application of these methods is on the analysis of the stability and lattice dynamics of alpha- and beta-cristobalite phases of SiO2. We also map the complete low-energy landscape connecting these two structures and give implications on the phase transition in this compound. Next we study a family of Pbnm perovskites that are promising candidates for silicon-compatible high-K dielectrics. We calculate their structure and dielectric response, and compare with experimental results where available. The third application of these methods is to the large isosymmetric reorientation of oxygen octahedra rotation axes in epitaxially strained perovskites. We explain the origin of the peculiar energy landscape topology as a function of epitaxial strain. In the part of the thesis devoted to the geometrical aspects of electronic structure theory, we begin by extending the concept of electronic polarization to a Chern insulators. These insulators are characterized by a non-zero off-diagonal sigma_xy conductivity tensor component, quantized in units of e 2/h. Finally we discuss another geometrical quantity, the Chern-Simons orbital magnetoelectric coupling. We present a first-principles based calculation of this quantity in several compounds, and motivated by recent developments in the theory of topological insulators, we speculate about the existence of "large-theta materials," in which this kind of coupling could be unusually large.

  7. Electronic Structure Studies of Amorphous Hydrogenated Boron Carbide

    NASA Astrophysics Data System (ADS)

    Sky Driver, M.; Sandstrom, Joseph; Boyko, Teak; Moewes, Alexander; Caruso, Anthony

    2010-03-01

    Boron carbide is a technologically relevant material with importance in voltaic transduction. However, the local physical, chemical and electronic structure of low temperature deposited thin films of amorphous boron carbide is far from understood, hindering its progress in application. X-ray absorption and emission spectroscopies (XAS/XES) were applied to thin films of B4C and B5C:Hx to study the near Fermi edge structure; the films were prepared by RF magnetron sputtering and plasma enhanced chemical vapor deposition (PECVD) and were thermally treated after deposition from 400 to 800 C. XES spectra indicate a physical structure transition from amorphous to nanocrystalline at 700 C, a much lower temperature than expected from traditional physical vapor deposition or flash annealing temperatures reported. These structural differences are of significant interest to transport measurements and will be discussed as a correlation. Further, x-ray and ultraviolet photoemission were also collected as a compliment to XES/XAS and will be discussed in the context of understanding the local intra vs. intermolecular electronic structure of these boron-rich molecular based solids.

  8. First-principles quantum transport with electron-vibration interactions: A maximally localized Wannier functions approach

    NASA Astrophysics Data System (ADS)

    Kim, Sejoong; Marzari, Nicola

    2013-06-01

    We present a first-principles approach for inelastic quantum transport calculations based on maximally localized Wannier functions. Electronic-structure properties are obtained from density-functional theory in a plane-wave basis, and electron-vibration coupling strengths and vibrational properties are determined with density-functional perturbation theory. Vibration-induced inelastic transport properties are calculated with nonequilibrium Green's function techniques; since these are based on a localized orbital representation we use maximally localized Wannier functions. Our formalism is applied first to investigate inelastic transport in a benzene molecular junction connected to monoatomic carbon chains. In this benchmark system the electron-vibration self-energy is calculated either in the self-consistent Born approximation or by lowest-order perturbation theory. It is observed that upward and downward conductance steps occur, which can be understood using multieigenchannel scattering theory and symmetry conditions. In a second example, where the monoatomic carbon chain electrode is replaced with a (3,3) carbon nanotube, we focus on the nonequilibrium vibration populations driven by the conducting electrons using a semiclassical rate equation and highlight and discuss in detail the appearance of vibrational cooling as a function of bias and the importance of matching the vibrational density of states of the conductor and the leads to minimize joule heating and breakdown.

  9. Electronic structure of oxygen functionalized graphene nanoribbons

    NASA Astrophysics Data System (ADS)

    Simbeck, Adam; Gu, Deyang; Kharche, Neerav; Nayak, Saroj

    2013-03-01

    We investigate the electronic and magnetic properties of armchair graphene nanoribbons whose edges are passivated by oxygen. Using a first-principles density functional approach and the many-body GW method we find that oxygen-passivation results in a rich geometrical environment which in turn determines the electronic and magnetic properties of the ribbon. For planar systems we report magnetic ground states whose electronic structure depends upon the magnetic coupling between edges. For non-planar ribbons we report a nonmagnetic ground state with a band gap that decreases as a function of increasing ribbon width. Our results will be discussed in light of previous experimental and computational studies. Interconnect Focus Center (MARCO program), State of New York, NSF IGERT program, Grant no. 0333314, and computing resources of the Computationial Center for Nanotechnology Innovation (CCNI), RPI

  10. Probing Structural and Electronic Dynamics with Ultrafast Electron Microscopy

    SciTech Connect

    Plemmons, DA; Suri, PK; Flannigan, DJ

    2015-05-12

    In this Perspective, we provide an overview,of the field of ultrafast electron microscopy (UEM). We begin by briefly discussing the emergence of methods for probing ultrafast structural dynamics and the information that can be obtained. Distinctions are drawn between the two main types a probes for femtosecond (fs) dynamics fast electrons and X-ray photons and emphasis is placed on hour the nature of charged particles is exploited in ultrafast electron-based' experiments:. Following this, we describe the versatility enabled by the ease with which electron trajectories and velocities can be manipulated with transmission electron microscopy (TEM): hardware configurations, and we emphasize how this is translated to the ability to measure scattering intensities in real, reciprocal, and energy space from presurveyed and selected rianoscale volumes. Owing to decades of ongoing research and development into TEM instrumentation combined with advances in specimen holder technology, comprehensive experiments can be conducted on a wide range of materials in various phases via in situ methods. Next, we describe the basic operating concepts, of UEM, and we emphasize that its development has led to extension of several of the formidable capabilities of TEM into the fs domain, dins increasing the accessible temporal parameter spade by several orders of magnitude. We then divide UEM studies into those conducted in real (imaging), reciprocal (diffraction), and energy (spectroscopy) spate. We begin each of these sections by providing a brief description of the basic operating principles and the types of information that can be gathered followed by descriptions of how these approaches are applied in UM, the type of specimen parameter space that can be probed, and an example of the types of dynamics that can be resolved. We conclude with an Outlook section, wherein we share our perspective on some future directions of the field pertaining to continued instrument development and

  11. Localized itinerant electrons and unique magnetic properties of SrRu2O6

    NASA Astrophysics Data System (ADS)

    Streltsov, S.; Mazin, I. I.; Foyevtsova, K.

    2015-10-01

    SrRu2O6 has unique magnetic properties. It is characterized by a very high Néel temperature, despite its quasi-two-dimensional structure, and has a magnetic moment more than twice reduced compared to the formal ionic count. First-principles calculations show that only an ideal Néel ordering in the Ru plane is possible, with no other metastable magnetic solutions, and, highly unusually, yield dielectric gaps for both antiferromagnetic and nonmagnetic states. We demonstrate that this strange behavior is the result of the formation of very specific electronic objects, recently suggested for a geometrically similar Na2IrO3 compound, whereby each electron is well localized on a particular Ru6 hexagon, and completely delocalized over the corresponding six Ru sites, thus making the compound both strongly localized and highly itinerant.

  12. Local structure of solid Rb at megabar pressures

    NASA Astrophysics Data System (ADS)

    De Panfilis, S.; Gorelli, F.; Santoro, M.; Ulivi, L.; Gregoryanz, E.; Irifune, T.; Shinmei, T.; Kantor, I.; Mathon, O.; Pascarelli, S.

    2015-06-01

    We have investigated the local and electronic structure of solid rubidium by means of x-ray absorption spectroscopy up to 101.0 GPa, thus doubling the maximum investigated experimental pressure. This study confirms the predicted stability of phase VI and was completed by the combination of two pivotal instrumental solutions. On one side, we made use of nanocrystalline diamond anvils, which, contrary to the more commonly used single crystal diamond anvils, do not generate sharp Bragg peaks (glitches) at specific energies that spoil the weak fine structure oscillations in the x-ray absorption cross section. Second, we exploited the performance of a state-of-the-art x-ray focussing device yielding a beam spot size of 5 × 5 μm2, spatially stable over the entire energy scan. An advanced data analysis protocol was implemented to extract the pressure dependence of the structural parameters in phase VI of solid Rb from 51.2 GPa up to the highest pressure. A continuous reduction of the nearest neighbour distances was observed, reaching about 6% over the probed pressure range. We also discuss a phenomenological model based on the Einstein approximation to describe the pressure behaviour of the mean-square relative displacement. Within this simplified scheme, we estimate the Grüneisen parameter for this high pressure Rb phase to be in the 1.3-1.5 interval.

  13. Local structure of solid Rb at megabar pressures.

    PubMed

    De Panfilis, S; Gorelli, F; Santoro, M; Ulivi, L; Gregoryanz, E; Irifune, T; Shinmei, T; Kantor, I; Mathon, O; Pascarelli, S

    2015-06-01

    We have investigated the local and electronic structure of solid rubidium by means of x-ray absorption spectroscopy up to 101.0 GPa, thus doubling the maximum investigated experimental pressure. This study confirms the predicted stability of phase VI and was completed by the combination of two pivotal instrumental solutions. On one side, we made use of nanocrystalline diamond anvils, which, contrary to the more commonly used single crystal diamond anvils, do not generate sharp Bragg peaks (glitches) at specific energies that spoil the weak fine structure oscillations in the x-ray absorption cross section. Second, we exploited the performance of a state-of-the-art x-ray focussing device yielding a beam spot size of 5 × 5 μm(2), spatially stable over the entire energy scan. An advanced data analysis protocol was implemented to extract the pressure dependence of the structural parameters in phase VI of solid Rb from 51.2 GPa up to the highest pressure. A continuous reduction of the nearest neighbour distances was observed, reaching about 6% over the probed pressure range. We also discuss a phenomenological model based on the Einstein approximation to describe the pressure behaviour of the mean-square relative displacement. Within this simplified scheme, we estimate the Grüneisen parameter for this high pressure Rb phase to be in the 1.3-1.5 interval. PMID:26049504

  14. Local structure of solid Rb at megabar pressures

    SciTech Connect

    De Panfilis, S.; Gorelli, F.; Santoro, M.; Ulivi, L.; Gregoryanz, E.; Irifune, T.; Shinmei, T.; Kantor, I.; Mathon, O.; Pascarelli, S.

    2015-06-07

    We have investigated the local and electronic structure of solid rubidium by means of x-ray absorption spectroscopy up to 101.0 GPa, thus doubling the maximum investigated experimental pressure. This study confirms the predicted stability of phase VI and was completed by the combination of two pivotal instrumental solutions. On one side, we made use of nanocrystalline diamond anvils, which, contrary to the more commonly used single crystal diamond anvils, do not generate sharp Bragg peaks (glitches) at specific energies that spoil the weak fine structure oscillations in the x-ray absorption cross section. Second, we exploited the performance of a state-of-the-art x-ray focussing device yielding a beam spot size of 5 × 5 μm{sup 2}, spatially stable over the entire energy scan. An advanced data analysis protocol was implemented to extract the pressure dependence of the structural parameters in phase VI of solid Rb from 51.2 GPa up to the highest pressure. A continuous reduction of the nearest neighbour distances was observed, reaching about 6% over the probed pressure range. We also discuss a phenomenological model based on the Einstein approximation to describe the pressure behaviour of the mean-square relative displacement. Within this simplified scheme, we estimate the Grüneisen parameter for this high pressure Rb phase to be in the 1.3–1.5 interval.

  15. Electronic Structure of Iridium Clusters on Graphene

    NASA Astrophysics Data System (ADS)

    Barker, Bradford A.; Bradley, Aaron J.; Ugeda, Miguel M.; Coh, Sinisa; Zettl, Alex; Crommie, Michael F.; Cohen, Marvin L.; Louie, Steven G.

    2015-03-01

    Graphene was predicted to exhibit non-trivial Z2 topology, but its exceedingly weak spin-orbit coupling prevented this from being observed. Previous theoretical work has proposed enhancing the spin-orbit coupling strength by depositing individual adatoms adsorbed onto the surface of graphene. We show experimental evidence that the iridium adatoms cluster, with a cluster size of at least two atoms. We investigate through theoretical calculations the orientation of the iridium dimers on graphene, contrast the electronic structure of iridium dimers with iridium monomers, and compare the theoretical iridium dimer electronic structure calculations with the experimental results determined via scanning tunneling spectroscopy. This work was supported by NSF Grant No. DMR10-1006184 and U.S. DOE under Contract No. DE-AC02-05CH11231. Computational resources have been provided by DOE at LBNL's NERSC facility.

  16. Electronic structure of the multivacancies in Si

    NASA Astrophysics Data System (ADS)

    Ren, Shang Yuan; Mao, Deqiang; Li, Mingfu

    A complete set of equations for determining the energy levels and the wavefunctions with different symmetries of electronic states of several well-known multivacancies in Si is given using the Koster-Slater Green's function method. By using an empirical tight binding Hamiltonian for the band structure of the host and the central-cell perturbation approximation for the defect, only the on-site and the off-site Green's functions of the host and their derivatives with respect to energy E appear in these equations. The electronic structure of the ideal multivacancies, especially the divacancy, are investigated and compared with known experimental results and previous qualitative analyses. Some misunderstandings of the experimental results are analyzed. The wavefunctions of some multivacancy states are accurately evaluated and compared with the EPR and ENDOR data for the first time.

  17. Structural and electronic properties of sodium nanoclusters

    NASA Astrophysics Data System (ADS)

    Perez, Luis A.; Reyes-Nava, Juan A.; Garzon, Ignacio L.

    2006-03-01

    Recent advances on mass selection of sodium nanoclusters and their characterization by photoemission electron spectroscopy [1] have given useful data for a variety of clusters sizes. These data may lead to assignments of the relevant structures by comparing the measured photoelectron spectra (PES) with the electronic density of states (DOS) obtained from DFT calculations. In this work, the lowest energy structures modeled by the many-body Gupta potential, are obtained by using molecular dynamics simulations for Nan (n= 178, 204, 271, 298-300, 309). DFT calculations were then performed for neutral, positively- and negatively-charged Nan clusters. A comparison between the DOS of clusters of the same size but different charge will be presented, as well as between the available experimental PES and the theoretical obtained DOS.[1] H. Haberland, T. Hippler, J. Donges, O. Kostko, M. Schmidt, B. von Issendorff, Phys. Rev. Lett. 94, 035701 (2005).

  18. Structure and Electronic Properties of Polycrystalline Dielectrics

    SciTech Connect

    Mckenna, Keith P.; Shluger, AL

    2013-07-07

    We present an overview of the theoretical approaches that can be employed to model polycrystalline oxides along with a discussion of their limitations and associated challenges. We then present results for two metal oxide materials, MgO and HfO2, where theory and experiment have come together to provide insight into the structure and electronic properties of grain boundaries. Finally, we conclude with a discussion and outlook.

  19. Polycrystalline graphene with single crystalline electronic structure.

    PubMed

    Brown, Lola; Lochocki, Edward B; Avila, José; Kim, Cheol-Joo; Ogawa, Yui; Havener, Robin W; Kim, Dong-Ki; Monkman, Eric J; Shai, Daniel E; Wei, Haofei I; Levendorf, Mark P; Asensio, María; Shen, Kyle M; Park, Jiwoong

    2014-10-01

    We report the scalable growth of aligned graphene and hexagonal boron nitride on commercial copper foils, where each film originates from multiple nucleations yet exhibits a single orientation. Thorough characterization of our graphene reveals uniform crystallographic and electronic structures on length scales ranging from nanometers to tens of centimeters. As we demonstrate with artificial twisted graphene bilayers, these inexpensive and versatile films are ideal building blocks for large-scale layered heterostructures with angle-tunable optoelectronic properties. PMID:25207847

  20. Smart electronics and MEMS for aerospace structures

    NASA Astrophysics Data System (ADS)

    Varadan, Vijay K.; Varadan, Vasundara V.

    1995-09-01

    In this paper, smart electronics and MEMS are employed to sense and control the drag in aircraft structures. The sensors are fabricated with interdigital transducers printed on a piezoelectric polymer. They in turn are mounted onto an ultra thin Penn State's novel RF antenna (Patent field). The sensor are designed to measure both pressure and shear of the fluid flow on aerospace structures. The wave form measurements may be monitored at a remote location either at the cockpit or elsewhere via the antennas in the sensors and an outside antenna. The integrated MEMS actuators which comprise of cantilever-, diaphram- and microbridge-based MEMS with suitable smart electronics etched onto the structure are controlled by the built-in antennas through feedback and feedforward control architecture. The integration of such materials and smart electronics into the skin of airfoil is ideal for sensing and controlling drag. The basic idea of this concept involves detection of the point of transition from laminar to turbulent flow and transmitting acoustical energy into the boundary layer so that the low energy fluid particles accelerate in the transverse direction and mix with the high energy flow outside of the boundary layer. 3D microriblets can be fabricated using stereo lithography and UV curable conducting polymers. The control of drag using these active microriblets are outlined.

  1. Spatially Resolved Electronic Structures of Atomically Precise Armchair Graphene Nanoribbons

    NASA Astrophysics Data System (ADS)

    Huang, Han; Wei, Dacheng; Sun, Jiatao; Wong, Swee Liang; Feng, Yuan Ping; Neto, A. H. Castro; Wee, Andrew Thye Shen

    2012-12-01

    Graphene has attracted much interest in both academia and industry. The challenge of making it semiconducting is crucial for applications in electronic devices. A promising approach is to reduce its physical size down to the nanometer scale. Here, we present the surface-assisted bottom-up fabrication of atomically precise armchair graphene nanoribbons (AGNRs) with predefined widths, namely 7-, 14- and 21-AGNRs, on Ag(111) as well as their spatially resolved width-dependent electronic structures. STM/STS measurements reveal their associated electron scattering patterns and the energy gaps over 1 eV. The mechanism to form such AGNRs is addressed based on the observed intermediate products. Our results provide new insights into the local properties of AGNRs, and have implications for the understanding of their electrical properties and potential applications.

  2. Spatially Resolved Electronic Structures of Atomically Precise Armchair Graphene Nanoribbons

    PubMed Central

    Huang, Han; Wei, Dacheng; Sun, Jiatao; Wong, Swee Liang; Feng, Yuan Ping; Neto, A. H. Castro; Wee, Andrew Thye Shen

    2012-01-01

    Graphene has attracted much interest in both academia and industry. The challenge of making it semiconducting is crucial for applications in electronic devices. A promising approach is to reduce its physical size down to the nanometer scale. Here, we present the surface-assisted bottom-up fabrication of atomically precise armchair graphene nanoribbons (AGNRs) with predefined widths, namely 7-, 14- and 21-AGNRs, on Ag(111) as well as their spatially resolved width-dependent electronic structures. STM/STS measurements reveal their associated electron scattering patterns and the energy gaps over 1 eV. The mechanism to form such AGNRs is addressed based on the observed intermediate products. Our results provide new insights into the local properties of AGNRs, and have implications for the understanding of their electrical properties and potential applications. PMID:23248746

  3. Electronic Structure Studies of Silicon Carbide Cationic Nanoclusters

    NASA Astrophysics Data System (ADS)

    Pradhan, Prachi

    2005-03-01

    As a continuation of our studies on the high stabilities and associated electronic structure properties of Si8C2 to Si14C2 and Si20Cn (n=3-6) clusters,^1 we report here detailed ab initio electronic and geometric structure studies of small SimCn^+ (1< m, n < 4) cationic clusters. The theoretical formalism used is the local density approximation (LDA) to density functional theory (DFT) and the Gaussian03 suite of programs^2 with an all electron 6-311++G** basis set has been used. Complete geometry optimizations of different possible structures have been carried out. The stability of the clusters varies with the ratio of the number of silicon to carbon atoms in the cluster. In contrast to the neutral clusters,^3 cationic clusters appear to prefer more open structures. Results will be presented for binding energies, relative energies, fragmentation energies, vibrational frequencies, and adiabatic ionization potentials^3 for the optimized clusters. Detailed comparisons with published data in the literature will also be presented. * Work supported, in part, by the Welch Foundation, Houston, Texas (Grant No. Y-1525) ^1M. N. Huda and A. K. Ray, Phys. Rev. A (R) 69, 011201 (2004); Eur. Phys. J. D 31, 63 (2004). ^2 Gaussian03, Revision A.1, M. J. Frisch et al., Gaussian Inc., Pittsburgh, PA , 2003. ^3 P. Pradhan and A. K. Ray, J. Mol. Structure (Theochem), in press.

  4. A Toolbox for Controlling the Energetics and Localization of Electronic States in Self‐Assembled Organic Monolayers

    PubMed Central

    Kretz, Bernhard; Egger, David A.

    2015-01-01

    Controlling the nature of the electronic states within organic layers holds the promise of truly molecular electronics. To achieve that we, here, develop a modular concept for a versatile tuning of electronic properties in organic monolayers and their interfaces. The suggested strategy relies on directly exploiting collective electrostatic effects, which emerge naturally in an ensemble of polar molecules. By means of quantum‐mechanical modeling we show that in this way monolayer‐based quantum‐cascades and quantum‐well structures can be realized, which allow a precise control of the local electronic structure and the localization of electronic states. Extending that concept, we furthermore discuss strategies for activating spin sensitivity in specific regions of an organic monolayer.

  5. Electronic structure of interfaces between hexagonal and rhombohedral graphite

    NASA Astrophysics Data System (ADS)

    Taut, M.; Koepernik, K.

    2016-07-01

    An analysis of the electronic structure of interfaces between hexagonal (A B ) and rhombohedral (A B C ) graphite based on density functional theory is presented. Both of the two simplest interface structures host (localized) interface bands, which are located around the K point in the Brillouin zone, and which give rise to strong peaks in the density of states at the Fermi level. All interface bands near the Fermi energy are localized at monomers (single atoms with dangling pz orbitals), whereas those around 0.5 eV belong to pz-bonded trimers, which are introduced by the interface and which are not found in the two adjacent bulk substances. There is also an interface band at the (A B ) side of the interface which resembles one of the interface states near a stacking fault in (A B ) graphite.

  6. Localized heating of electrons in ionization zones: Going beyond the Penning-Thornton paradigm in magnetron sputtering

    SciTech Connect

    Anders, Andre

    2014-12-07

    The fundamental question of how energy is supplied to a magnetron discharge is commonly answered by the Penning-Thornton paradigm invoking secondary electrons. Huo et al. (Plasma Sources Sci. Technol. 22, 045005, (2013)) used a global discharge model to show that electron heating in the electric field of the magnetic presheath is dominant. In this contribution, this concept is applied locally taking into account the electric potential structure of ionization zones. Images of ionization zones can and should be interpreted as diagrams of the localization of electric potential and related electron energy, where certain collisions promote or dampen their formation.

  7. Atomic and electronic structure of Ni-Nb metallic glasses

    SciTech Connect

    Yuan, C. C.; Yang, Y.-F. Xi, X. K.

    2013-12-07

    Solid state {sup 93}Nb nuclear magnetic resonance spectroscopy has been employed to investigate the atomic and electronic structures in Ni-Nb based metallic glass (MG) model system. {sup 93}Nb nuclear magnetic resonance (NMR) isotropic metallic shift of Ni{sub 60}Nb{sub 35}Sn{sub 5} has been found to be ∼100 ppm lower than that of Ni{sub 60}Nb{sub 35}Zr{sub 5} MG, which is correlated with their intrinsic fracture toughness. The evolution of {sup 93}Nb NMR isotropic metallic shifts upon alloying is clearly an electronic origin, as revealed by both local hyperfine fields analysis and first-principle computations. This preliminary result indicates that, in addition to geometrical considerations, atomic form factors should be taken into a description of atomic structures for better understanding the mechanical behaviors of MGs.

  8. A Synchrotron Investigation Of The Electronic Structure Of Lanthanide Zirconates

    NASA Astrophysics Data System (ADS)

    Clements, Richard; Kennedy, Brendan; Ling, Christopher; Stampfl, Anton P. J.

    2010-03-01

    abstract- The lanthanide zirconates are of interest for use in inert matrix fuels and nuclear wasteforms. For use in these applications, the material's structure must be resistant to radiation damage and its thermal, thermodynamic and mechanical properties must be known. The rare earth zirconates are interesting model systems to explore such problems. In such materials the f-electrons may play a localized valence decisive role in determining their thermo-mechanical properties. We have undertaken a synthesis of the full range of the lanthanide zirconate series using solid state techniques. We have performed X-ray photoemission spectroscopy (XPS) and X-ray absorption near edge spectroscopy (XANES) with synchrotron radiation on a selection of the series, in conjunction with a density functional theory (DFT) determination of the electronic structure. -

  9. Elongation method for electronic structure calculations of random DNA sequences.

    PubMed

    Orimoto, Yuuichi; Liu, Kai; Aoki, Yuriko

    2015-10-30

    We applied ab initio order-N elongation (ELG) method to calculate electronic structures of various deoxyribonucleic acid (DNA) models. We aim to test potential application of the method for building a database of DNA electronic structures. The ELG method mimics polymerization reactions on a computer and meets the requirements for linear scaling computational efficiency and high accuracy, even for huge systems. As a benchmark test, we applied the method for calculations of various types of random sequenced A- and B-type DNA models with and without counterions. In each case, the ELG method maintained high accuracy with small errors in energy on the order of 10(-8) hartree/atom compared with conventional calculations. We demonstrate that the ELG method can provide valuable information such as stabilization energies and local densities of states for each DNA sequence. In addition, we discuss the "restarting" feature of the ELG method for constructing a database that exhaustively covers DNA species. PMID:26337429

  10. Localized reconstruction of subunits from electron cryomicroscopy images of macromolecular complexes.

    PubMed

    Ilca, Serban L; Kotecha, Abhay; Sun, Xiaoyu; Poranen, Minna M; Stuart, David I; Huiskonen, Juha T

    2015-01-01

    Electron cryomicroscopy can yield near-atomic resolution structures of highly ordered macromolecular complexes. Often however some subunits bind in a flexible manner, have different symmetry from the rest of the complex, or are present in sub-stoichiometric amounts, limiting the attainable resolution. Here we report a general method for the localized three-dimensional reconstruction of such subunits. After determining the particle orientations, local areas corresponding to the subunits can be extracted and treated as single particles. We demonstrate the method using three examples including a flexible assembly and complexes harbouring subunits with either partial occupancy or mismatched symmetry. Most notably, the method allows accurate fitting of the monomeric RNA-dependent RNA polymerase bound at the threefold axis of symmetry inside a viral capsid, revealing for the first time its exact orientation and interactions with the capsid proteins. Localized reconstruction is expected to provide novel biological insights in a range of challenging biological systems. PMID:26534841

  11. Localized reconstruction of subunits from electron cryomicroscopy images of macromolecular complexes

    PubMed Central

    Ilca, Serban L.; Kotecha, Abhay; Sun, Xiaoyu; Poranen, Minna M.; Stuart, David I.; Huiskonen, Juha T.

    2015-01-01

    Electron cryomicroscopy can yield near-atomic resolution structures of highly ordered macromolecular complexes. Often however some subunits bind in a flexible manner, have different symmetry from the rest of the complex, or are present in sub-stoichiometric amounts, limiting the attainable resolution. Here we report a general method for the localized three-dimensional reconstruction of such subunits. After determining the particle orientations, local areas corresponding to the subunits can be extracted and treated as single particles. We demonstrate the method using three examples including a flexible assembly and complexes harbouring subunits with either partial occupancy or mismatched symmetry. Most notably, the method allows accurate fitting of the monomeric RNA-dependent RNA polymerase bound at the threefold axis of symmetry inside a viral capsid, revealing for the first time its exact orientation and interactions with the capsid proteins. Localized reconstruction is expected to provide novel biological insights in a range of challenging biological systems. PMID:26534841

  12. Local structure of equality constrained NLP problems

    SciTech Connect

    Mari, J.

    1994-12-31

    We show that locally around a feasible point, the behavior of an equality constrained nonlinear program is described by the gradient and the Hessian of the Lagrangian on the tangent subspace. In particular this holds true for reduced gradient approaches. Applying the same ideas to the control of nonlinear ODE:s, one can device first and second order methods that can be applied also to stiff problems. We finally describe an application of these ideas to the optimization of the production of human growth factor by fed-batch fermentation.

  13. Electronic structure and crystal phase stability of palladium hydrides

    SciTech Connect

    Houari, Abdesalem; Matar, Samir F.; Eyert, Volker

    2014-11-07

    The results of electronic structure calculations for a variety of palladium hydrides are presented. The calculations are based on density functional theory and used different local and semilocal approximations. The thermodynamic stability of all structures as well as the electronic and chemical bonding properties are addressed. For the monohydride, taking into account the zero-point energy is important to identify the octahedral Pd-H arrangement with its larger voids and, hence, softer hydrogen vibrational modes as favorable over the tetrahedral arrangement as found in the zincblende and wurtzite structures. Stabilization of the rocksalt structure is due to strong bonding of the 4d and 1s orbitals, which form a characteristic split-off band separated from the main d-band group. Increased filling of the formerly pure d states of the metal causes strong reduction of the density of states at the Fermi energy, which undermines possible long-range ferromagnetic order otherwise favored by strong magnetovolume effects. For the dihydride, octahedral Pd-H arrangement as realized, e.g., in the pyrite structure turns out to be unstable against tetrahedral arrangement as found in the fluorite structure. Yet, from both heat of formation and chemical bonding considerations, the dihydride turns out to be less favorable than the monohydride. Finally, the vacancy ordered defect phase Pd{sub 3}H{sub 4} follows the general trend of favoring the octahedral arrangement of the rocksalt structure for Pd:H ratios less or equal to one.

  14. Electronic Structure of NiPdP Amorphous Metals

    NASA Astrophysics Data System (ADS)

    Swihart, J. C.; Nicholson, D. M. C.; Shelton, W. A.; Wang, Y.

    1996-03-01

    The understanding of the structure, properties and required cooling rates for bulk amorphous alloys is hindered by the the large number of constituents in the typical alloy. One of the compositionally simplest systems that can be cast into bulk specimens is Ni_0.4Pd_0.4P_0.2. Furthermore, the thoroughly studied structure of amorphous Ni_0.8P_0.2 provides a useful starting point for its investigation. We use the locally selfconsistent multiple scattering (LSMS) method to determine the electronic structure, mass density, and energy as Pd is substituted at random for Ni in the Ni_0.8P_0.2 amorphous structure. Work supported by Laboratory Directors Research Development program at Oak Ridge National Laboratory, Division of Materials Science, and the Mathematical Information and Computational Science Division of the Office of Computational Technology Research, US DOE under subcontract DEAC05-84OR21400 with Lockheed-Martin Energy Systems, Inc.

  15. Local Moments and Localized Conduction Electrons in Amorphous Gadolinium-Silicon

    NASA Astrophysics Data System (ADS)

    Zink, B. L.; Queen, D. R.; Sappey, R.; Revaz, B.; Janod, E.; Potok, R. M.; Hellman, F.

    2000-03-01

    Investigations of amorphous gadolinium-silicon have revealed many fascinating phenomena including enormous negative magnetoresistance and spin glass behavior that give insight into magnetic interactions near a Metal-Insulator transition(F. Hellman et al., PRL 77, 4652 (1996))^,(P. Xiong et al., PRB 59, R3929 (1999))^,(F. Hellman et al., submitted to PRL). The heat capacities of a-GdSi thin-films measured with our unique microcalorimeter show large magnetic contributions at temperatures below 40 K. The resulting magnetic entropy is larger than that available from Gd moments alone. We suggest that this additional entropy is provided by the interaction of localized electron spins with the Gd moments(B. L. Zink et al., PRL 83, 2266 (1999)). New heat capacity data on samples with different compositions, at temperatures below the spin glass freezing temperature and in large magnetic fields provides further insight into these dramatic phenomena and the magnetic interactions that cause them.

  16. Enhancing community detection by using local structural information

    NASA Astrophysics Data System (ADS)

    Xiang, Ju; Hu, Ke; Zhang, Yan; Bao, Mei-Hua; Tang, Liang; Tang, Yan-Ni; Gao, Yuan-Yuan; Li, Jian-Ming; Chen, Benyan; Hu, Jing-Bo

    2016-03-01

    Many real-world networks, such as gene networks, protein-protein interaction networks and metabolic networks, exhibit community structures, meaning the existence of groups of densely connected vertices in the networks. Many local similarity measures in the networks are closely related to the concept of the community structures, and may have a positive effect on community detection in the networks. Here, various local similarity measures are used to extract local structural information, which is then applied to community detection in the networks by using the edge-reweighting strategy. The effect of the local similarity measures on community detection is carefully investigated and compared in various networks. The experimental results show that the local similarity measures are crucial for the improvement of community detection methods, while the positive effect of the local similarity measures is closely related to the networks under study and applied community detection methods.

  17. Thermal transfer structures coupling electronics card(s) to coolant-cooled structure(s)

    DOEpatents

    David, Milnes P; Graybill, David P; Iyengar, Madhusudan K; Kamath, Vinod; Kochuparambil, Bejoy J; Parida, Pritish R; Schmidt, Roger R

    2014-12-16

    Cooling apparatuses and coolant-cooled electronic systems are provided which include thermal transfer structures configured to engage with a spring force one or more electronics cards with docking of the electronics card(s) within a respective socket(s) of the electronic system. A thermal transfer structure of the cooling apparatus includes a thermal spreader having a first thermal conduction surface, and a thermally conductive spring assembly coupled to the conduction surface of the thermal spreader and positioned and configured to reside between and physically couple a first surface of an electronics card to the first surface of the thermal spreader with docking of the electronics card within a socket of the electronic system. The thermal transfer structure is, in one embodiment, metallurgically bonded to a coolant-cooled structure and facilitates transfer of heat from the electronics card to coolant flowing through the coolant-cooled structure.

  18. Electronic structure theory of the superheavy elements

    NASA Astrophysics Data System (ADS)

    Eliav, Ephraim; Fritzsche, Stephan; Kaldor, Uzi

    2015-12-01

    High-accuracy calculations of atomic properties of the superheavy elements (SHE) up to element 122 are reviewed. The properties discussed include ionization potentials, electron affinities and excitation energies, which are associated with the spectroscopic and chemical behavior of these elements, and are therefore of considerable interest. Accurate predictions of these quantities require high-order inclusion of relativity and electron correlation, as well as large, converged basis sets. The Dirac-Coulomb-Breit Hamiltonian, which includes all terms up to second order in the fine-structure constant α, serves as the framework for the treatment; higher-order Lamb shift terms are considered in some selected cases. Electron correlation is treated by either the multiconfiguration self-consistent-field approach or by Fock-space coupled cluster theory. The latter is enhanced by the intermediate Hamiltonian scheme, allowing the use of larger model (P) spaces. The quality of the calculations is assessed by applying the same methods to lighter homologs of the SHEs and comparing with available experimental information. Very good agreement is obtained, within a few hundredths of an eV, and similar accuracy is expected for the SHEs. Many of the properties predicted for the SHEs differ significantly from what may be expected by straightforward extrapolation of lighter homologs, demonstrating that the structure and chemistry of SHEs are strongly affected by relativity. The major scientific challenge of the calculations is to find the electronic structure and basic atomic properties of the SHE and assign its proper place in the periodic table. Significant recent developments include joint experimental-computational studies of the excitation spectrum of Fm and the ionization energy of Lr, with excellent agreement of experiment and theory, auguring well for the future of research in the field.

  19. Resolving Presynaptic Structure by Electron Tomography

    PubMed Central

    Perkins, Guy A.; Jackson, Dakota R.; Spirou, George A.

    2016-01-01

    A key goal in neurobiology is to generate a theoretical framework that merges structural, physiological and molecular explanations of brain function. These categories of explanation do not advance in synchrony; advances in one category define new experiments in other categories. For example, the synapse was defined physiologically and biochemically before it was visualized using electron microscopy. Indeed, the original descriptions of synapses in the 1950s were lent credence by the presence of spherical vesicles in presynaptic terminals that were considered to be the substrate for quantal neurotransmission. In the last few decades, our understanding of synaptic function has again been driven by physiological and molecular techniques. The key molecular players for synaptic vesicle structure, mobility and fusion were identified and applications of the patch clamp technique permitted physiological estimation of neurotransmitter release and receptor properties. These advances demand higher resolution structural images of synapses. During the 1990s a second renaissance in cell biology driven by EM was fueled by improved techniques for electron tomography (ET) with the ability to compute virtual images with nm resolution between image planes. Over the last fifteen years, ET has been applied to the presynaptic terminal with special attention to the active zone and organelles of the nerve terminal. In this review, we first summarize the technical improvements that have led to a resurgence in utilization of ET and then we summarize new insights gained by the application of ET to reveal the high-resolution structure of the nerve terminal. PMID:25683026

  20. Resolving presynaptic structure by electron tomography.

    PubMed

    Perkins, Guy A; Jackson, Dakota R; Spirou, George A

    2015-05-01

    A key goal in neurobiology is to generate a theoretical framework that merges structural, physiological, and molecular explanations of brain function. These categories of explanation do not advance in synchrony; advances in one category define new experiments in other categories. For example, the synapse was defined physiologically and biochemically before it was visualized using electron microscopy. Indeed, the original descriptions of synapses in the 1950s were lent credence by the presence of spherical vesicles in presynaptic terminals that were considered to be the substrate for quantal neurotransmission. In the last few decades, our understanding of synaptic function has again been driven by physiological and molecular techniques. The key molecular players for synaptic vesicle structure, mobility and fusion were identified and applications of the patch clamp technique permitted physiological estimation of neurotransmitter release and receptor properties. These advances demand higher resolution structural images of synapses. During the 1990s a second renaissance in cell biology driven by EM was fueled by improved techniques for electron tomography (ET) with the ability to compute virtual images with nm resolution between image planes. Over the last 15 years, ET has been applied to the presynaptic terminal with special attention to the active zone and organelles of the nerve terminal. In this review, we first summarize the technical improvements that have led to a resurgence in utilization of ET and then we summarize new insights gained by the application of ET to reveal the high-resolution structure of the nerve terminal. PMID:25683026

  1. Weak localization and electron-electron interactions in indium-doped ZnO nanowires.

    PubMed

    Thompson, Richard S; Li, Dongdong; Witte, Christopher M; Lu, Jia G

    2009-12-01

    Single crystal ZnO nanowires doped with indium are synthesized via the laser-assisted chemical vapor deposition method. The conductivity of the nanowires is measured at low temperatures in magnetic fields with directions both perpendicular and parallel to the wire axes. A quantitative fit of our data is obtained, consistent with the theory of a quasi-one-dimensional metallic system with quantum corrections due to weak localization and electron-electron interactions. The anisotropy of the magneto-conductivity agrees with theory. The two quantum corrections are of approximately equal magnitude with respective temperature dependences of T(-1/3)and T(-1/2). The alternative model of quasi-two-dimensional surface conductivity is excluded by the absence of oscillations in the magneto-conductivity in parallel magnetic fields. PMID:19831413

  2. Synaptic Ribbons Require Ribeye for Electron Density, Proper Synaptic Localization, and Recruitment of Calcium Channels.

    PubMed

    Lv, Caixia; Stewart, William J; Akanyeti, Otar; Frederick, Courtney; Zhu, Jie; Santos-Sacchi, Joseph; Sheets, Lavinia; Liao, James C; Zenisek, David

    2016-06-21

    Synaptic ribbons are structures made largely of the protein Ribeye that hold synaptic vesicles near release sites in non-spiking cells in some sensory systems. Here, we introduce frameshift mutations in the two zebrafish genes encoding for Ribeye and thus remove Ribeye protein from neuromast hair cells. Despite Ribeye depletion, vesicles collect around ribbon-like structures that lack electron density, which we term "ghost ribbons." Ghost ribbons are smaller in size but possess a similar number of smaller vesicles and are poorly localized to synapses and calcium channels. These hair cells exhibit enhanced exocytosis, as measured by capacitance, and recordings from afferent neurons post-synaptic to hair cells show no significant difference in spike rates. Our results suggest that Ribeye makes up most of the synaptic ribbon density in neuromast hair cells and is necessary for proper localization of calcium channels and synaptic ribbons. PMID:27292637

  3. The structure of the hydrated electron in bulk and at interfaces: Does the hydrated electron occupy a cavity?

    NASA Astrophysics Data System (ADS)

    Casey, Jennifer Ryan

    Since its discovery over fifty years ago, the hydrated electron has been the subject of much interest. Hydrated electrons, which are free electrons in water, are found in fields ranging from biochemistry to radiation chemistry, so it is important that we understand the structure and dynamics of this species. Because of its high reactivity, the hydrated electron's structure has proven difficult to pin down, especially its molecular details. One-electron mixed quantum/classical molecular dynamics simulations have proven useful in helping elucidate the structure of the hydrated electron. The picture most commonly presented from these studies is one of the electron residing in a cavity, disrupting the local water structure much like an anion the size of bromide. Our group has recently proposed a completely different structure for the hydrated electron, which arose from rigorous calculations of a new electron-water potential. The picture that emerged was of an electron that does not occupy a cavity but instead draws water within itself; this non-cavity electron resides in a region of enhanced water density. The one-electron cavity and non-cavity models all predict similar experimental observables that probe the electronic structure of the hydrated electron, such as the optical absorption spectrum, which makes it difficult to determine which model most accurately describes the true structure of the hydrated electron. In this thesis, we work to calculate experimental observables for various simulated cavity and non-cavity models that are particularly sensitive to the local water structure near the electron, in an effort to distinguish the various models from each other. Two particular observables we are interested in are the resonance Raman spectrum and the temperature dependent optical absorption spectrum of the hydrated electron. We find that for both of these experiments, only the non-cavity model has qualitative agreement with experiment; the cavity models miss the

  4. Optical Evidence of Itinerant-Localized Crossover of 4f Electrons in Cerium Compounds

    NASA Astrophysics Data System (ADS)

    Kimura, Shin-ichi; Kwon, Yong Seung; Matsumoto, Yuji; Aoki, Haruyoshi; Sakai, Osamu

    2016-08-01

    Cerium (Ce)-based heavy-fermion materials have a characteristic double-peak structure (mid-IR peak) in the optical conductivity [σ(ω)] spectra originating from the strong conduction (c)-f electron hybridization. To clarify the behavior of the mid-IR peak at a low c-f hybridization strength, we compared the σ(ω) spectra of the isostructural antiferromagnetic and heavy-fermion Ce compounds with the calculated unoccupied density of states and the spectra obtained from the impurity Anderson model. With decreasing c-f hybridization intensity, the mid-IR peak shifts to the low-energy side owing to the renormalization of the unoccupied 4f state, but suddenly shifts to the high-energy side owing to the f-f on-site Coulomb interaction at a slight localized side from the quantum critical point (QCP). This finding gives us information on the change in the electronic structure across QCP.

  5. Spin Structure Functions from Electron Scattering

    SciTech Connect

    Seonho Choi

    2012-09-01

    The spin structure of the nucleon can play a key testing ground for Quantum Chromo-Dynamics (QCD) at wide kinematic ranges from smaller to large four momentum transfer Q{sup 2}. The pioneering experiments have confirmed several QCD sum rules at high Q{sup 2} where a perturbative picture holds. For a full understanding of QCD at various scales, various measurements were made at intermediate and small Q{sup 2} region and their interpretation would be a challenging task due to the non-perturbative nature. Jefferson Lab has been one of the major experimental facilities for the spin structure with its polarized electron beams and various polarized targets. A few QCD sum rules have been compared with the measured spin structure functions g{sub 1}(x, Q{sup 2}) and g{sub 2}(x, Q{sup 2}) at low Q{sup 2} and surprising results have been obtained for the spin polarizabilities, {gamma}{sub 0} and {delta}{sub LT} . As for the proton spin structure functions, the lack of data for g{sub 2}(x,Q{sup 2}) structure functions has been complemented with a new experiment at Jefferson Lab, SANE. The results from SANE will provide a better picture of the proton spin structure at a wide kinematic range in x and Q{sup 2}.

  6. Extraordinary electronic properties in uncommon structure types

    NASA Astrophysics Data System (ADS)

    Ali, Mazhar Nawaz

    In this thesis I present the results of explorations into several uncommon structure types. In Chapter 1 I go through the underlying idea of how we search for new compounds with exotic properties in solid state chemistry. The ideas of exploring uncommon structure types, building up from the simple to the complex, using chemical intuition and thinking by analogy are discussed. Also, the history and basic concepts of superconductivity, Dirac semimetals, and magnetoresistance are briefly reviewed. In chapter 2, the 1s-InTaS2 structural family is introduced along with the discovery of a new member of the family, Ag0:79VS2; the synthesis, structure, and physical properties of two different polymorphs of the material are detailed. Also in this chapter, we report the observation of superconductivity in another 1s structure, PbTaSe2. This material is especially interesting due to it being very heavy (resulting in very strong spin orbit coulping (SOC)), layered, and noncentrosymmetric. Electronic structure calculations reveal the presence of a bulk 3D Dirac cone (very similar to graphene) that is gapped by SOC originating from the hexagonal Pb layer. In Chapter 3 we show the re-investigation of the crystal structure of the 3D Dirac semimetal, Cd3As2. It is found to be centrosymmetric, rather than noncentrosymmetric, and as such all bands are spin degenerate and there is a 4-fold degenerate bulk Dirac point at the Fermi level, making Cd3As2 a 3D electronic analog to graphene. Also, for the first time, scanning tunneling microscopy experiments identify a 2x2 surface reconstruction in what we identify as the (112) cleavage plane of single crystals; needle crystals grow with a [110] long axis direction. Lastly, in chapter 4 we report the discovery of "titanic" (sadly dubbed ⪉rge, nonsaturating" by Nature editors and given the acronym XMR) magnetoresistance (MR) in the non-magnetic, noncentrosymmetric, layered transition metal dichalcogenide WTe2; over 13 million% at 0.53 K in

  7. Local Structural Alignment of RNA with Affine Gap Model

    NASA Astrophysics Data System (ADS)

    Wong, Thomas K. F.; Cheung, Brenda W. Y.; Lam, T. W.; Yiu, S. M.

    Predicting new non-coding RNAs (ncRNAs) of a family can be done by aligning the potential candidate with a member of the family with known sequence and secondary structure. Existing tools either only consider the sequence similarity or cannot handle local alignment with gaps. In this paper, we consider the problem of finding the optimal local structural alignment between a query RNA sequence (with known secondary structure) and a target sequence (with unknown secondary structure) with the affine gap penalty model. We provide the algorithm to solve the problem. Based on a preliminary experiment, we show that there are ncRNA families in which considering local structural alignment with gap penalty model can identify real hits more effectively than using global alignment or local alignment without gap penalty model.

  8. Real-time feedback from iterative electronic structure calculations.

    PubMed

    Vaucher, Alain C; Haag, Moritz P; Reiher, Markus

    2016-04-01

    Real-time feedback from iterative electronic structure calculations requires to mediate between the inherently unpredictable execution times of the iterative algorithm used and the necessity to provide data in fixed and short time intervals for real-time rendering. We introduce the concept of a mediator as a component able to deal with infrequent and unpredictable reference data to generate reliable feedback. In the context of real-time quantum chemistry, the mediator takes the form of a surrogate potential that has the same local shape as the first-principles potential and can be evaluated efficiently to deliver atomic forces as real-time feedback. The surrogate potential is updated continuously by electronic structure calculations and guarantees to provide a reliable response to the operator for any molecular structure. To demonstrate the application of iterative electronic structure methods in real-time reactivity exploration, we implement self-consistent semiempirical methods as the data source and apply the surrogate-potential mediator to deliver reliable real-time feedback. © 2015 Wiley Periodicals, Inc. PMID:26678030

  9. Analysis of the electronic structure of crystals through band structure unfolding

    NASA Astrophysics Data System (ADS)

    Gordienko, A. B.; Kosobutsky, A. V.

    2016-03-01

    In this work, we consider an alternative implementation of the band structure unfolding method within the framework of the density functional theory, which combines the advantages of the basis of localized functions and plane waves. This approach has been used to analyze the electronic structure of the ordered CuCl x Br1- x copper halide alloys and F 0 center in MgO that enables us to reveal qualitatively the features remaining hidden when using the standard supercell method, because of the complex band structure of systems with defects.

  10. Local atomic structure modulations activate metal oxide as electrocatalyst for hydrogen evolution in acidic water

    PubMed Central

    Li, Yu Hang; Liu, Peng Fei; Pan, Lin Feng; Wang, Hai Feng; Yang, Zhen Zhong; Zheng, Li Rong; Hu, P.; Zhao, Hui Jun; Gu, Lin; Yang, Hua Gui

    2015-01-01

    Modifications of local structure at atomic level could precisely and effectively tune the capacity of materials, enabling enhancement in the catalytic activity. Here we modulate the local atomic structure of a classical but inert transition metal oxide, tungsten trioxide, to be an efficient electrocatalyst for hydrogen evolution in acidic water, which has shown promise as an alternative to platinum. Structural analyses and theoretical calculations together indicate that the origin of the enhanced activity could be attributed to the tailored electronic structure by means of the local atomic structure modulations. We anticipate that suitable structure modulations might be applied on other transition metal oxides to meet the optimal thermodynamic and kinetic requirements, which may pave the way to unlock the potential of other promising candidates as cost-effective electrocatalysts for hydrogen evolution in industry. PMID:26286479

  11. Local atomic structure modulations activate metal oxide as electrocatalyst for hydrogen evolution in acidic water.

    PubMed

    Li, Yu Hang; Liu, Peng Fei; Pan, Lin Feng; Wang, Hai Feng; Yang, Zhen Zhong; Zheng, Li Rong; Hu, P; Zhao, Hui Jun; Gu, Lin; Yang, Hua Gui

    2015-01-01

    Modifications of local structure at atomic level could precisely and effectively tune the capacity of materials, enabling enhancement in the catalytic activity. Here we modulate the local atomic structure of a classical but inert transition metal oxide, tungsten trioxide, to be an efficient electrocatalyst for hydrogen evolution in acidic water, which has shown promise as an alternative to platinum. Structural analyses and theoretical calculations together indicate that the origin of the enhanced activity could be attributed to the tailored electronic structure by means of the local atomic structure modulations. We anticipate that suitable structure modulations might be applied on other transition metal oxides to meet the optimal thermodynamic and kinetic requirements, which may pave the way to unlock the potential of other promising candidates as cost-effective electrocatalysts for hydrogen evolution in industry. PMID:26286479

  12. Pu electronic structure and photoelectron spectroscopy

    SciTech Connect

    Joyce, John J; Durakiewicz, Tomasz; Graham, Kevin S; Bauer, Eric D; Moore, David P; Mitchell, Jeremy N; Kennison, John A; Martin, Richard L; Roy, Lindsay E; Scuseria, G. E.

    2010-01-01

    The electronic structure of PuCoGa{sub 5}, Pu metal, and PuO{sub 2} is explored using photoelectron spectroscopy. Ground state electronic properties are inferred from temperature dependent photoemission near the Fermi energy for Pu metal. Angle-resolved photoemission details the energy vs. crystaJ momentum landscape near the Fermi energy for PuCoGa{sub 5} which shows significant dispersion in the quasiparticle peak near the Fermi energy. For the Mott insulators AnO{sub 2}(An = U, Pu) the photoemission results are compared against hybrid functional calculations and the model prediction of a cross over from ionic to covalent bonding is found to be reasonable.

  13. Global-local finite element analysis of composite structures

    SciTech Connect

    Deibler, J.E.

    1992-06-01

    The development of layered finite elements has facilitated analysis of laminated composite structures. However, the analysis of a structure containing both isotropic and composite materials remains a difficult problem. A methodology has been developed to conduct a ``global-local`` finite element analysis. A ``global`` analysis of the entire structure is conducted at the appropriate loads with the composite portions replaced with an orthotropic material of equivalent materials properties. A ``local`` layered composite analysis is then conducted on the region of interest. The displacement results from the ``global`` analysis are used as loads to the ``local`` analysis. the laminate stresses and strains can then be examined and failure criteria evaluated.

  14. Global-local finite element analysis of composite structures

    SciTech Connect

    Deibler, J.E.

    1992-06-01

    The development of layered finite elements has facilitated analysis of laminated composite structures. However, the analysis of a structure containing both isotropic and composite materials remains a difficult problem. A methodology has been developed to conduct a global-local'' finite element analysis. A global'' analysis of the entire structure is conducted at the appropriate loads with the composite portions replaced with an orthotropic material of equivalent materials properties. A local'' layered composite analysis is then conducted on the region of interest. The displacement results from the global'' analysis are used as loads to the local'' analysis. the laminate stresses and strains can then be examined and failure criteria evaluated.

  15. Local gravity and large-scale structure

    NASA Technical Reports Server (NTRS)

    Juszkiewicz, Roman; Vittorio, Nicola; Wyse, Rosemary F. G.

    1990-01-01

    The magnitude and direction of the observed dipole anisotropy of the galaxy distribution can in principle constrain the amount of large-scale power present in the spectrum of primordial density fluctuations. This paper confronts the data, provided by a recent redshift survey of galaxies detected by the IRAS satellite, with the predictions of two cosmological models with very different levels of large-scale power: the biased Cold Dark Matter dominated model (CDM) and a baryon-dominated model (BDM) with isocurvature initial conditions. Model predictions are investigated for the Local Group peculiar velocity, v(R), induced by mass inhomogeneities distributed out to a given radius, R, for R less than about 10,000 km/s. Several convergence measures for v(R) are developed, which can become powerful cosmological tests when deep enough samples become available. For the present data sets, the CDM and BDM predictions are indistinguishable at the 2 sigma level and both are consistent with observations. A promising discriminant between cosmological models is the misalignment angle between v(R) and the apex of the dipole anisotropy of the microwave background.

  16. Electronic Structure of Buried Interfaces - Oral Presentation

    SciTech Connect

    Porter, Zachary

    2015-08-25

    In the electronics behind computer memory storage, the speed and size are dictated by the performance of permanent magnets inside devices called read heads. Complicated magnets made of stacked layers of thin films can be engineered to have properties that yield more energy storage and faster switching times compared to conventional iron or cobalt magnets. The reason is that magnetism is a result of subtle interactions amongst electrons; just how neurons come together on large scales to make cat brains and dog brains, ensembles of electrons interact and become ferromagnets and paramagnets. These interactions make magnets too difficult to study in their entirety, so I focus on the interfaces between layers, which are responsible for the coupling materials physicists hope to exploit to produce next-generation magnets. This project, I study a transition metal oxide material called LSCO, Lanthanum Cobaltite, which can be a paramagnet or a ferromagnet depending on how you tweak the electronic structure. It exhibits an exciting behavior: its sum is greater than the sum of its parts. When another similar material called a LSMO, Lanthanum Manganite, is grown on top of it, their interface has a different type of magnetism from the LSCO or the LSMO! I hope to explain this by demonstrating differently charged ions in the interface. The typical method for quantifying this is x-ray absorption, but all conventional techniques look at every layer simultaneously, averaging the interfaces and the LSCO layers that we want to characterize separately. Instead, I must use a new reflectivity technique, which tracks the intensity of reflected x-rays at different angles, at energies near the absorption peaks of certain elements, to track changes in the electronic structure of the material. The samples were grown by collaborators at the Takamura group at U.C. Davis and probed with this “resonant reflectivity” technique on Beamline 2-1 at the Stanford Synchrotron Radiation Lightsource

  17. 8th international conference on electronic spectroscopy and structure

    SciTech Connect

    Robinson, Art

    2000-10-16

    Gathering from 33 countries around the world, 408 registrants and a number of local drop-in participants descended on the Clark Kerr Campus of the University of California, Berkeley, from Monday, August 7 through Saturday, August 12, 2000 for the Eighth International Conference on Electronic Structure and Spectroscopy (ICESS8). At the conference, participants benefited from an extensive scientific program comprising more than 100 oral presentations (plenary lectures and invited and contributed talks) and 330 poster presentations, as well as ample time for socializing and a tour of the Advanced Light Source (ALS) at the nearby Lawrence Berkeley National Laboratory.

  18. Effects of Paramagnetism and Electron Correlations on the Electronic Structure of MnO: Ab Initio Study

    NASA Astrophysics Data System (ADS)

    Yoon, Sangmoon; Jin, Kyoungsuk; Kang, Seoung-Hun; Nam, Ki Tae; Kim, Miyoung; Kwon, Young-Kyun

    Manganese oxide nanoparticles have attracted a lot of attentions as a promising candidate for next-generation catalyst. Therefore, understanding the electronic structure of manganese oxide in room temperature is highly required for the rational design of catalysts. We study the effects of paramagnetism and electron correlations on the electronic structure of MnO using ab initio density functional theory. Spin configurations of paramagnetism are postulated as the ensemble average of various spin disorders. Each initial disordered spin configuration is randomly generated with two constraints on magnetic local moments. We first investigate the influence of magnetic ordering on the elctronic structure of MnO using noncollinear spin calculations and find that the magnetic disorders make valence band maximum more delocalized. Moreover, we examine the role of electron correlations in the electronic structure of paramagnetic MnO using DFT +U calculations. Strong electron correlations modify not only the size of band gap but also the magnitude of local moments as in the antiferromagnetic MnO. Besides, the initialized spin disorder remains almost unchanged as electron correlation get stronger. Furthermore, our results obtained by considering both strong electron correlation and paramagnetism confirm experimentally-observed oxygen K edge X-ray emission spectra [1] reflecting the feature of valence bands. [1] E. Z. Kurmaev et al., Phys. Rev. B. 77, 165127 (2008).

  19. Femtosecond X-ray absorption study of electron localization in photoexcited anatase TiO2

    NASA Astrophysics Data System (ADS)

    Santomauro, F. G.; Lübcke, A.; Rittmann, J.; Baldini, E.; Ferrer, A.; Silatani, M.; Zimmermann, P.; Grübel, S.; Johnson, J. A.; Mariager, S. O.; Beaud, P.; Grolimund, D.; Borca, C.; Ingold, G.; Johnson, S. L.; Chergui, M.

    2015-10-01

    Transition metal oxides are among the most promising solar materials, whose properties rely on the generation, transport and trapping of charge carriers (electrons and holes). Identifying the latter’s dynamics at room temperature requires tools that combine elemental and structural sensitivity, with the atomic scale resolution of time (femtoseconds, fs). Here, we use fs Ti K-edge X-ray absorption spectroscopy (XAS) upon 3.49 eV (355 nm) excitation of aqueous colloidal anatase titanium dioxide nanoparticles to probe the trapping dynamics of photogenerated electrons. We find that their localization at Titanium atoms occurs in <300 fs, forming Ti3+ centres, in or near the unit cell where the electron is created. We conclude that electron localization is due to its trapping at pentacoordinated sites, mostly present in the surface shell region. The present demonstration of fs hard X-ray absorption capabilities opens the way to a detailed description of the charge carrier dynamics in transition metal oxides.

  20. Femtosecond X-ray absorption study of electron localization in photoexcited anatase TiO2.

    PubMed

    Santomauro, F G; Lübcke, A; Rittmann, J; Baldini, E; Ferrer, A; Silatani, M; Zimmermann, P; Grübel, S; Johnson, J A; Mariager, S O; Beaud, P; Grolimund, D; Borca, C; Ingold, G; Johnson, S L; Chergui, M

    2015-01-01

    Transition metal oxides are among the most promising solar materials, whose properties rely on the generation, transport and trapping of charge carriers (electrons and holes). Identifying the latter's dynamics at room temperature requires tools that combine elemental and structural sensitivity, with the atomic scale resolution of time (femtoseconds, fs). Here, we use fs Ti K-edge X-ray absorption spectroscopy (XAS) upon 3.49 eV (355 nm) excitation of aqueous colloidal anatase titanium dioxide nanoparticles to probe the trapping dynamics of photogenerated electrons. We find that their localization at Titanium atoms occurs in <300 fs, forming Ti(3+) centres, in or near the unit cell where the electron is created. We conclude that electron localization is due to its trapping at pentacoordinated sites, mostly present in the surface shell region. The present demonstration of fs hard X-ray absorption capabilities opens the way to a detailed description of the charge carrier dynamics in transition metal oxides. PMID:26437873

  1. Femtosecond X-ray absorption study of electron localization in photoexcited anatase TiO2

    PubMed Central

    Santomauro, F. G.; Lübcke, A.; Rittmann, J.; Baldini, E.; Ferrer, A.; Silatani, M.; Zimmermann, P.; Grübel, S.; Johnson, J. A.; Mariager, S. O.; Beaud, P.; Grolimund, D.; Borca, C.; Ingold, G.; Johnson, S.L.; Chergui, M.

    2015-01-01

    Transition metal oxides are among the most promising solar materials, whose properties rely on the generation, transport and trapping of charge carriers (electrons and holes). Identifying the latter’s dynamics at room temperature requires tools that combine elemental and structural sensitivity, with the atomic scale resolution of time (femtoseconds, fs). Here, we use fs Ti K-edge X-ray absorption spectroscopy (XAS) upon 3.49 eV (355 nm) excitation of aqueous colloidal anatase titanium dioxide nanoparticles to probe the trapping dynamics of photogenerated electrons. We find that their localization at Titanium atoms occurs in <300 fs, forming Ti3+ centres, in or near the unit cell where the electron is created. We conclude that electron localization is due to its trapping at pentacoordinated sites, mostly present in the surface shell region. The present demonstration of fs hard X-ray absorption capabilities opens the way to a detailed description of the charge carrier dynamics in transition metal oxides. PMID:26437873

  2. Electronic and magnetic structures of chain structured iron selenide compounds

    NASA Astrophysics Data System (ADS)

    Li, Wei; Setty, Chandan; Chen, X. H.; Hu, Jiangping

    2014-08-01

    Electronic and magnetic structures of iron selenide compounds Ce2O2FeSe2 (2212*) and BaFe2Se3 (123*) are studied by the first-principles calculations. We find that while all these compounds are composed of one-dimensional (1D) Fe chain (or ladder) structures, their electronic structures are not close to be quasi-1D. The magnetic exchange couplings between two nearest-neighbor (NN) chains in 2212* and between two NN two-leg-ladders in 123* are both antiferromagnetic (AFM), which is consistent with the presence of significant third NN AFM coupling, a common feature shared in other iron-chalcogenides, FeTe (11*) and K y Fe2- x Se2 (122*). In magnetic ground states, each Fe chain of 2212* is ferromagnetic and each two-leg ladder of 123* form a block-AFM structure. We suggest that all magnetic structures in iron-selenide compounds can be unified into an extended J 1- J 2- J 3 model. Spin-wave excitations of the model are calculated and can be tested by future experiments on these two systems.

  3. Electronic structure and optical properties of resin

    NASA Astrophysics Data System (ADS)

    Rao, Zhi-Fan; Zhou, Rong-Feng

    2013-03-01

    We used the density of functional theory (DFT) to study the electronic structure and density of states of resin by ab initio calculation. The results show the band gap of resin is 1.7 eV. The covalent bond is combined C/O atoms with H atoms. The O 2p orbital is the biggest effect near the Fermi level. The results of optical properties show the reflectivity is low, and the refractive index is 1.7 in visible light range. The highest absorption coefficient peak is in 490 nm and the value is 75,000.

  4. Lattice Boltzmann Model for Electronic Structure Simulations

    NASA Astrophysics Data System (ADS)

    Mendoza, M.; Herrmann, H. J.; Succi, S.

    2015-09-01

    Recently, a new connection between density functional theory and kinetic theory has been proposed. In particular, it was shown that the Kohn-Sham (KS) equations can be reformulated as a macroscopic limit of the steady-state solution of a suitable single-particle kinetic equation. By using a discrete version of this new formalism, the exchange and correlation energies of simple atoms and the geometrical configuration of the methane molecule were calculated accurately. Here, we discuss the main ideas behind the lattice kinetic approach to electronic structure computations, offer some considerations for prospective extensions, and also show additional numerical results, namely the geometrical configuration of the water molecule.

  5. Surface structure and electronic properties of materials

    NASA Technical Reports Server (NTRS)

    Siekhaus, W. J.; Somorjai, G. A.

    1975-01-01

    A surface potential model is developed to explain dopant effects on chemical vapor deposition. Auger analysis of the interaction between allotropic forms of carbon and silicon films has shown Si-C formation for all forms by glassy carbon. LEED intensity measurements have been used to determine the mean square displacement of surface atoms of silicon single crystals, and electron loss spectroscopy has shown the effect of structure and impurities on surface states located within the band gap. A thin film of Al has been used to enhance film crystallinity at low temperature.

  6. Electronic Document Imaging and Optical Storage Systems for Local Governments: An Introduction. Local Government Records Technical Information Series. Number 21.

    ERIC Educational Resources Information Center

    Schwartz, Stanley F.

    This publication introduces electronic document imaging systems and provides guidance for local governments in New York in deciding whether such systems should be adopted for their own records and information management purposes. It advises local governments on how to develop plans for using such technology by discussing its advantages and…

  7. Local structure analyzers as determinants of preattentive pattern discrimination.

    PubMed

    Kröse, B J

    1987-01-01

    Contemporary literature suggests that preattentive texture or pattern discrimination is induced by differences between local structure features or "textons." This paper presents a model for the description of such local structure features based on the computation of local autocorrelations within the image. By means of this structure model a measure of structure dissimilarity is introduced. Experiments have been carried out to test a hypothesized relation between the detectability of a target pattern in a field of background patterns and the value of the structure dissimilarity measure. The experimental results show that it seems justified to relate, in a quantitative way, the detectability of the target pattern to the value of the structure dissimilarity measure. PMID:3828403

  8. Glass formation and local topological instability of atomic structure

    SciTech Connect

    Egami, T.

    1997-12-31

    A direct connection between the local topology of the atomic structure of liquids and glasses and thermodynamic quantities through the atomic level stresses is suggested for metallic alloys. In particular the role of local topological instability in the phase transformation involving liquid and glass will be discussed. It is pointed out that a single local geometrical criterion can explain various phase transformations, such as melting, glass transition, and glass formation by solid state reaction and liquid quenching.

  9. Improving Boundary Conditions for Electronic Structure Calculations

    NASA Astrophysics Data System (ADS)

    Benesh, G. A.; Haydock, Roger

    Boundary conditions imposed on a local system joined to a much larger substrate system routinely introduce unphysical reflections that affect the calculation of electronic properties such as energies, charge densities, and densities of states. These problems persist in atomic cluster, slab, and supercell calculations alike. However, wave functions in real, physical systems do not reflect at artificial boundaries. Instead, they carry current smoothly across the surface separating the local system from the underlying medium. Haydock and Nex have derived a non-reflecting boundary condition that works well for discrete systems [Phys. Rev. B 75, 205121 (2006)]. Solutions satisfying their maximal breaking of time-reversal symmetry (MBTS) boundary condition carry current away from the boundary at a maximal rate--in much the same way as exact wave functions in physical systems. The MBTS approach has now been extended to studies employing continuous basis functions. In model systems, MBTS boundary conditions work well for calculating wave functions, eigenenergies, and densities of states. Results are reported for an Al(001) surface. Comparisons are made with slab calculations, embedding calculations, and experiment.

  10. Quantum mirages formed by coherent projection of electronic structure

    PubMed

    Manoharan; Lutz; Eigler

    2000-02-01

    Image projection relies on classical wave mechanics and the use of natural or engineered structures such as lenses or resonant cavities. Well-known examples include the bending of light to create mirages in the atmosphere, and the focusing of sound by whispering galleries. However, the observation of analogous phenomena in condensed matter systems is a more recent development, facilitated by advances in nanofabrication. Here we report the projection of the electronic structure surrounding a magnetic Co atom to a remote location on the surface of a Cu crystal; electron partial waves scattered from the real Co atom are coherently refocused to form a spectral image or 'quantum mirage'. The focusing device is an elliptical quantum corral, assembled on the Cu surface. The corral acts as a quantum mechanical resonator, while the two-dimensional Cu surface-state electrons form the projection medium. When placed on the surface, Co atoms display a distinctive spectroscopic signature, known as the many-particle Kondo resonance, which arises from their magnetic moment. By positioning a Co atom at one focus of the ellipse, we detect a strong Kondo signature not only at the atom, but also at the empty focus. This behaviour contrasts with the usual spatially-decreasing response of an electron gas to a localized perturbation. PMID:10676952

  11. Local Influence Analysis of Nonlinear Structural Equation Models

    ERIC Educational Resources Information Center

    Lee, Sik-Yum; Tang, Nian-Sheng

    2004-01-01

    By regarding the latent random vectors as hypothetical missing data and based on the conditional expectation of the complete-data log-likelihood function in the EM algorithm, we investigate assessment of local influence of various perturbation schemes in a nonlinear structural equation model. The basic building blocks of local influence analysis…

  12. Electronic structure effects in liquid water studied by photoelectron spectroscopy and density functional theory

    SciTech Connect

    Nordlund, Dennis; Odelius, Michael; Bluhm, Hendrik; Ogasawara, Hirohito; Pettersson, Lars G.M.; Nilsson, Anders

    2008-04-29

    We present valence photoelectron emission spectra of liquid water in comparison with gas-phase water, ice close to the melting point, low temperature amorphous and crystalline ice. All aggregation states have major electronic structure changes relative to the free molecule, with rehybridization and development of bonding and anti-bonding states accompanying the hydrogen bond formation. Sensitivity to the local structural order, most prominent in the shape and splitting of the occupied 3a{sub 1} orbital, is understood from the electronic structure averaging over various geometrical structures, and reflects the local nature of the orbital interaction.

  13. The CECAM Electronic Structure Library: community-driven development of software libraries for electronic structure simulations

    NASA Astrophysics Data System (ADS)

    Oliveira, Micael

    The CECAM Electronic Structure Library (ESL) is a community-driven effort to segregate shared pieces of software as libraries that could be contributed and used by the community. Besides allowing to share the burden of developing and maintaining complex pieces of software, these can also become a target for re-coding by software engineers as hardware evolves, ensuring that electronic structure codes remain at the forefront of HPC trends. In a series of workshops hosted at the CECAM HQ in Lausanne, the tools and infrastructure for the project were prepared, and the first contributions were included and made available online (http://esl.cecam.org). In this talk I will present the different aspects and aims of the ESL and how these can be useful for the electronic structure community.

  14. Electron Beam Freeform Fabrication of Titanium Alloy Gradient Structures

    NASA Technical Reports Server (NTRS)

    Brice, Craig A.; Newman, John A.; Bird, Richard Keith; Shenoy, Ravi N.; Baughman, James M.; Gupta, Vipul K.

    2014-01-01

    Historically, the structural optimization of aerospace components has been done through geometric methods. A monolithic material is chosen based on the best compromise between the competing design limiting criteria. Then the structure is geometrically optimized to give the best overall performance using the single material chosen. Functionally graded materials offer the potential to further improve structural efficiency by allowing the material composition and/or microstructural features to spatially vary within a single structure. Thus, local properties could be tailored to the local design limiting criteria. Additive manufacturing techniques enable the fabrication of such graded materials and structures. This paper presents the results of a graded material study using two titanium alloys processed using electron beam freeform fabrication, an additive manufacturing process. The results show that the two alloys uniformly mix at various ratios and the resultant static tensile properties of the mixed alloys behave according to rule-of-mixtures. Additionally, the crack growth behavior across an abrupt change from one alloy to the other shows no discontinuity and the crack smoothly transitions from one crack growth regime into another.

  15. Fischer Tropsch synthesis : an in-situ TPR-EXAFS/XANES investigation of the influence of Group I alkali promoters on the local atomic and electronic structure of carburized iron/silica catalysts.

    SciTech Connect

    Ribeiro, M. C.; Jacobs, G.; Davis, B. H.; Cronauer, D. C.; Kropf, A. J.; Marshall, C. L.

    2010-01-01

    The promoting impact of alkali metals (i.e., Li, Na, K, Rb, Cs) on the carburization rate of Fe in Fe/Si catalysts was investigated by X-ray absorption spectroscopy. A multisample holder was used, allowing nearly simultaneous examination of the catalysts during activation in a CO/He mixture. With the white line intensity and shape as a fingerprint for oxidation state, TPR/XANES analysis enabled us to measure the relative composition of the different compounds as a function of the carburization time, temperature, and atomic number of the group 1 promoter. At the same time, TPR/EXAFS provided information on the changes in local atomic structure that accompanied the oxidation state changes. The rate of carburization increased in the following order: unpromoted < Li < Na < K = Rb = Cs. After 10 h of treatment the samples containing K, Rb, and Cs were completely carburized, and residual quantities of iron oxides were detected in both unpromoted and Li-promoted samples. The EXAFS spectra after carburization could be fitted well by considering a model containing Hagg carbide and Fe{sub 3}O{sub 4}. After 10 h of CO/He treatment at 290 C, the main component observed was Hagg carbide. A model containing Hagg and {var_epsilon}-carbides, and Fe{sub 3}O{sub 4}, was also investigated. However, the r-factor was not significantly impacted by including {var_epsilon}-carbide in the fitting, and the resulting contribution of {var_epsilon}-carbide in each catalyst from the model was virtually negligible. Selectivity differences are thus not likely due to changes in the carbide distribution. Rather, the alkali promoter increases the CO dissociative adsorption rate, resulting in an increase in the surface coverage of dissociated CO and an inhibition in the olefin readsorption rate. This in turn results in higher olefin selectivities, in agreement with previous catalytic tests.

  16. Analysis of boron carbides' electronic structure

    NASA Technical Reports Server (NTRS)

    Howard, Iris A.; Beckel, Charles L.

    1986-01-01

    The electronic properties of boron-rich icosahedral clusters were studied as a means of understanding the electronic structure of the icosahedral borides such as boron carbide. A lower bound was estimated on bipolaron formation energies in B12 and B11C icosahedra, and the associated distortions. While the magnitude of the distortion associated with bipolaron formation is similar in both cases, the calculated formation energies differ greatly, formation being much more favorable on B11C icosahedra. The stable positions of a divalent atom relative to an icosahedral borane was also investigated, with the result that a stable energy minimum was found when the atom is at the center of the borane, internal to the B12 cage. If incorporation of dopant atoms into B12 cages in icosahedral boride solids is feasible, novel materials might result. In addition, the normal modes of a B12H12 cluster, of the C2B10 cage in para-carborane, and of a B12 icosahedron of reduced (D sub 3d) symmetry, such as is found in the icosahedral borides, were calculated. The nature of these vibrational modes will be important in determining, for instance, the character of the electron-lattice coupling in the borides, and in analyzing the lattice contribution to the thermal conductivity.

  17. Electron beam coupling to a metamaterial structure

    SciTech Connect

    French, David M.; Shiffler, Don; Cartwright, Keith

    2013-08-15

    Microwave metamaterials have shown promise in numerous applications, ranging from strip lines and antennas to metamaterial-based electron beam driven devices. In general, metamaterials allow microwave designers to obtain electromagnetic characteristics not typically available in nature. High Power Microwave (HPM) sources have in the past drawn inspiration from work done in the conventional microwave source community. In this article, the use of metamaterials in an HPM application is considered by using an effective medium model to determine the coupling of an electron beam to a metamaterial structure in a geometry similar to that of a dielectric Cerenkov maser. Use of the effective medium model allows for the analysis of a wide range of parameter space, including the “mu-negative,”“epsilon-negative,” and “double negative” regimes of the metamaterial. The physics of such a system are modeled analytically and by utilizing the particle-in-cell code ICEPIC. For this geometry and effective medium representation, optimum coupling of the electron beam to the metamaterial, and thus the optimum microwave or RF production, occurs in the epsilon negative regime of the metamaterial. Given that HPM tubes have been proposed that utilize a metamaterial, this model provides a rapid method of characterizing a source geometry that can be used to quickly understand the basic physics of such an HPM device.

  18. Experimental Benchmarking of Pu Electronic Structure

    SciTech Connect

    Tobin, J G; Moore, K T; Chung, B W; Wall, M A; Schwartz, A J; Ebbinghaus, B B; Butterfield, M T; Teslich, Jr., N E; Bliss, R A; Morton, S A; Yu, S W; Komesu, T; Waddill, G D; der Laan, G v; Kutepov, A L

    2005-10-13

    The standard method to determine the band structure of a condensed phase material is to (1) obtain a single crystal with a well defined surface and (2) map the bands with angle resolved photoelectron spectroscopy (occupied or valence bands) and inverse photoelectron spectroscopy (unoccupied or conduction bands). Unfortunately, in the case of Pu, the single crystals of Pu are either nonexistent, very small and/or having poorly defined surfaces. Furthermore, effects such as electron correlation and a large spin-orbit splitting in the 5f states have further complicated the situation. Thus, we have embarked upon the utilization of unorthodox electron spectroscopies, to circumvent the problems caused by the absence of large single crystals of Pu with well-defined surfaces. Our approach includes the techniques of resonant photoelectron spectroscopy [1], x-ray absorption spectroscopy [1,2,3,4], electron energy loss spectroscopy [2,3,4], Fano Effect measurements [5], and Bremstrahlung Isochromat Spectroscopy [6], including the utilization of micro-focused beams to probe single-crystallite regions of polycrystalline Pu samples. [2,3,6

  19. Electronically induced structure transformations in graphite & silver, studied using ultrafast electron crystallography

    NASA Astrophysics Data System (ADS)

    Raman, Ramani K.

    photoexcited graphite surface. It is shown that such photoemission plays a minor role in the refraction shifts observed in the UEC study and a sub-surface dipole field is sufficient to explain the structural and charge relaxations observed. Investigations utilizing scanning electron microscope imaging of structures generated from laser ablation of graphite reveals the creation of geometrically faceted crystalline features, whose Raman spectrum exhibit sp3 like characteristics, though unambiguous identification of diamond structures generated requires further study. In the case of silver nanocrystals (Ag NC), photoexcitation near the surface plasmon resonance (SPR) is observed to lead to fragmentation at fluences below their melting threshold. By isolating each NC from other neighboring NCs in a surface supported geometry, the normally irreversible process becomes reversible and amenable to multi-shot pump-probe diffraction investigations just below the fragmentation threshold. Transient structural, thermal and Coulombic signatures of the pre-fragmented state are extracted from the UEC investigation and combined with a progressive Reverse Monte-Carlo structure refinement scheme to visualize the atomic dynamics leading up to the fragmentation. Such multi-faceted analysis reveals the fragmentation to proceed through the creation and growth of undercoordinated defect sites along which the lattice is weakened. These defects are likely seeded by the strong coupling between SPR dephasing pathways and inter-band transitions that can lead to bond-softening effects and local valence instabilities. The creation of sufficient number of such defect sites at elevated fluences are believed to lead to the eventual fragmentation of the entire NC. This thesis also details the design and principle of UEC systems employed in a surface probing geometry for the study of nanostructures and interfaces.

  20. Localized vibrations: moles in structure-land

    NASA Astrophysics Data System (ADS)

    van der Maas, John H.

    1992-03-01

    Functional groups reveal specific information about their direct surroundings; in fact, they form the moles, the undercover agents, in molecules. However, as with agents, the information is produced in coded form (spectral data) so one has to know the code in detail before the message is completely understood. The substantially improved accuracy (wavenumber, intensity) and sensitivity brought about by FT-instruments, in combination with computer software, offer extended spectral information. Functional groups can now be examined in great detail. Obviously the amount of deducible structural items is group dependent, implying that one has to pursue the probing qualities of a functionality prior to use. The OH-group, and more in particular the OH-stretching vibration, proves to be an extremely good mole. Its potentials are demonstrated on conformational studies of various saturated alcohols, the presence of OH(DOT)(DOT)(DOT)(pi) bridges, the strength and type of OH(DOT)(DOT)(DOT)O bridges, all in an apolar solvent, and on the disclosure of different hydrogen bonds in some solid samples.

  1. Photonic crystal structures for efficent localization or extraction of light

    NASA Astrophysics Data System (ADS)

    Vuckovic, Jelena

    Three-dimensional (3D) photonic crystals offer the opportunity of light manipulation in all directions in space, but they are very difficult to fabricate. On the other hand, planar photonic crystals are much simpler to make, but they exhibit only a "quasi-3D" confinement, resulting from the combined action of 2D photonic crystal and internal reflection. The imperfect confinement in the third dimension produces some unwanted out-of-plane loss, which is usually a limiting factor in performance of these structures. This thesis proposes how to fully take advantage of the relatively simple fabrication of planar photonic crystals, by addressing a problem of loss-reduction. One of the greatest challenges in photonics is a construction of optical microcavities with small mode volumes and large quality factors, for efficient localization of light. Beside standard applications of these structures (such as lasers or filters), they can potentially be used for cavity QED experiments, or as building blocks for quantum networks. This work also presents the design and fabrication of optical microcavities based on planar photonic crystals, with mode volumes of the order of one half of cubic wavelength of light (measured in material) and with Q factors predicted to be even larger than 10 4. In addition to photonic crystals fabricated in semiconductors, we also address interesting properties of metallic photonic crystals and present our theoretical and experimental work on using them to improve the output of light emissive devices. Feature sizes of structures presented here are below those achievable by photolithography. Therefore, a high resolution lithography is necessary for their fabrication. The presently used e-beam writing techniques suffer from limitations in speed and wafer throughput, and they represent a huge obstacle to commercialization of photonic crystals. Our preliminary work on electron beam projection lithography, the technique that could provide us with the speed

  2. Proteins comparison through probabilistic optimal structure local alignment

    PubMed Central

    Micale, Giovanni; Pulvirenti, Alfredo; Giugno, Rosalba; Ferro, Alfredo

    2014-01-01

    Multiple local structure comparison helps to identify common structural motifs or conserved binding sites in 3D structures in distantly related proteins. Since there is no best way to compare structures and evaluate the alignment, a wide variety of techniques and different similarity scoring schemes have been proposed. Existing algorithms usually compute the best superposition of two structures or attempt to solve it as an optimization problem in a simpler setting (e.g., considering contact maps or distance matrices). Here, we present PROPOSAL (PROteins comparison through Probabilistic Optimal Structure local ALignment), a stochastic algorithm based on iterative sampling for multiple local alignment of protein structures. Our method can efficiently find conserved motifs across a set of protein structures. Only the distances between all pairs of residues in the structures are computed. To show the accuracy and the effectiveness of PROPOSAL we tested it on a few families of protein structures. We also compared PROPOSAL with two state-of-the-art tools for pairwise local alignment on a dataset of manually annotated motifs. PROPOSAL is available as a Java 2D standalone application or a command line program at http://ferrolab.dmi.unict.it/proposal/proposal.html. PMID:25228906

  3. Electronic structure of rare-earth hexaborides

    NASA Astrophysics Data System (ADS)

    Kimura, S.; Nanba, T.; Tomikawa, M.; Kunii, S.; Kasuya, T.

    1992-11-01

    Reflectivity spectra of all rare-earth hexaboride RB6 (R=La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Yb, and Y) single crystals have been measured systematically in the energy region from 1 meV to 40 eV at 300 K in order to investigate the electronic state and the contribution of the 4f electron to the band structure. The analysis of the optical conductivity and the loss-function spectra, which were derived from the Kramers-Kronig transformation of the reflectivity spectra, allowed us to make clear the origin of the peak structure in the spectrum due to the various interband transitions. The origins of the main peaks in the spectrum were assigned to the interband transitions from the bonding to the antibonding bands of the boron 2s and 2p states and to the rare-earth 5d state. The intra-atomic transition from the 4f and the 5p to the 5d(t2g) states in the rare-earth ion was also observed.

  4. Structure and navigation for electronic publishing

    NASA Astrophysics Data System (ADS)

    Tillinghast, John; Beretta, Giordano B.

    1998-01-01

    The sudden explosion of the World Wide Web as a new publication medium has given a dramatic boost to the electronic publishing industry, which previously was a limited market centered around CD-ROMs and on-line databases. While the phenomenon has parallels to the advent of the tabloid press in the middle of last century, the electronic nature of the medium brings with it the typical characteristic of 4th wave media, namely the acceleration in its propagation speed and the volume of information. Consequently, e-publications are even flatter than print media; Shakespeare's Romeo and Juliet share the same computer screen with a home-made plagiarized copy of Deep Throat. The most touted tool for locating useful information on the World Wide Web is the search engine. However, due to the medium's flatness, sought information is drowned in a sea of useless information. A better solution is to build tools that allow authors to structure information so that it can easily be navigated. We experimented with the use of ontologies as a tool to formulate structures for information about a specific topic, so that related concepts are placed in adjacent locations and can easily be navigated using simple and ergonomic user models. We describe our effort in building a World Wide Web based photo album that is shared among a small network of people.

  5. Electronic Structure Studies of Silicon Carbide Anionic Nanoclusters

    NASA Astrophysics Data System (ADS)

    Pradhan, Prachi

    2005-03-01

    As a continuation of our studies on the high stabilities and electronic structure properties of Si8C2 to Si14C2 clusters and Si60Cn (n=3-6) clusters,^1 we report here ab initio studies of small SimCn^- (1< m, n < 4) anionic clusters. The theoretical formalism used is the local density approximation (LDA) to density functional theory (DFT) and the Gaussian03 suite of programs^2 with an all electron 6-311++G** basis set has been used. Complete geometry optimizations of different possible structures have been carried out. Carbon-rich and silicon rich species show distinctly different patterns with respect to the vertical detachment energies. For carbon-rich aggregates, the VDE's show an even odd alternation, similar to that of the carbon anions. We present results on binding energies, relative energies, fragmentation energies, vertical detachment energies, vibrational frequencies, and adiabatic electron affinities^3 for the optimized clusters. Detailed comparisons with published data in the literature will also be presented. * Work supported, in part, by the Welch Foundation, Houston, Texas (Grant No. Y-1525). ^1M. N. Huda and A. K. Ray, Phys. Rev. A (R) 69, 011201 (2004); Eur. Phys. J. D 31, 63 (2004). ^2 Gaussian03, Revision A.1, M. J. Frisch et al., Gaussian Inc., Pittsburgh, PA , 2003. ^3 P. Pradhan and A. K. Ray, J. Mol. Structure (Theochem), in press.

  6. Electronic Structure and Bonding in Complex Biomolecule

    NASA Astrophysics Data System (ADS)

    Ouyang, Lizhi

    2005-03-01

    For over a century vitamin B12 and its enzyme cofactor derivates have persistently attracted research efforts for their vital biological role, unique Co-C bonding, rich red-ox chemistry, and recently their candidacies as drug delivery vehicles etc. However, our understanding of this complex metalorganic molecule's efficient enzyme activated catalytic power is still controversial. We have for the first time calculated the electronic structure, Mulliken effective charge and bonding of a whole Vitamin B12 molecule without any structural simplification by first- principles approaches based on density functional theory using structures determined by high resolution X-ray diffraction. A partial density of states analysis shows excellent agreement with X-ray absorption data and has been used successfully to interpret measured optical absorption spectra. Mulliken bonding analysis of B12 and its derivatives reveal noticeable correlations between the two axial ligands which could be exploited by the enzyme to control the catalytic process. Our calculated X-ray near edge structure of B12 and its derivates using Slater's transition state theory are also in good agreement with experiments. The same approach has been applied to other B12 derivatives, ferrocene peptides, and recently DNA molecules.

  7. Multigrid Methods in Electronic Structure Calculations

    NASA Astrophysics Data System (ADS)

    Briggs, Emil

    1996-03-01

    Multigrid techniques have become the method of choice for a broad range of computational problems. Their use in electronic structure calculations introduces a new set of issues when compared to traditional plane wave approaches. We have developed a set of techniques that address these issues and permit multigrid algorithms to be applied to the electronic structure problem in an efficient manner. In our approach the Kohn-Sham equations are discretized on a real-space mesh using a compact representation of the Hamiltonian. The resulting equations are solved directly on the mesh using multigrid iterations. This produces rapid convergence rates even for ill-conditioned systems with large length and/or energy scales. The method has been applied to both periodic and non-periodic systems containing over 400 atoms and the results are in very good agreement with both theory and experiment. Example applications include a vacancy in diamond, an isolated C60 molecule, and a 64-atom cell of GaN with the Ga d-electrons in valence which required a 250 Ry cutoff. A particular strength of a real-space multigrid approach is its ready adaptability to massively parallel computer architectures. The compact representation of the Hamiltonian is especially well suited to such machines. Tests on the Cray-T3D have shown nearly linear scaling of the execution time up to the maximum number of processors (512). The MPP implementation has been used for studies of a large Amyloid Beta Peptide (C_146O_45N_42H_210) found in the brains of Alzheimers disease patients. Further applications of the multigrid method will also be described. (in collaboration D. J. Sullivan and J. Bernholc)

  8. Protein tertiary structure recognition using optimized Hamiltonians with local interactions.

    PubMed Central

    Goldstein, R A; Luthey-Schulten, Z A; Wolynes, P G

    1992-01-01

    Protein folding codes embodying local interactions including surface and secondary structure propensities and residue-residue contacts are optimized for a set of training proteins by using spin-glass theory. A screening method based on these codes correctly matches the structure of a set of test proteins with proteins of similar topology with 100% accuracy, even with limited sequence similarity between the test proteins and the structural homologs and the absence of any structurally similar proteins in the training set. PMID:1409599

  9. Electronic structure of benzene adsorbed on Ni and Cu surfaces

    SciTech Connect

    Weinelt, M.; Nilsson, A.; Wassdahl, N.

    1997-04-01

    Benzene has for a long time served as a prototype adsorption system of large molecules. It adsorbs with the molecular plane parallel to the surface. The bonding of benzene to a transition metal is typically viewed to involve the {pi} system. Benzene adsorbs weakly on Cu and strongly on Ni. It is interesting to study how the adsorption strength is reflected in the electronic structure of the adsorbate-substrate complex. The authors have used X-ray Emission (XE) and X-ray Absorption (XA) spectroscopies to selectively study the electronic states localized on the adsorbed benzene molecule. Using XES the occupied states can be studies and with XAS the unoccupied states. The authors have used beamline 8.0 and the Swedish endstation equipped with a grazing incidence x-ray spectrometer and a partial yield absorption detector. The resolution in the XES and XAS were 0.5 eV and 0.05 eV, respectively.

  10. Electronic structure of Ca, Sr, and Ba under pressure.

    NASA Technical Reports Server (NTRS)

    Animalu, A. O. E.; Heine, V.; Vasvari, B.

    1967-01-01

    Electronic band structure calculations phase of Ca, Sr and Ba over wide range of atomic volumes under pressure electronic band structure calculations for fcc phase of Ca, Sr and Ba over wide range of atomic volumes under pressure electronic band structure calculations for fcc phase of Ca, Sr and Ba over wide range of atomic volumes under pressure

  11. Reversible Hydrogen Storage Materials – Structure, Chemistry, and Electronic Structure

    SciTech Connect

    Robertson, Ian M.; Johnson, Duane D.

    2014-06-21

    To understand the processes involved in the uptake and release of hydrogen from candidate light-weight metal hydride storage systems, a combination of materials characterization techniques and first principle calculation methods have been employed. In addition to conventional microstructural characterization in the transmission electron microscope, which provides projected information about the through thickness microstructure, electron tomography methods were employed to determine the three-dimensional spatial distribution of catalyst species for select systems both before and after dehydrogenation. Catalyst species identification as well as compositional analysis of the storage material before and after hydrogen charging and discharging was performed using a combination of energy dispersive spectroscopy, EDS, and electron energy loss spectroscopy, EELS. The characterization effort was coupled with first-principles, electronic-structure and thermodynamic techniques to predict and assess meta-stable and stable phases, reaction pathways, and thermodynamic and kinetic barriers. Systems studied included:NaAlH4, CaH2/CaB6 and Ca(BH4)2, MgH2/MgB2, Ni-Catalyzed Magnesium Hydride, TiH2-Catalyzed Magnesium Hydride, LiBH4, Aluminum-based systems and Aluminum

  12. Electronic structure and ionicity of actinide oxides from first principles

    NASA Astrophysics Data System (ADS)

    Petit, L.; Svane, A.; Szotek, Z.; Temmerman, W. M.; Stocks, G. M.

    2010-01-01

    The ground-state electronic structures of the actinide oxides AO , A2O3 , and AO2 ( A=U , Np, Pu, Am, Cm, Bk, and Cf) are determined from first-principles calculations, using the self-interaction corrected local spin-density approximation. Emphasis is put on the degree of f -electron localization, which for AO2 and A2O3 is found to follow the stoichiometry, namely, corresponding to A4+ ions in the dioxide and A3+ ions in the sesquioxides. In contrast, the A2+ ionic configuration is not favorable in the monoxides, which therefore become metallic. The energetics of the oxidation and reduction in the actinide dioxides is discussed, and it is found that the dioxide is the most stable oxide for the actinides from Np onward. Our study reveals a strong link between preferred oxidation number and degree of localization which is confirmed by comparing to the ground-state configurations of the corresponding lanthanide oxides. The ionic nature of the actinide oxides emerges from the fact that only those compounds will form where the calculated ground-state valency agrees with the nominal valency expected from a simple charge counting.

  13. Electronic structure of disordered Fe-V alloys

    SciTech Connect

    Krause, J.C.; Paduani, C.; Schaff, J.; da Costa, M.I. , Jr.

    1998-01-01

    The first-principles discrete variational method is employed to investigate the electronic structure and local magnetic properties of disordered Fe-V alloys. The spin-polarized case is considered in the formalism of the local-spin-density approximation, with the exchange-correlation term of von Barth{endash}Hedin. The effect on the local magnetic properties of adding V atoms in the immediate neighborhood of iron atoms is investigated. The partial density of states, hyperfine field (H{sub c}), magnetic moment ({mu}), and isomer shift are obtained for the central atom of the cluster. For the impurity V atom in the bcc iron host the calculated values for H{sub c} and {mu} are {minus}203 kG and {minus}0.86{mu}{sub B}, respectively. The isolated Fe atom in a bcc vanadium host exhibits a collapsed moment and acts as a receptor for electrons. In ordered alloys the calculations indicate also a vanishing moment at iron sites. {copyright} {ital 1998} {ital The American Physical Society}

  14. Negative local resistance due to viscous electron backflow in graphene

    NASA Astrophysics Data System (ADS)

    Bandurin, Denis

    Theoretical and experimental studies of systems in which particles undergo frequent mutual collisions date back to more than two centuries ago. Transport in such systems is described by hydrodynamic theory that was found very successful in explaining the response of classical liquids and gases to external fields. It has been argued for a long time that collective behavior of charge carriers in solids can be also described by hydrodynamic approach. However, there has been almost no direct evidence to hydrodynamic electron transport so far. This is because the conditions at which the hydrodynamic effects become observable are very strict: the electron-electron scattering length should provide the shortest spatial scale in the problem. First of all, this requires ultra clean systems where the scattering at impurities is diminished. Second, the electron-phonon scattering rate should be smaller than that of electron-electron scattering. Due to weak electron-phonon coupling high mobility graphene devices offer an ideal system to study electron hydrodynamics. To amplify the hydrodynamic effects we employed a special measurement geometry. The idea is that in case of hydrodynamic electron flow, vortices emerge in the spatial electric current distribution near the current injection contact. That results in a development of a negative voltage drop at the nearby contacts. We were able to detect such negative signal over the range of temperatures when the electronic system is in a hydrodynamic regime. Finally, we performed a rheological study of electron liquid in graphene. The electron viscosity was found to be an order of magnitude larger than that of honey which is in good agreement with many-body calculation.

  15. Electronic structure and bonding in transuranics: comparison with lanthanides

    SciTech Connect

    Ward, J.W.

    1983-01-01

    The physico-chemical properties of the actinide metals, alloys, and compounds show interesting parallels and contrasts with the rare earths, beyond uranium. At first there is a transition region where the unique bonding properties of the early actinides become less prominent, due to progressive f-electron localization. Nevertheless, in contrast to the rare earths, f-electron energies remain close to the Fermi level, resulting in complex behavior as a function of temperature, pressure and structure. Particularly interesting in this region are the metallic hydrides, whose chemistry is clearly rare-earth like, but whose electronic properties are entirely different. At americium a major localization and f-band narrowing occurs, but the explanation of americium behavior is obscured by the occurrence of the unique f/sup 6/ non-magnetic solid-state configuration. Beyond americium, it would appear that real rare-earth-like behavior finally begins; this has been born out by recent studies on the thermodynamics and cohesive energies of curium, berkelium, californium and einsteinium metals. However, a new complication arises almost immediately, in the onset of incipient stabilization of the divalent state, which already appears in californium, whose physico-chemical properties are remarkably similar to samarium. Einsteinium appears to be fully divalent, thus heralding the beginning of a mini-series of truly divalent metals.

  16. The electronic structure of a liquid Pb film

    NASA Astrophysics Data System (ADS)

    Osterwalder, Jürg

    2007-03-01

    Our understanding of the electronic structure of condensed matter in the liquid phase is far from complete. We used angle-resolved photoemission spectroscopy (ARPES) in order to study the evolution of the electronic bands, the Fermi surface and the spectral function of a lead monolayer on Cu(111) as the film went through its melting transition at 568 K [1]. The crystalline copper substrate provides the reciprocal lattice vectors, absent in the liquid state, that are needed in ARPES for wave-number conservation in the excitation process, and the well-resolved copper bands serve as an important reference frame for identifying the dramatic changes in the lead states. Electron spectra and momentum distribution maps of the liquid film reveal three important features: the persistence of a Fermi surface, the filling of band gaps, and the localization of the wave functions upon melting. Distinct coherence lengths for different sheets of the Fermi surface are found, indicating a strong dependence of the localization lengths on the character of the constituent atomic wave functions. [1] F. Baumberger, W. Auw"arter, T. Greber, J. Osterwalder, Science 306, 2221 (2004).

  17. Probing local order in glasses from limited-volume electron and x-ray diffraction

    NASA Astrophysics Data System (ADS)

    Liu, A. C. Y.; Tabor, R. F.; Bourgeois, L.; de Jonge, M. D.; Mudie, S. T.; Petersen, T. C.

    2016-05-01

    It has long been recognised that spatial fluctuations in local order in disordered assemblies of particles can be probed using limited-volume diffraction measurements. These measurements have unique advantages over broad-beam diffraction experiments that isotropically average over many structural configurations and result in one-dimensional intensity curves, requiring modelling to interpret. Despite the advantages of limiting illumination to a low number of particle configurations, obtaining quantitative measurements of local order from such experiments remains a challenge. The effects on the diffraction pattern of changing the beam energy, lateral size, aberrations and coherence and the specimen thickness have only recently been clarified. We review theoretical and experimental efforts in this direction in the fields of both electron and x-ray diffraction and identify promising areas of future development.

  18. Structural evolution and valence electron-state change during ultra thin silicon-oxide growth

    NASA Astrophysics Data System (ADS)

    Shimizu, A.; Abe, S.; Nakayama, H.; Nishino, T.; Iida, S.

    2000-06-01

    We have studied valence electron-state changes of Si during initial oxidation of Si(111) clean surface, HF-treated Si(001) and Si(111) surfaces by Auger valence electron spectroscopy (AVES). The results showed that the valence electron-state changes during initial oxidation were sensitively reflected in Si[2s,2p,V] (V=3s,3p) AVES spectra and that they depended on both initial surface treatment and surface orientation. The local valence electron-states, local density of states in other words, showed the characteristic-structure evolution depending on the initial surface treatment and surface orientation.

  19. Core-hole effect on XANES and electronic structure of minor actinide dioxides with fluorite structure

    NASA Astrophysics Data System (ADS)

    Suzuki, Chikashi; Nishi, Tsuyoshi; Nakada, Masami; Akabori, Mitsuo; Hirata, Masaru; Kaji, Yoshiyuki

    2012-02-01

    The authors investigated theoretically core-hole effects on X-ray absorption near-edge structures (XANES) of Np and Am LIII in neptunium dioxide (NpO2) and americium dioxide (AmO2) with CaF2-type crystal lattices using the all-electron full-potential linearized augmented plane-wave (FP-LAPW) method. The peak creation mechanism of XANES was shown by examining the electronic structures of these oxides, which indicated that core-hole screening was more marked for AmO2 than for NpO2 because of the difference in the charge transfer between these oxides. Furthermore, the results of charge density analysis suggested that the white line was assigned to the quasi-bound state composed of the localized Np d or Am d components and O components, and that the tail structure was created as a result of delocalized standing waves between the Np or Am atoms.

  20. Electronic stopping power calculation method for molecular dynamics simulations using local Firsov and free electron-gas models

    NASA Astrophysics Data System (ADS)

    Peltola, J.; Nordlund, K.; Keinonen, J.

    2006-09-01

    Molecular dynamics simulations have proven to be accurate in predicting depth distributions of low-energy ions implanted in materials. Free parameters adjusted for every ion-target combination are conventionally used to obtain depth profiles in accordance with the experimental ones. We have previously developed a model for predicting depth profiles in crystalline Si without free parameters. The electronic stopping power was calculated using local total electron density. The model underestimated the stopping in the < 1 1 0 > channeling direction. We have now taken a new approach to calculate the electronic stopping power. We use the local valence (3p(2)) electron density to account for the electronic energy loss between collisions and the Firsov model to account for the electronic energy loss during collision. The lowest electron densities are adjusted with a parametrization that is same for all ions in all implanting directions to correct the problems in the < 1 1 0 > channeling direction.

  1. Nature and localization of avian lens glycogen by electron microscopy and Raman spectroscopy.

    PubMed Central

    Castillo, C G; Lo, W K; Kuck, J F; Yu, N T

    1992-01-01

    Electron microscopy confirms the presence of a high concentration of glycogen particles in the lens nuclear region of birds of flying habit such as the ring-neck dove and pigeon. This observation is consistent with Raman spectroscopy. The glycogen particles in the dove lens, which are approximately 35 nm in diameter, are classified as beta type particles. Although this type has been previously characterized by high rates of glycogen turnover in other tissues, its localization in the lens nucleus indicates that it may serve a structural function rather than as a storage depot of carbohydrate in the lens. In a comparative electron microscopy study, glycogen particles were not observed in the chicken lens. Images FIGURE 3 FIGURE 4 FIGURE 5 PMID:1581498

  2. Energetics and electronic structure of UAl4 with point defects

    NASA Astrophysics Data System (ADS)

    Kniznik, L.; Alonso, P. R.; Gargano, P. H.; Rubiolo, G. H.

    2015-11-01

    UAl4 ideal and defect structures were studied within the framework of the Density Functional Theory. The structural and magnetic ordering of UAl4 in paramagnetic, ferromagnetic, and antiferromagnetic states have been investigated, within the collinear and non-collinear spin approximation, using the GGA model, as embedded in the program package VASP. An antiferromagnetic (0 1 bar 1) layer structure with spins aligned to the [010] direction was found to be energetically preferred. The analysis of density of states and bonding charge density point out that the bonding mechanism consists primarily of band mixing between the U 5f and Al 3p states. Supercells were built from UAl4 unit cells with the established magnetic structure. For those supercells we calculated the energy of formation of vacancies and antisite defects taking into account the existence of three distinct aluminum sites. Point defect formation energies, local lattice relaxations, as well as the defect induced magnetic ordering and electronic density redistribution, are discussed. It is shown that antiferromagnetism is locally broken. Al antisites and U antisites in Al 4e Wyckoff positions are the constitutional point defects in Al-rich and U-rich oI20 UAl4, respectively. In this way we have presented here the first set of data which makes it possible to discuss and quantify the point defects concentrations in the experimental composition range for existence of this uranium aluminide.

  3. Local imaging of high mobility two-dimensional electron systems with virtual scanning tunneling microscopy

    SciTech Connect

    Pelliccione, M.; Bartel, J.; Goldhaber-Gordon, D.; Sciambi, A.; Pfeiffer, L. N.; West, K. W.

    2014-11-03

    Correlated electron states in high mobility two-dimensional electron systems (2DESs), including charge density waves and microemulsion phases intermediate between a Fermi liquid and Wigner crystal, are predicted to exhibit complex local charge order. Existing experimental studies, however, have mainly probed these systems at micron to millimeter scales rather than directly mapping spatial organization. Scanning probes should be well-suited to study the spatial structure of these states, but high mobility 2DESs are found at buried semiconductor interfaces, beyond the reach of conventional scanning tunneling microscopy. Scanning techniques based on electrostatic coupling to the 2DES deliver important insights, but generally with resolution limited by the depth of the 2DES. In this letter, we present our progress in developing a technique called “virtual scanning tunneling microscopy” that allows local tunneling into a high mobility 2DES. Using a specially designed bilayer GaAs/AlGaAs heterostructure where the tunnel coupling between two separate 2DESs is tunable via electrostatic gating, combined with a scanning gate, we show that the local tunneling can be controlled with sub-250 nm resolution.

  4. Local imaging of high mobility two-dimensional electron systems with virtual scanning tunneling microscopy

    NASA Astrophysics Data System (ADS)

    Pelliccione, M.; Bartel, J.; Sciambi, A.; Pfeiffer, L. N.; West, K. W.; Goldhaber-Gordon, D.

    2014-11-01

    Correlated electron states in high mobility two-dimensional electron systems (2DESs), including charge density waves and microemulsion phases intermediate between a Fermi liquid and Wigner crystal, are predicted to exhibit complex local charge order. Existing experimental studies, however, have mainly probed these systems at micron to millimeter scales rather than directly mapping spatial organization. Scanning probes should be well-suited to study the spatial structure of these states, but high mobility 2DESs are found at buried semiconductor interfaces, beyond the reach of conventional scanning tunneling microscopy. Scanning techniques based on electrostatic coupling to the 2DES deliver important insights, but generally with resolution limited by the depth of the 2DES. In this letter, we present our progress in developing a technique called "virtual scanning tunneling microscopy" that allows local tunneling into a high mobility 2DES. Using a specially designed bilayer GaAs/AlGaAs heterostructure where the tunnel coupling between two separate 2DESs is tunable via electrostatic gating, combined with a scanning gate, we show that the local tunneling can be controlled with sub-250 nm resolution.

  5. Structure of local interactions in complex financial dynamics

    PubMed Central

    Jiang, X. F.; Chen, T. T.; Zheng, B.

    2014-01-01

    With the network methods and random matrix theory, we investigate the interaction structure of communities in financial markets. In particular, based on the random matrix decomposition, we clarify that the local interactions between the business sectors (subsectors) are mainly contained in the sector mode. In the sector mode, the average correlation inside the sectors is positive, while that between the sectors is negative. Further, we explore the time evolution of the interaction structure of the business sectors, and observe that the local interaction structure changes dramatically during a financial bubble or crisis. PMID:24936906

  6. Structure of local interactions in complex financial dynamics

    NASA Astrophysics Data System (ADS)

    Jiang, X. F.; Chen, T. T.; Zheng, B.

    2014-06-01

    With the network methods and random matrix theory, we investigate the interaction structure of communities in financial markets. In particular, based on the random matrix decomposition, we clarify that the local interactions between the business sectors (subsectors) are mainly contained in the sector mode. In the sector mode, the average correlation inside the sectors is positive, while that between the sectors is negative. Further, we explore the time evolution of the interaction structure of the business sectors, and observe that the local interaction structure changes dramatically during a financial bubble or crisis.

  7. Electronic structures of reconstructed zigzag silicene nanoribbons

    SciTech Connect

    Ding, Yi E-mail: wangyanli-04@tsinghua.org.cn; Wang, Yanli E-mail: wangyanli-04@tsinghua.org.cn

    2014-02-24

    Edge states and magnetism are crucial for spintronic applications of nanoribbons. Here, using first-principles calculations, we explore structural stabilities and electronic properties of zigzag silicene nanoribbons (ZSiNRs) with Klein and pentagon-heptagon reconstructions. Comparing to unreconstructed zigzag edges, deformed bare pentagon-heptagon ones are favored under H-poor conditions, while H-rich surroundings stabilize di-hydrogenated Klein edges. These Klein edges have analogous magnetism to zigzag ones, which also possess the electric-field-induced half-metallicity of nanoribbons. Moreover, diverse magnetic states can be achieved by asymmetric Klein and zigzag edges into ZSiNRs, which could be transformed from antiferromagnetic-semiconductors to bipolar spin-gapless-semiconductors and ferromagnetic-metals depending on edge hydrogenations.

  8. Electronic Structure Calculations of Highly Charged Ions

    NASA Astrophysics Data System (ADS)

    Bromley, Steve; Ziolkowski, Marcin; Marler, Joan

    2016-05-01

    Exotic systems like Highly Charged Ions (HCIs) are attracting more attention based on their properties and possible interactions. Abundance of HCIs in the solar wind and their interaction with the upper atmosphere puts them in the attention of astro- and atmospheric physicists. Also, their unique properties originating in the high charge make them an excellent candidate for precision measurements and the next generation of atomic clocks. For a better understanding of the dynamics of processes involving HCIs a combined theoretical and experimental effort is needed to study their basic properties and interactions. Both theory and experiment need to be combined due to the extreme nature of these systems. We present preliminary insight into electronic structure of light HCIs, their interactions with neutral atoms and dynamics of charge transfer processes.

  9. Electron Liquids in Semiconductor Quantum Structures

    SciTech Connect

    Aron Pinczuk

    2009-05-25

    The groups led by Stormer and Pinczuk have focused this project on goals that seek the elucidation of novel many-particle effects that emerge in two-dimensional electron systems (2DES) as the result from fundamental quantum interactions. This experimental research is conducted under extreme conditions of temperature and magnetic field. From the materials point of view, the ultra-high mobility systems in GaAs/AlGaAs quantum structures continue to be at the forefront of this research. The newcomer materials are based on graphene, a single atomic layer of graphite. The graphene research is attracting enormous attention from many communities involved in condensed matter research. The investigated many-particle phenomena include the integer and fractional quantum Hall effect, composite fermions, and Dirac fermions, and a diverse group of electron solid and liquid crystal phases. The Stormer group performed magneto-transport experiments and far-infrared spectroscopy, while the Pinczuk group explores manifestations of such phases in optical spectra.

  10. Local electron spectrum above 100 MeV derived from gamma-ray emissivity spectra

    NASA Technical Reports Server (NTRS)

    Strong, A. W.

    1985-01-01

    Two new determinations of the local gamma-ray emmissivity spectrum are in good accord and were used to derive constraints on the local electron spectrum. The requirement for an electron intensity above 1 GeV larger than previously believed is confirmed and no low energy upturn is then needed.

  11. Reconstruction of biofilm images: combining local and global structural parameters.

    PubMed

    Resat, Haluk; Renslow, Ryan S; Beyenal, Haluk

    2014-10-01

    Digitized images can be used for quantitative comparison of biofilms grown under different conditions. Using biofilm image reconstruction, it was previously found that biofilms with a completely different look can have nearly identical structural parameters and that the most commonly utilized global structural parameters were not sufficient to uniquely define these biofilms. Here, additional local and global parameters are introduced to show that these parameters considerably increase the reliability of the image reconstruction process. Assessment using human evaluators indicated that the correct identification rate of the reconstructed images increased from 50% to 72% with the introduction of the new parameters into the reconstruction procedure. An expanded set of parameters especially improved the identification of biofilm structures with internal orientational features and of structures in which colony sizes and spatial locations varied. Hence, the newly introduced structural parameter sets helped to better classify the biofilms by incorporating finer local structural details into the reconstruction process. PMID:25377487

  12. Reconstruction of biofilm images: combining local and global structural parameters

    SciTech Connect

    Resat, Haluk; Renslow, Ryan S.; Beyenal, Haluk

    2014-11-07

    Digitized images can be used for quantitative comparison of biofilms grown under different conditions. Using biofilm image reconstruction, it was previously found that biofilms with a completely different look can have nearly identical structural parameters and that the most commonly utilized global structural parameters were not sufficient to uniquely define these biofilms. Here, additional local and global parameters are introduced to show that these parameters considerably increase the reliability of the image reconstruction process. Assessment using human evaluators indicated that the correct identification rate of the reconstructed images increased from 50% to 72% with the introduction of the new parameters into the reconstruction procedure. An expanded set of parameters especially improved the identification of biofilm structures with internal orientational features and of structures in which colony sizes and spatial locations varied. Hence, the newly introduced structural parameter sets helped to better classify the biofilms by incorporating finer local structural details into the reconstruction process.

  13. Global/local methods for probabilistic structural analysis

    NASA Technical Reports Server (NTRS)

    Millwater, H. R.; Wu, Y.-T.

    1993-01-01

    A probabilistic global/local method is proposed to reduce the computational requirements of probabilistic structural analysis. A coarser global model is used for most of the computations with a local more refined model used only at key probabilistic conditions. The global model is used to establish the cumulative distribution function (cdf) and the Most Probable Point (MPP). The local model then uses the predicted MPP to adjust the cdf value. The global/local method is used within the advanced mean value probabilistic algorithm. The local model can be more refined with respect to the g1obal model in terms of finer mesh, smaller time step, tighter tolerances, etc. and can be used with linear or nonlinear models. The basis for this approach is described in terms of the correlation between the global and local models which can be estimated from the global and local MPPs. A numerical example is presented using the NESSUS probabilistic structural analysis program with the finite element method used for the structural modeling. The results clearly indicate a significant computer savings with minimal loss in accuracy.

  14. Structure and Electronic Properties of Cerium Orthophosphate: Theory and Experiment

    SciTech Connect

    Adelstein, Nicole; Mun, B. Simon; Ray, Hannah; Ross Jr, Phillip; Neaton, Jeffrey; De Jonghe, Lutgard

    2010-07-27

    Structural and electronic properties of cerium orthophosphate (CePO{sub 4}) are calculated using density functional theory (DFT) with the local spin-density approximation (LSDA+U), with and without gradient corrections (GGA-(PBE)+U), and compared to X-ray diffraction and photoemission spectroscopy measurements. The density of states is found to change significantly as the Hubbard parameter U, which is applied to the Ce 4f states, is varied from 0 to 5 eV. The calculated structural properties are in good agreement with experiment and do not change significantly with U. Choosing U = 3 eV for LDSA provides the best agreement between the calculated density of states and the experimental photoemission spectra.

  15. Electronic properties of acenes: Oligomer to polymer structure

    NASA Astrophysics Data System (ADS)

    Dos Santos, M. C.

    2006-07-01

    The conformations and electronic structures of long oligoacenes [ C2H2(C4H2)n , 20⩽n⩽23 ] and polyacene [(C8H4)x] were theoretically investigated through density functional theory adopting the hybrid B3LYP/6-31G(d) functional. The long oligoacenes present a cis conformation and solitonlike distortions along the chain. The defective regions having uniform bond lengths produce localized states on the top of the oligomer valence band. The spontaneous creation of bond alternation defects leads to high-spin magnetic ground states. The nonmagnetic state of polyacene presents a Peierls-distorted trans conformation which is lower in energy by a few meV per unit cell from the symmetric (nonalternating) state. The lowest-energy structure is predicted to present a cis pattern of bonds with alternation defects and a triplet state per unit cell.

  16. Atomic and electronic structure of twin growth defects in magnetite

    PubMed Central

    Gilks, Daniel; Nedelkoski, Zlatko; Lari, Leonardo; Kuerbanjiang, Balati; Matsuzaki, Kosuke; Susaki, Tomofumi; Kepaptsoglou, Demie; Ramasse, Quentin; Evans, Richard; McKenna, Keith; Lazarov, Vlado K.

    2016-01-01

    We report the existence of a stable twin defect in Fe3O4 thin films. By using aberration corrected scanning transmission electron microscopy and spectroscopy the atomic structure of the twin boundary has been determined. The boundary is confined to the (111) growth plane and it is non-stoichiometric due to a missing Fe octahedral plane. By first principles calculations we show that the local atomic structural configuration of the twin boundary does not change the nature of the superexchange interactions between the two Fe sublattices across the twin grain boundary. Besides decreasing the half-metallic band gap at the boundary the altered atomic stacking at the boundary does not change the overall ferromagnetic (FM) coupling between the grains. PMID:26876049

  17. Exchange coupling in transition metal monoxides: Electronic structure calculations

    SciTech Connect

    Fischer, Guntram; Daene, Markus W; Ernst, Arthur; Bruno, Patrick; Lueders, Martin; Szotek, Zdzislawa; Temmerman, Walter M; Wolfam, Hergert

    2009-01-01

    An ab initio study of magnetic-exchange interactions in antiferromagnetic and strongly correlated 3d transition metal monoxides is presented. Their electronic structure is calculated using the local self-interaction correction approach, implemented within the Korringa-Kohn-Rostoker band-structure method, which is based on multiple scattering theory. The Heisenberg exchange constants are evaluated with the magnetic force theorem. Based on these the corresponding Neel temperatures TN and spin-wave dispersions are calculated. The Neel temperatures are obtained using mean-field approximation, random-phase approximation and Monte Carlo simulations. The pressure dependence of TN is investigated using exchange constants calculated for different lattice constants. All the calculated results are compared to experimental data.

  18. Crossover from low-temperature itinerant to high-temperature localized electron behavior in the electron-doped rare-earth metal cobaltate perovskites

    NASA Astrophysics Data System (ADS)

    Ramos, S. L. L. M.; Oguni, M.; Masuda, Y.; Inada, Y.

    2011-02-01

    We present a study on the temperature dependence of the electronic structure and magnetic properties of CexEu1-xCoO3 by means of x-ray absorption spectroscopy (XAS) and magnetic susceptibility measurements. Contrary to what was previously reported in literature for this compound, we identified the partially substituted Ce species to be tetravalent within the whole temperature range investigated, i.e., 300 ⩾ T/K ⩾ 40. It is shown that, as a result, corresponding amounts of Co2+ are formed at room temperature, indicating an electron-doping effect. At T = 40 K, however, even though electron doping could be identified through Co XAS pre-edge features, the Co2+ species were not identifiable. These results indicate a change in the Co-related electronic structure with temperature, and we interpret this as indicative of a crossover from a low-temperature itinerant-electron state to a high-temperature localized-electron state. The magnetic susceptibility revealed the onset of low-temperature itinerant ferromagnetism for the higher Ce-doping concentrations, while the room-temperature effective magnetic moment μeff value for the lowest Ce-concentrated sample was in complete agreement with the theoretical one for Co2+, thus being consistent with the itinerant-localized-electron crossover scenario as depicted from the XAS results.

  19. 5f-electron localization in the actinide metals: thorides, actinides and the Mott transition

    NASA Astrophysics Data System (ADS)

    Lawson, A. C.

    2016-03-01

    For the light actinides Ac-Cm, the numbers of localized and itinerant 5f-electrons are determined by comparing various estimates of the f-electron counts. At least one itinerant f-electron is found for each element, Pa-Cm. These results resolve certain disagreements among electron counts determined by different methods and are consistent with the Mott transition model and with the picture of the 5f-electrons' dual nature.

  20. Local structure and superconductivity of the Ce1-xLaxRu2 Laves phase system

    NASA Astrophysics Data System (ADS)

    Saini, N. L.; Agrestini, S.; Amato, E.; Filippi, M.; di Castro, D.; Bianconi, A.; Manfrinetti, P.; Palenzona, A.; Marcelli, A.

    2004-09-01

    We have studied local structure of the Laves phase Ce1-xLaxRu2 superconductor by Ru K-edge extended x-ray absorption fine-structure measurements focusing on the small La concentration regime where the transition temperature Tc passes through a local maximum. We find that correlated Debye-Waller factor of the Ru-Ru bonds follows Tc with the varying La concentration in the system. Although, this remarkable Tc correlation on the local atomic structure suggests important role of the electron-lattice interactions, the band-structure effects seem more likely the reason to drive the anomalous superconducting behavior and the Tc maximum in this 4f system.

  1. Metallic carbon nanotubes with metal contacts: electronic structure and transport

    NASA Astrophysics Data System (ADS)

    Zienert, A.; Schuster, J.; Gessner, T.

    2014-10-01

    We study quasi-ballistic electron transport in metallic (6,0) carbon nanotubes (CNTs) of variable length in contact with Al, Cu, Pd, Pt, Ag, and Au electrodes by using the non-equilibrium Green's function formalism in combination with either density functional theory or self-consistent extended Hückel theory. We find good agreement between both. Visualizing the local device density of states of the systems gives a descriptive link between electronic structure and transport properties. In comparison with bare finite and infinite tubes, we show that the electronic structure of short metallic CNTs is strongly modified by the presence of the metallic electrodes, which leads to pronounced size effects in the conductance. The mean conductances and linear response currents allow a ranking of the metals regarding their ability to form low-Ohmic contacts with the nanotube: Ag≲ Au\\lt Cu\\ll Pt≈ Pd\\ll Al. These findings are contrasted with similar trends in contact distance, binding energy, calculated work function of the metal surfaces, and various results from literature.

  2. Structural phase transition and electronic properties in samarium chalcogenides

    NASA Astrophysics Data System (ADS)

    Panwar, Y. S.; Aynyas, Mahendra; Pataiya, J.; Sanyal, Sankar P.

    2016-05-01

    The electronic structure and high pressure properties of samarium monochalcogenides SmS, SmSe and SmTe have been reported by using tight binding linear muffin-tin-orbital (TB-LMTO) method within the local density approximation (LDA). The total energy as a function of volume is evaluated. It is found that these monochalcogenides are stable in NaCl-type structure under ambient pressure. We predict a structural phase transition from NaCl-type (B1-phase) structure to CsCl-type (B2-type) structure for these compounds. Phase transition pressures were found to be 1.7, 4.4 and 6.6 GPa, for SmS, SmSe and SmTe respectively. Apart from this, the lattice parameter (a0), bulk modulus (B0), band structure (BS) and density of states (DOS) are calculated. From energy band diagram we observed that these compounds exhibit metallic character. The calculated values of equilibrium lattice parameter and phase transition pressure are in general good agreement with available data.

  3. Characterizing Localized Surface Plasmons Using Electron Energy-Loss Spectroscopy

    NASA Astrophysics Data System (ADS)

    Cherqui, Charles; Thakkar, Niket; Li, Guoliang; Camden, Jon P.; Masiello, David J.

    2016-05-01

    Electron energy-loss spectroscopy (EELS) offers a window to view nanoscale properties and processes. When performed in a scanning transmission electron microscope, EELS can simultaneously render images of nanoscale objects with subnanometer spatial resolution and correlate them with spectroscopic information at a spectral resolution of ˜10-100 meV. Consequently, EELS is a near-perfect tool for understanding the optical and electronic properties of individual plasmonic metal nanoparticles and few-nanoparticle assemblies, which are significant in a wide range of fields. This review presents an overview of basic plasmonics and EELS theory and highlights several recent noteworthy experiments involving the interrogation of plasmonic metal nanoparticle systems using electron beams.

  4. Generation of superhot electrons by intense field structures

    SciTech Connect

    Salomaa, R. R. E.; Karttunen, S. J.; Paettikangas, T. J. H.; Mulser, P.; Schneider, W.

    1998-02-20

    Strong, localized electrostatic fields created in laser plasma interactions act as a source of hot electrons. We have derived analytical formulas based on adiabatic invariants for explaining of the main characteristics of the electron spectra found in test particle calculations and in full wave-particle simulations. The electrons are treated relativistically. Simple models for phenomenological description of nonlinear wave damping are discussed.

  5. Localization-delocalization transition of electrons at the percolation threshold of semiconductor GaAs1–xNx alloys: The appearance of a mobility edge

    DOE PAGESBeta

    Alberi, K.; Fluegel, B.; Beaton, D. A.; Ptak, A. J.; Mascarenhas, A.

    2012-07-09

    Electrons in semiconductor alloys have generally been described in terms of Bloch states that evolve from constructive interference of electron waves scattering from perfectly periodic potentials, despite the loss of structural periodicity that occurs on alloying. Using the semiconductor alloy GaAs₁₋xNx as a prototype, we demonstrate a localized to delocalized transition of the electronic states at a percolation threshold, the emergence of a mobility edge, and the onset of an abrupt perturbation to the host GaAs electronic structure, shedding light on the evolution of electronic structure in these abnormal alloys.

  6. Quantum pressure in molecules and solids: Influence of magnetic fields and spin-orbit coupling on electron localization

    NASA Astrophysics Data System (ADS)

    Tao, Jianmin; Liu, Shi; Zheng, Fan; Rappe, Andrew M.

    2015-03-01

    The most important concept in chemistry is chemical bond, which has been used by chemists to explain the properties of molecules and solids as well as chemical processes. Considerable efforts have been made toward a simple and yet fundamental understanding of this concept. Here we formulate the quantum pressure in an external magnetic field, allowing us to study the influence of magnetic fields and spin-orbit coupling on electron localization in molecules and solids. We find that electrons in conjugated molecules become more localized in strong magnetic fields, due to the induced currents. We demonstrate that the quantum pressure not only can reveal electronic shell structures of atoms, but also can be used to visualize bonding structures of molecules and solids, significantly extending the applicability of this descriptive tool. This work was supported by NSF, USAF, and DOE.

  7. Kinetics of vertical transport and localization of electrons in strained semiconductor supperlattices

    SciTech Connect

    Gerchikov, L. G. Mamaev, Yu. A.; Yashin, Yu. P.

    2015-08-15

    The kinetics of vertical electron transport in a semiconductor superlattice is considered taking into account partial localization of electrons. The time dependences of photoemission currents from samples based on a strained semiconductor superlattice calculated by numerically solving the kinetic equation are in good agreement with experimental data. Comparison of the theory with experiment makes it possible to determine the characteristic electron localization and thermoactivation times, the diffusion length, and losses of photoelectrons in the superlattice.

  8. Ab initio electronic structure study for TTF-TCNQ under uniaxial compression

    NASA Astrophysics Data System (ADS)

    Ishibashi, Shoji; Hashimoto, Tamotsu; Kohyama, Masanori; Terakura, Kiyoyuki

    2004-04-01

    We have investigated the electronic structure of TTF-TCNQ under uniaxial compression with ab initio plane-wave pseudopotential calculations within the local-density approximation and generalized gradient approximation. Depending on the compression direction, the constituent molecules are deformed in different ways. Along with these structural deformations, quasi-one-dimensional Fermi surfaces show dramatic changes in their shapes and sizes.

  9. Confidence-Guided Local Structure Prediction with HHfrag

    PubMed Central

    Kalev, Ivan; Habeck, Michael

    2013-01-01

    We present a method to assess the reliability of local structure prediction from sequence. We introduce a greedy algorithm for filtering and enrichment of dynamic fragment libraries, compiled with remote-homology detection methods such as HHfrag. After filtering false hits at each target position, we reduce the fragment library to a minimal set of representative fragments, which are guaranteed to have correct local structure in regions of detectable conservation. We demonstrate that the location of conserved motifs in a protein sequence can be predicted by examining the recurrence and structural homogeneity of detected fragments. The resulting confidence score correlates with the local RMSD of the representative fragments and allows us to predict torsion angles from sequence with better accuracy compared to existing machine learning methods. PMID:24146881

  10. Influences of consolidation processes on local paper structure

    NASA Astrophysics Data System (ADS)

    Sung, Yongjoo

    The accurate measurement of the structural parameters such as thickness, grammage, apparent density and surface topography, and the proper evaluation of the variation of each parameter, are very important not only for predicting the end use properties of the paper, but also for diagnosing the pa permaking processes. The difficulty of the measurement of thickness at fine scale ˜1 mm has been an impediment to the understanding of local paper structure. To address this problem, a twin laser profilometer instrument (TLP) for non-contacting measurement of local thickness and surface topography was developed, characterized and calibrated in this work. The fundamental relationships between structural parameters were reexamined with various handsheet samples. The effects of wet pressing on the local paper structure were evaluated using laboratory static press and commercial press felts. The different press pressure had no significant influence on the local density variation of the handsheet samples. The influences of felts on the surface topography were also successfully observed. The different densification effects of soft nip and hard nip calendering processes were evaluated by direct comparison of structural parameters before and after processing. The much higher selective reduction in local thickness (larger reduction for the thicker area) by the hard nip calendering process resulted in different relationships between structural parameters. The various periodic variations in the paper structure were also detected, analyzed and identified. The effects of different forming elements such as the conventional foil system and the velocity induced drainage (VID) system on the paper structure and end use properties were evaluated with pilot machine trials and commercial product produced using different forming elements. Generally, the VID samples showed better formation, less two sidedness in the fine distribution through thickness direction, and less densification during

  11. First principle investigation of structural and electronic properties of bulk ZnSe

    SciTech Connect

    Khatta, Swati; Tripathi, S. K. Prakash, Satya

    2015-08-28

    Electronic and structural properties of ZnSe are investigated using plane-wave self-consistent field method within the framework of density functional theory. The pseudopotential method within the local density approximation is used for the exchange-correlation potential. The equilibrium lattice parameter, static bulk modulus and its pressure derivative are calculated. The electronic band structure, partial density of states and density of states are also obtained. The results are compared with available theoretical calculations and experimental results.

  12. Investigation of crystal structure and associated electronic structure of Sr 6BP 5O 20

    NASA Astrophysics Data System (ADS)

    Ehrenberg, Helmut; Laubach, Sonja; Schmidt, P. C.; McSweeney, R.; Knapp, M.; Mishra, K. C.

    2006-04-01

    Strontium borophosphate phosphate (Sr 6BP 5O 20, SrBP), activated by divalent europium ions is a bluish-green phosphor emitting in a broad band with the emission peak near 480 nm. In this paper, we report the crystal structure of SrBP determined from an analysis of the X-ray diffraction pattern of a prismatic single crystal (size 60 μm×50 μm×40 μm). This crystal was chosen from undoped phosphor powder samples prepared for this purpose by solid-state reaction. SrBP is observed to crystallize in a body-centered tetragonal lattice with the lattice parameters a=9.7895(7) Å and c=19.032(3) Å, the associated space group being I4¯c2 (space group 120). Using the structural data from this study, we have also calculated its electronic structure using the augmented spherical wave method and the local density approximation (LDA). We show the ordering of the electronic states by the density of states (DOS) and the partial DOS plots. The LDA gives a direct optical band gap at the Γ point of about 5 eV. The significance of the crystal structure and associated electronic structure is discussed with respect to maintenance of this phosphor in Hg-discharge lamps.

  13. RESCU: A real space electronic structure method

    NASA Astrophysics Data System (ADS)

    Michaud-Rioux, Vincent; Zhang, Lei; Guo, Hong

    2016-02-01

    In this work we present RESCU, a powerful MATLAB-based Kohn-Sham density functional theory (KS-DFT) solver. We demonstrate that RESCU can compute the electronic structure properties of systems comprising many thousands of atoms using modest computer resources, e.g. 16 to 256 cores. Its computational efficiency is achieved from exploiting four routes. First, we use numerical atomic orbital (NAO) techniques to efficiently generate a good quality initial subspace which is crucially required by Chebyshev filtering methods. Second, we exploit the fact that only a subspace spanning the occupied Kohn-Sham states is required, and solving accurately the KS equation using eigensolvers can generally be avoided. Third, by judiciously analyzing and optimizing various parts of the procedure in RESCU, we delay the O (N3) scaling to large N, and our tests show that RESCU scales consistently as O (N2.3) from a few hundred atoms to more than 5000 atoms when using a real space grid discretization. The scaling is better or comparable in a NAO basis up to the 14,000 atoms level. Fourth, we exploit various numerical algorithms and, in particular, we introduce a partial Rayleigh-Ritz algorithm to achieve efficiency gains for systems comprising more than 10,000 electrons. We demonstrate the power of RESCU in solving KS-DFT problems using many examples running on 16, 64 and/or 256 cores: a 5832 Si atoms supercell; a 8788 Al atoms supercell; a 5324 Cu atoms supercell and a small DNA molecule submerged in 1713 water molecules for a total 5399 atoms. The KS-DFT is entirely converged in a few hours in all cases. Our results suggest that the RESCU method has reached a milestone of solving thousands of atoms by KS-DFT on a modest computer cluster.

  14. Research Update: Spatially resolved mapping of electronic structure on atomic level by multivariate statistical analysis

    NASA Astrophysics Data System (ADS)

    Belianinov, Alex; Ganesh, Panchapakesan; Lin, Wenzhi; Sales, Brian C.; Sefat, Athena S.; Jesse, Stephen; Pan, Minghu; Kalinin, Sergei V.

    2014-12-01

    Atomic level spatial variability of electronic structure in Fe-based superconductor FeTe0.55Se0.45 (Tc = 15 K) is explored using current-imaging tunneling-spectroscopy. Multivariate statistical analysis of the data differentiates regions of dissimilar electronic behavior that can be identified with the segregation of chalcogen atoms, as well as boundaries between terminations and near neighbor interactions. Subsequent clustering analysis allows identification of the spatial localization of these dissimilar regions. Similar statistical analysis of modeled calculated density of states of chemically inhomogeneous FeTe1-xSex structures further confirms that the two types of chalcogens, i.e., Te and Se, can be identified by their electronic signature and differentiated by their local chemical environment. This approach allows detailed chemical discrimination of the scanning tunneling microscopy data including separation of atomic identities, proximity, and local configuration effects and can be universally applicable to chemically and electronically inhomogeneous surfaces.

  15. Research Update: Spatially resolved mapping of electronic structure on atomic level by multivariate statistical analysis

    SciTech Connect

    Belianinov, Alex; Panchapakesan, G.; Lin, Wenzhi; Sales, Brian C.; Sefat, Athena Safa; Jesse, Stephen; Pan, Minghu; Kalinin, Sergei V.

    2014-12-02

    Atomic level spatial variability of electronic structure in Fe-based superconductor FeTe0.55Se0.45 (Tc = 15 K) is explored using current-imaging tunneling-spectroscopy. Multivariate statistical analysis of the data differentiates regions of dissimilar electronic behavior that can be identified with the segregation of chalcogen atoms, as well as boundaries between terminations and near neighbor interactions. Subsequent clustering analysis allows identification of the spatial localization of these dissimilar regions. Similar statistical analysis of modeled calculated density of states of chemically inhomogeneous FeTe1 x Sex structures further confirms that the two types of chalcogens, i.e., Te and Se, can be identified by their electronic signature and differentiated by their local chemical environment. This approach allows detailed chemical discrimination of the scanning tunneling microscopy data including separation of atomic identities, proximity, and local configuration effects and can be universally applicable to chemically and electronically inhomogeneous surfaces.

  16. The electronic structure of hard materials

    NASA Astrophysics Data System (ADS)

    Winarski, Robert Paul

    This research dissertation involves an experimental as well as a theoretical examination of the electronic structure of hard materials. The materials that are presented in this dissertation cover a wide class of materials, consisting of transition metal borides, irradiated polymer films, theoretically predicted superhard semiconductors, doped intermetallic alloys, and transition metal carbides. The borides are traditionally used in high temperature, hard coating applications, such as rocket nozzle linings, extreme wear surfaces, and corrosion coatings. Measurements of the borides appear to show that the bonding in these hard materials is primarily between the boron atoms in these systems. Also of note are the remarkably short interatomic distances between the boron atoms and between the boron and metal atoms in these materials. Irradiated polymer films are being developed for electronic applications, in the hopes that circuits can be developed that can benefit from the high thermal stability, dielectric properties, and mechanical properties provided by these materials. C3N4 is a theoretically predicted superhard material, and some of the first soft x-ray emission measurements of well-characterized samples of this compound are discussed in this work. Intermetallic alloys, in particular Ni3Al, are rather hard, but brittle metallic alloys. It has been found that the addition of boron atoms, in rather low concentrations, can increase the ductility of these alloys, allowing them to be utilized in a wider variety of applications. Measurements of this system have examined a question regarding the positioning of the boron atoms in the structures of this alloy. Finally, the transition metal carbides are used extensively as coatings in industrial applications such as cutting and grinding tools, and polishing compounds. Measurements of these materials suggest that the high degree of covalency between the metal and carbon atoms is primarily responsible for the hardness of

  17. Our Milky Way structure in the context of local galaxies

    NASA Astrophysics Data System (ADS)

    Shen, Juntai

    2015-08-01

    The Milky Way is the closest galaxy to us, and has been studied extensively due to its proximity. Understanding its structure and dynamics will help us understand spiral galaxies in general. I will review the latest research progress in the structure, kinematics, and dynamics of the Milky Way in the context of local galaxies. I will cover most structural components (the bulge/bar, disk, and spiral structures) and discuss the implications of some new results on the formation history of our home galaxy.

  18. Electronic structure of the primary electron donor of Blastochloris viridis heterodimer mutants : high field EPR study.

    SciTech Connect

    Ponomarenko, N. S.; Poluektov, O. G.; Bylina, E. J.; Norris, J. R.; Chemical Sciences and Engineering Division; Univ. of Chicago

    2010-09-01

    High-field electron paramagnetic resonance (HF EPR) has been employed to investigate the primary electron donor electronic structure of Blastochloris viridis heterodimer mutant reaction centers (RCs). In these mutants the amino acid substitution His(M200)Leu or His(L173)Leu eliminates a ligand to the primary electron donor, resulting in the loss of a magnesium in one of the constituent bacteriochlorophylls (BChl). Thus, the native BChl/BChl homodimer primary donor is converted into a BChl/bacteriopheophytin (BPhe) heterodimer. The heterodimer primary donor radical in chemically oxidized RCs exhibits a broadened EPR line indicating a highly asymmetric distribution of the unpaired electron over both dimer constituents. Observed triplet state EPR signals confirm localization of the excitation on the BChl half of the heterodimer primary donor. Theoretical simulation of the triplet EPR lineshapes clearly shows that, in the case of mutants, triplet states are formed by an intersystem crossing mechanism in contrast to the radical pair mechanism in wild type RCs. Photooxidation of the mutant RCs results in formation of a BPhe anion radical within the heterodimer pair. The accumulation of an intradimer BPhe anion is caused by the substantial loss of interaction between constituents of the heterodimer primary donor along with an increase in the reduction potential of the heterodimer primary donor D/D{sup +} couple. This allows oxidation of the cytochrome even at cryogenic temperatures and reduction of each constituent of the heterodimer primary donor individually. Despite a low yield of primary donor radicals, the enhancement of the semiquinone-iron pair EPR signals in these mutants indicates the presence of kinetically viable electron donors.

  19. Simulation of Probe Position-Dependent Electron Energy-Loss Fine Structure

    SciTech Connect

    Oxley, M. P.; Kapetanakis, M. D.; Prange, Micah P.; Varela, M.; Pennycook, Stephen J.; Pantelides, Sokrates T.

    2014-03-31

    We present a theoretical framework for calculating probe-position-dependent electron energy-loss near-edge structure for the scanning transmission electron microscope by combining density functional theory with dynamical scattering theory. We show how simpler approaches to calculating near-edge structure fail to include the fundamental physics needed to understand the evolution of near-edge structure as a function of probe position and investigate the dependence of near-edge structure on probe size. It is within this framework that density functional theory should be presented, in order to ensure that variations of near-edge structure are truly due to local electronic structure and how much from the diffraction and focusing of the electron beam.

  20. Using the electron localization function to correct for confinement physics in semi-local density functional theory

    SciTech Connect

    Hao, Feng Mattsson, Ann E.; Armiento, Rickard

    2014-05-14

    We have previously proposed that further improved functionals for density functional theory can be constructed based on the Armiento-Mattsson subsystem functional scheme if, in addition to the uniform electron gas and surface models used in the Armiento-Mattsson 2005 functional, a model for the strongly confined electron gas is also added. However, of central importance for this scheme is an index that identifies regions in space where the correction provided by the confined electron gas should be applied. The electron localization function (ELF) is a well-known indicator of strongly localized electrons. We use a model of a confined electron gas based on the harmonic oscillator to show that regions with high ELF directly coincide with regions where common exchange energy functionals have large errors. This suggests that the harmonic oscillator model together with an index based on the ELF provides the crucial ingredients for future improved semi-local functionals. For a practical illustration of how the proposed scheme is intended to work for a physical system we discuss monoclinic cupric oxide, CuO. A thorough discussion of this system leads us to promote the cell geometry of CuO as a useful benchmark for future semi-local functionals. Very high ELF values are found in a shell around the O ions, and take its maximum value along the Cu–O directions. An estimate of the exchange functional error from the effect of electron confinement in these regions suggests a magnitude and sign that could account for the error in cell geometry.

  1. Electronic Structures of Uranium Compounds Studied by Soft X-ray Photoelectron Spectroscopy

    NASA Astrophysics Data System (ADS)

    Fujimori, Shin-ichi; Takeda, Yukiharu; Okane, Tetsuo; Saitoh, Yuji; Fujimori, Atsushi; Yamagami, Hiroshi; Haga, Yoshinori; Yamamoto, Etsuji; Ōnuki, Yoshichika

    2016-06-01

    The electronic structures of uranium-based compounds have been studied by photoelectron spectroscopy with soft X-ray synchrotron radiation. Angle-resolved photoelectron spectroscopy with soft X-rays has made it possible to directly observe their bulk band structures and Fermi surfaces. It has been shown that the band structures and Fermi surfaces of itinerant compounds such as UB2, UN, and UFeGa5 are quantitatively described by a band-structure calculation treating all U 5f electrons as itinerant. Furthermore, the overall electronic structures of heavy-fermion compounds such as UPd2Al3, UNi2Al3, and URu2Si2 are also explained by a band-structure calculation, although some disagreements exist, which might originate from the electron correlation effect. This suggests that the itinerant description of U 5f states is an appropriate starting point for the description of their electronic structures. The situation is similar for ferromagnetic superconductors such as UGe2, URhGe, UCoGe, and UIr, although the complications from their low-symmetry crystal structures make it more difficult to describe their detailed electronic structures. The local electronic structures of the uranium site have been probed by core-level photoelectron spectroscopy with soft X-rays. The comparisons of core-level spectra of heavy-fermion compounds with typical itinerant and localized compounds suggest that the local electronic structures of most itinerant and heavy-fermion compounds are close to the U 5f3 configuration except for UPd2Al3 and UPt3. The core-level spectrum of UPd2Al3 has similarities to those of both itinerant and localized compounds, suggesting that it is located at the boundary between the itinerant and localized states. Moreover, the spectrum of UPt3 is very close to that of the localized compound UPd3, suggesting that it is nearly localized, although there are narrow quasi-particle bands in the vicinity of EF.

  2. Local Function Conservation in Sequence and Structure Space

    PubMed Central

    Weinhold, Nils; Sander, Oliver; Domingues, Francisco S.; Lengauer, Thomas; Sommer, Ingolf

    2008-01-01

    We assess the variability of protein function in protein sequence and structure space. Various regions in this space exhibit considerable difference in the local conservation of molecular function. We analyze and capture local function conservation by means of logistic curves. Based on this analysis, we propose a method for predicting molecular function of a query protein with known structure but unknown function. The prediction method is rigorously assessed and compared with a previously published function predictor. Furthermore, we apply the method to 500 functionally unannotated PDB structures and discuss selected examples. The proposed approach provides a simple yet consistent statistical model for the complex relations between protein sequence, structure, and function. The GOdot method is available online (http://godot.bioinf.mpi-inf.mpg.de). PMID:18604264

  3. A novel method to compare protein structures using local descriptors

    PubMed Central

    2011-01-01

    Background Protein structure comparison is one of the most widely performed tasks in bioinformatics. However, currently used methods have problems with the so-called "difficult similarities", including considerable shifts and distortions of structure, sequential swaps and circular permutations. There is a demand for efficient and automated systems capable of overcoming these difficulties, which may lead to the discovery of previously unknown structural relationships. Results We present a novel method for protein structure comparison based on the formalism of local descriptors of protein structure - DEscriptor Defined Alignment (DEDAL). Local similarities identified by pairs of similar descriptors are extended into global structural alignments. We demonstrate the method's capability by aligning structures in difficult benchmark sets: curated alignments in the SISYPHUS database, as well as SISY and RIPC sets, including non-sequential and non-rigid-body alignments. On the most difficult RIPC set of sequence alignment pairs the method achieves an accuracy of 77% (the second best method tested achieves 60% accuracy). Conclusions DEDAL is fast enough to be used in whole proteome applications, and by lowering the threshold of detectable structure similarity it may shed additional light on molecular evolution processes. It is well suited to improving automatic classification of structure domains, helping analyze protein fold space, or to improving protein classification schemes. DEDAL is available online at http://bioexploratorium.pl/EP/DEDAL. PMID:21849047

  4. Local Structure of Implicated Pd in Si Using PAC

    NASA Astrophysics Data System (ADS)

    Brett, D. A.; Dogra, R.; Byrne, A. P.; Ridgway, M. C.; Bartels, J.; Vianden, R.

    2004-11-01

    TDPAC has been employed to study the local structure of implanted palladium in silicon utilizing 87 75 keV γ γ cascade of probe nucleus 100Pd. The observed hyperfine parameters revealed the presence of Pd V defect pair only in highly doped n-type silicon. A dumbbell structure with substitutional palladium and silicon vacancy as nearest neigbor is suggested for this defect.

  5. Cosmic Flows and the Structure of the Local Universe

    NASA Astrophysics Data System (ADS)

    Steinmetz, Matthias

    2016-03-01

    The Local Volume is the area of the cosmos we can analyze in most detail with respect to the properties of its galaxy population, their abundance, their inner structure, their distribution, and their formation. Indeed, many challenges of the cosmological concordance model such as the substructure crisis or the surprising occurrence of vast planes of satellite galaxies are intimately linked to observations of the local galaxy population. However, owing to the peculiar environment of our Milky Way system and its cosmic neighborhood, the Local Volume may also be severely biased. Cosmography, i.e. the reconstruction of the local cosmic web from cosmic flows, and constrained simulations of structure formation as a tool to produce simulated local group analogues provide a powerful method to analyze and quantify these biases. Possible applications include the analysis of the local distribution of dwarf galaxies around luminous galaxies and the characterization of the mass accretion history of these objects. Thanks to the extension of galaxy velocity data out to distances in excess of 200Mpc, we are now capable to reconstruct the 3D matter distribution out to these distances, thus constraining the formation history of object such as the Virgo Cluster.

  6. Local dynamic range compensation for scanning electron microscope imaging system.

    PubMed

    Sim, K S; Huang, Y H

    2015-01-01

    This is the extended project by introducing the modified dynamic range histogram modification (MDRHM) and is presented in this paper. This technique is used to enhance the scanning electron microscope (SEM) imaging system. By comparing with the conventional histogram modification compensators, this technique utilizes histogram profiling by extending the dynamic range of each tile of an image to the limit of 0-255 range while retains its histogram shape. The proposed technique yields better image compensation compared to conventional methods. PMID:25969945

  7. One Single Static Measurement Predicts Wave Localization in Complex Structures

    NASA Astrophysics Data System (ADS)

    Lefebvre, Gautier; Gondel, Alexane; Dubois, Marc; Atlan, Michael; Feppon, Florian; Labbé, Aimé; Gillot, Camille; Garelli, Alix; Ernoult, Maxence; Mayboroda, Svitlana; Filoche, Marcel; Sebbah, Patrick

    2016-08-01

    A recent theoretical breakthrough has brought a new tool, called the localization landscape, for predicting the localization regions of vibration modes in complex or disordered systems. Here, we report on the first experiment which measures the localization landscape and demonstrates its predictive power. Holographic measurement of the static deformation under uniform load of a thin plate with complex geometry provides direct access to the landscape function. When put in vibration, this system shows modes precisely confined within the subregions delineated by the landscape function. Also the maxima of this function match the measured eigenfrequencies, while the minima of the valley network gives the frequencies at which modes become extended. This approach fully characterizes the low frequency spectrum of a complex structure from a single static measurement. It paves the way for controlling and engineering eigenmodes in any vibratory system, especially where a structural or microscopic description is not accessible.

  8. One Single Static Measurement Predicts Wave Localization in Complex Structures.

    PubMed

    Lefebvre, Gautier; Gondel, Alexane; Dubois, Marc; Atlan, Michael; Feppon, Florian; Labbé, Aimé; Gillot, Camille; Garelli, Alix; Ernoult, Maxence; Mayboroda, Svitlana; Filoche, Marcel; Sebbah, Patrick

    2016-08-12

    A recent theoretical breakthrough has brought a new tool, called the localization landscape, for predicting the localization regions of vibration modes in complex or disordered systems. Here, we report on the first experiment which measures the localization landscape and demonstrates its predictive power. Holographic measurement of the static deformation under uniform load of a thin plate with complex geometry provides direct access to the landscape function. When put in vibration, this system shows modes precisely confined within the subregions delineated by the landscape function. Also the maxima of this function match the measured eigenfrequencies, while the minima of the valley network gives the frequencies at which modes become extended. This approach fully characterizes the low frequency spectrum of a complex structure from a single static measurement. It paves the way for controlling and engineering eigenmodes in any vibratory system, especially where a structural or microscopic description is not accessible. PMID:27563967

  9. The Changing Market Structure of Local Television News.

    ERIC Educational Resources Information Center

    Powers, Angela

    The growth in competition for revenues, along with the advent of cable, independent television and video cassette recorders (VCR), may signify a change in the market structure of local television news. To explain if and how this change may be occurring, an explanation of economic theory as well as evidence from "Broadcast and Cable Yearbook" and…

  10. Structures of Participation in the "University of Local Knowledge"

    ERIC Educational Resources Information Center

    Evans, Penny; Irish, Sharon

    2013-01-01

    "Structures of Participation" concerns a recent media arts project, the University of Local Knowledge (ULK). ULK is simultaneously a critique of established academic institutions and disciplines and a system for self-organized learning among the residents of Knowle West, an area of south Bristol (UK). Beginning in 2009, the Knowle West…

  11. Local Structure of CuIn3Se5

    SciTech Connect

    Chang, C. H.; Wei, S. H.; Leyarovska, N.; Johnson, J. W.; Zhang, S. B.; Stanbery, B. J.; Anderson, T. J.

    2000-01-01

    The results of a detailed EXAFS study of the Cu-K, In-K, and Se-K edges CuIn3Se5 are reported. The Cu and In first nearest neighbor local structures were found to be almost identical to those in CuInSe2.

  12. Taking advantage of local structure descriptors to analyze interresidue contacts in protein structures and protein complexes.

    PubMed

    Martin, Juliette; Regad, Leslie; Etchebest, Catherine; Camproux, Anne-Claude

    2008-11-15

    Interresidue protein contacts in proteins structures and at protein-protein interface are classically described by the amino acid types of interacting residues and the local structural context of the contact, if any, is described using secondary structures. In this study, we present an alternate analysis of interresidue contact using local structures defined by the structural alphabet introduced by Camproux et al. This structural alphabet allows to describe a 3D structure as a sequence of prototype fragments called structural letters, of 27 different types. Each residue can then be assigned to a particular local structure, even in loop regions. The analysis of interresidue contacts within protein structures defined using Voronoï tessellations reveals that pairwise contact specificity is greater in terms of structural letters than amino acids. Using a simple heuristic based on specificity score comparison, we find that 74% of the long-range contacts within protein structures are better described using structural letters than amino acid types. The investigation is extended to a set of protein-protein complexes, showing that the similar global rules apply as for intraprotein contacts, with 64% of the interprotein contacts best described by local structures. We then present an evaluation of pairing functions integrating structural letters to decoy scoring and show that some complexes could benefit from the use of structural letter-based pairing functions. PMID:18491388

  13. Electron and hole dynamics in the electronic and structural phase transitions of VO2

    NASA Astrophysics Data System (ADS)

    Haglund, Richard

    2015-03-01

    The ultrafast, optically induced insulator-to-metal transition (IMT) and the associated structural phase transition (SPT) in vanadium dioxide (VO2) have been studied for over a decade. However, only recently have effects due to the combined presence of electron-hole pairs and injected electrons been observed. Here we compare and contrast IMT dynamics when both hot electrons and optically excited electron-hole pairs are involved, in (1) thin films of VO2 overlaid by a thin gold foil, in which hot electrons are generated by 1.5 eV photons absorbed in the foil and accelerated through the VO2 by an applied electric field; (2) VO2 nanoparticles covered with a sparse mesh of gold nanoparticles averaging 20-30 nm in diameter in which hot electrons are generated by resonant excitation and decay of the localized surface plasmon; and (3) bare VO2 thin films excited by intense near-single-cycle THz pulses. In the first case, the IMT is driven by excitation of the bulk gold plasmon, and the SPT appears on a few-picosecond time scale. In the second case, density-functional calculations indicate that above a critical carrier density, the addition of a single electron to a 27-unit supercell drives the catastrophic collapse of the coherent phonon associated with, and leading to, the SPT. In the third case, sub-bandgap-energy photons (approximately 0.1 eV) initiate the IMT, but exhibit the same sub-100 femtosecond switching time and coherent phonon dynamics as observed when the IMT is initiated by 1.5 eV photons. This suggests that the underlying mechanism must be quite different, possibly THz-field induced interband tunneling of spatially separated electron-hole pairs. The implications of these findings for ultrafast switching in opto-electronic devices - such as hybrid VO2 silicon ring resonators - are briefly considered. Support from the National Science Foundation (DMR-1207407), the Office of Science, U.S. Department of Energy (DE-FG02-01ER45916) and the Defense Threat

  14. O(N) methods in electronic structure calculations

    NASA Astrophysics Data System (ADS)

    Bowler, D. R.; Miyazaki, T.

    2012-03-01

    Linear-scaling methods, or O(N) methods, have computational and memory requirements which scale linearly with the number of atoms in the system, N, in contrast to standard approaches which scale with the cube of the number of atoms. These methods, which rely on the short-ranged nature of electronic structure, will allow accurate, ab initio simulations of systems of unprecedented size. The theory behind the locality of electronic structure is described and related to physical properties of systems to be modelled, along with a survey of recent developments in real-space methods which are important for efficient use of high-performance computers. The linear-scaling methods proposed to date can be divided into seven different areas, and the applicability, efficiency and advantages of the methods proposed in these areas are then discussed. The applications of linear-scaling methods, as well as the implementations available as computer programs, are considered. Finally, the prospects for and the challenges facing linear-scaling methods are discussed.

  15. Graph-based linear scaling electronic structure theory

    NASA Astrophysics Data System (ADS)

    Niklasson, Anders M. N.; Mniszewski, Susan M.; Negre, Christian F. A.; Cawkwell, Marc J.; Swart, Pieter J.; Mohd-Yusof, Jamal; Germann, Timothy C.; Wall, Michael E.; Bock, Nicolas; Rubensson, Emanuel H.; Djidjev, Hristo

    2016-06-01

    We show how graph theory can be combined with quantum theory to calculate the electronic structure of large complex systems. The graph formalism is general and applicable to a broad range of electronic structure methods and materials, including challenging systems such as biomolecules. The methodology combines well-controlled accuracy, low computational cost, and natural low-communication parallelism. This combination addresses substantial shortcomings of linear scaling electronic structure theory, in particular with respect to quantum-based molecular dynamics simulations.

  16. Probing Actinide Electronic Structure through Pu Cluster Calculations

    DOE PAGESBeta

    Ryzhkov, Mickhail V.; Mirmelstein, Alexei; Yu, Sung-Woo; Chung, Brandon W.; Tobin, James G.

    2013-02-26

    The calculations for the electronic structure of clusters of plutonium have been performed, within the framework of the relativistic discrete-variational method. Moreover, these theoretical results and those calculated earlier for related systems have been compared to spectroscopic data produced in the experimental investigations of bulk systems, including photoelectron spectroscopy. Observation of the changes in the Pu electronic structure as a function of size provides powerful insight for aspects of bulk Pu electronic structure.

  17. Graph-based linear scaling electronic structure theory.

    PubMed

    Niklasson, Anders M N; Mniszewski, Susan M; Negre, Christian F A; Cawkwell, Marc J; Swart, Pieter J; Mohd-Yusof, Jamal; Germann, Timothy C; Wall, Michael E; Bock, Nicolas; Rubensson, Emanuel H; Djidjev, Hristo

    2016-06-21

    We show how graph theory can be combined with quantum theory to calculate the electronic structure of large complex systems. The graph formalism is general and applicable to a broad range of electronic structure methods and materials, including challenging systems such as biomolecules. The methodology combines well-controlled accuracy, low computational cost, and natural low-communication parallelism. This combination addresses substantial shortcomings of linear scaling electronic structure theory, in particular with respect to quantum-based molecular dynamics simulations. PMID:27334148

  18. PredyFlexy: flexibility and local structure prediction from sequence

    PubMed Central

    de Brevern, Alexandre G.; Bornot, Aurélie; Craveur, Pierrick; Etchebest, Catherine; Gelly, Jean-Christophe

    2012-01-01

    Protein structures are necessary for understanding protein function at a molecular level. Dynamics and flexibility of protein structures are also key elements of protein function. So, we have proposed to look at protein flexibility using novel methods: (i) using a structural alphabet and (ii) combining classical X-ray B-factor data and molecular dynamics simulations. First, we established a library composed of structural prototypes (LSPs) to describe protein structure by a limited set of recurring local structures. We developed a prediction method that proposes structural candidates in terms of LSPs and predict protein flexibility along a given sequence. Second, we examine flexibility according to two different descriptors: X-ray B-factors considered as good indicators of flexibility and the root mean square fluctuations, based on molecular dynamics simulations. We then define three flexibility classes and propose a method based on the LSP prediction method for predicting flexibility along the sequence. This method does not resort to sophisticate learning of flexibility but predicts flexibility from average flexibility of predicted local structures. The method is implemented in PredyFlexy web server. Results are similar to those obtained with the most recent, cutting-edge methods based on direct learning of flexibility data conducted with sophisticated algorithms. PredyFlexy can be accessed at http://www.dsimb.inserm.fr/dsimb_tools/predyflexy/. PMID:22689641

  19. The limits of local correlation theory: electronic delocalization and chemically smooth potential energy surfaces.

    PubMed

    Subotnik, Joseph E; Sodt, Alex; Head-Gordon, Martin

    2008-01-21

    Local coupled-cluster theory provides an algorithm for measuring electronic correlation quickly, using only the spatial locality of localized electronic orbitals. Previously, we showed [J. Subotnik et al., J. Chem. Phys. 125, 074116 (2006)] that one may construct a local coupled-cluster singles-doubles theory which (i) yields smooth potential energy surfaces and (ii) achieves near linear scaling. That theory selected which orbitals to correlate based only on the distances between the centers of different, localized orbitals, and the approximate potential energy surfaces were characterized as smooth using only visual identification. This paper now extends our previous algorithm in three important ways. First, locality is now based on both the distances between the centers of orbitals as well as the spatial extent of the orbitals. We find that, by accounting for the spatial extent of a delocalized orbital, one can account for electronic correlation in systems with some electronic delocalization using fast correlation methods designed around orbital locality. Second, we now enforce locality on not just the amplitudes (which measure the exact electron-electron correlation), but also on the two-electron integrals themselves (which measure the bare electron-electron interaction). Our conclusion is that we can bump integrals as well as amplitudes, thereby gaining a tremendous increase in speed and paradoxically increasing the accuracy of our LCCSD approach. Third and finally, we now make a rigorous definition of chemical smoothness as requiring that potential energy surfaces not support artificial maxima, minima, or inflection points. By looking at first and second derivatives from finite difference techniques, we demonstrate complete chemical smoothness of our potential energy surfaces (bumping both amplitudes and integrals). These results are significant both from a theoretical and from a computationally practical point of view. PMID:18205484

  20. Quantum Localization of Coherent π-Electron Angular Momentum in (P)-2,2'-Biphenol.

    PubMed

    Yamaki, Masahiro; Mineo, Hirobumi; Teranishi, Yoshiaki; Hayashi, Michitoshi; Fujimura, Yuichi; Nakamura, Hiroki; Lin, Sheng Hsien

    2014-06-01

    Controlling π-electrons with delocalized character is one of the fundamental issues in femtosecond and attosecond chemistry. Localization of π-electron rotation by using laser pulses is expected to play an essential role in nanoscience. The π-electron rotation created at a selected aromatic ring of a single molecule induces a local intense electromagnetic field, which is a new type of ultrafast optical control functioning. We propose a quantum localization of coherent π-electron angular momentum in (P)-2,2'-biphenol, which is a simple, covalently linked chiral aromatic ring chain molecule. The localization considered here consists of sequential two steps: the first step is to localize the π-electron angular momentum at a selected ring of the two benzene rings, and the other is to maintain the localization. Optimal control theory was used for obtaining the optimized electric fields of linearly polarized laser pulses to realize the localization. The optimal electric fields and the resultant coherent electronic dynamics are analyzed. PMID:26273893

  1. Structural, electronic, and magnetic characteristics of Np2Co17

    NASA Astrophysics Data System (ADS)

    Halevy, I.; Hen, A.; Orion, I.; Colineau, E.; Eloirdi, R.; Griveau, J.-C.; Gaczyński, P.; Wilhelm, F.; Rogalev, A.; Sanchez, J.-P.; Winterrose, M. L.; Magnani, N.; Shick, A. B.; Caciuffo, R.

    2012-01-01

    A previously unknown neptunium-transition-metal binary compound Np2Co17 has been synthesized and characterized by means of powder x-ray diffraction, 237Np Mössbauer spectroscopy, superconducting-quantum-interference-device magnetometry, and x-ray magnetic circular dichroism (XMCD). The compound crystallizes in a Th2Ni17-type hexagonal structure with room-temperature lattice parameters a=8.3107(1) Å and c=8.1058(1) Å. Magnetization curves indicate the occurrence of ferromagnetic order below TC>350 K. Mössbauer spectra suggest a Np3+ oxidation state and give an ordered moment of μNp=1.57(4) μB and μNp=1.63(4) μB for the Np atoms located, respectively, at the 2b and 2d crystallographic positions of the P63/mmc space group. Combining these values with a sum-rule analysis of the XMCD spectra measured at the neptunium M4,5 absorption edges, one obtains the spin and orbital contributions to the site-averaged Np moment [μS=-1.88(9) μB, μL=3.48(9) μB]. The ratio between the expectation value of the magnetic-dipole moment and the spin magnetic moment (mmd/μS=+1.36) is positive as predicted for localized 5f electrons and lies between the values calculated in intermediate-coupling (IC) and jj approximations. The expectation value of the angular part of the spin-orbit-interaction operator is in excellent agreement with the IC estimate. The ordered moment averaged over the four inequivalent Co sites, as obtained from the saturation value of the magnetization, is μCo≃1.6 μB. The experimental results are discussed against the predictions of first-principles electronic-structure calculations based on the spin-polarized local-spin-density approximation plus the Hubbard interaction.

  2. Localization of acoustic modes in periodic porous silicon structures

    PubMed Central

    2014-01-01

    The propagation of longitudinal acoustic waves in multilayer structures based on porous silicon and the experimental measurement of acoustic transmission for the structures in the gigahertz range are reported and studied theoretically. The considered structures exhibit band gaps in the transmission spectrum and these are localized modes inside the band gap, coming from defect layers introduced in periodic systems. The frequency at which the acoustic resonances appear can be tuned by changing the porosity and/or thickness of the defect layer. PMID:25206317

  3. Local magnetic structure determination using polarized neutron holography

    SciTech Connect

    Szakál, Alex Markó, Márton Cser, László

    2015-05-07

    A unique and important property of the neutron is that it possesses magnetic moment. This property is widely used for determination of magnetic structure of crystalline samples observing the magnetic components of the diffraction peaks. Investigations of diffraction patterns give information only about the averaged structure of a crystal but for discovering of local spin arrangement around a specific (e.g., impurity) nucleus remains still a challenging problem. Neutron holography is a useful tool to investigate the local structure around a specific nucleus embedded in a crystal lattice. The method has been successfully applied experimentally in several cases using non-magnetic short range interaction of the neutron and the nucleus. A mathematical model of the hologram using interaction between magnetic moment of the atom and the neutron spin for polarized neutron holography is provided. Validity of a polarized neutron holographic experiment is demonstrated by applying the proposed method on model systems.

  4. European X-Ray Free Electron Laser (EXFEL): local implications

    NASA Astrophysics Data System (ADS)

    Romaniuk, Ryszard S.

    2013-10-01

    European X-Ray FEL - free electron laser is under construction in DESY Hamburg. It is scheduled to be operational at 2015/16 at a cost more than 1 billion Euro. The laser uses SASE method to generate x-ray light. It is propelled by an electron linac of 17,5GeV energy and more than 2km in length. The linac uses superconducting SRF TESLA technology working at 1,3 GHz in frequency. The prototype of EXFEL is FLASH Laser (200 m in length), where the "proof of principle" was checked, and from the technologies were transferred to the bigger machine. The project was stared in the nineties by building a TTF Laboratory -Tesla Test Facility. The EXFEL laser is a child of a much bigger teraelectronovolt collider project TESLA (now abandoned in Germany but undertaken by international community in a form the ILC). A number of experts and young researchers from Poland participate in the design, construction and research of the FLASH and EXFEL lasers.

  5. A Theoretical Study of NO2 Complexes with Aluminium and Gallium Based on Topological Analysis of Electron Density and Electron Localization Function

    SciTech Connect

    Panek, Jaroslaw; Latajaka, Zdzislaw

    2000-12-26

    Results of DFT and MP4 calculations on AlNO2 and GaNO2 molecules are presented. One Cs and two C2v structures (two minima and one TS) are found and their energies and vibrational frequencies are reported and discussed. The minima are close in energy and lie ca. 70 kcal mol-1 below reactants (M+NO2). More insight is obtained via topological analysis of electron density and electron localization function (ELF). It is shown that the molecules are bound mainly via electrostatic interactions, and there is a significant charge transfer from metal atom to the NO2 moiety. Detailed analysis of the ELF shows that the loss of stability of gallium complexes with respect to aluminium structures is best explained by (antibonding) influence of gallium semi-cored electrons.

  6. Early detection of local buckling in structural members

    NASA Astrophysics Data System (ADS)

    Ali, Bashir; Sundaresan, Mannur J.; Schulz, Mark J.; Hughes, Derke

    2005-05-01

    Most structural health monitoring analyses to date have focused on the determination of damage in the form of crack growth in metallic materials or delamination or other types of damage growth in composite materials. However, in many applications, local instability in the form of buckling can be the precursor to more extensive damage and unstable failure of the structure. If buckling could be detected in the very early stages, there is a possibility of taking preventive measures to stabilize and save the structure. Relatively few investigations have addressed this type of damage initiation in structures. Recently, during the structural health monitoring of a wind turbine blade, local buckling was identified as the cause of premature failure. A stress wave propagation technique was used in this test to detect the precursor to the buckling failure in the form of early changes in the local curvature of the blade. These conditions have also been replicated in the laboratory and results are reported in this paper. A composite column was subjected to axial compression to induce various levels of buckling deformation. Two different techniques were used to detect the precursors to buckling in this column. The first identifier is the change in the vibration shapes and natural frequencies of the column. The second is the change in the characteristics of diagnostic Lamb waves during the buckling deformation. Experiments indicate that very small changes in curvature during the initial stages of buckling are detectable using the structural health monitoring techniques. The experimental vibration characteristics of the column with slight initial curvatures compared qualitatively with finite element results. The finite element analysis is used to identify the frequencies that are most sensitive to buckling deformation, and to select suitable locations for the placement of sensors that can detect even small changes in the local curvature.

  7. Topological framework for local structure analysis in condensed matter

    PubMed Central

    Lazar, Emanuel A.; Han, Jian; Srolovitz, David J.

    2015-01-01

    Physical systems are frequently modeled as sets of points in space, each representing the position of an atom, molecule, or mesoscale particle. As many properties of such systems depend on the underlying ordering of their constituent particles, understanding that structure is a primary objective of condensed matter research. Although perfect crystals are fully described by a set of translation and basis vectors, real-world materials are never perfect, as thermal vibrations and defects introduce significant deviation from ideal order. Meanwhile, liquids and glasses present yet more complexity. A complete understanding of structure thus remains a central, open problem. Here we propose a unified mathematical framework, based on the topology of the Voronoi cell of a particle, for classifying local structure in ordered and disordered systems that is powerful and practical. We explain the underlying reason why this topological description of local structure is better suited for structural analysis than continuous descriptions. We demonstrate the connection of this approach to the behavior of physical systems and explore how crystalline structure is compromised at elevated temperatures. We also illustrate potential applications to identifying defects in plastically deformed polycrystals at high temperatures, automating analysis of complex structures, and characterizing general disordered systems. PMID:26460045

  8. Topological framework for local structure analysis in condensed matter.

    PubMed

    Lazar, Emanuel A; Han, Jian; Srolovitz, David J

    2015-10-27

    Physical systems are frequently modeled as sets of points in space, each representing the position of an atom, molecule, or mesoscale particle. As many properties of such systems depend on the underlying ordering of their constituent particles, understanding that structure is a primary objective of condensed matter research. Although perfect crystals are fully described by a set of translation and basis vectors, real-world materials are never perfect, as thermal vibrations and defects introduce significant deviation from ideal order. Meanwhile, liquids and glasses present yet more complexity. A complete understanding of structure thus remains a central, open problem. Here we propose a unified mathematical framework, based on the topology of the Voronoi cell of a particle, for classifying local structure in ordered and disordered systems that is powerful and practical. We explain the underlying reason why this topological description of local structure is better suited for structural analysis than continuous descriptions. We demonstrate the connection of this approach to the behavior of physical systems and explore how crystalline structure is compromised at elevated temperatures. We also illustrate potential applications to identifying defects in plastically deformed polycrystals at high temperatures, automating analysis of complex structures, and characterizing general disordered systems. PMID:26460045

  9. DOLORS: versatile strategy for internal labeling and domain localization in electron microscopy.

    PubMed

    Lau, Pick-Wei; Potter, Clinton S; Carragher, Bridget; MacRae, Ian J

    2012-12-01

    Single-particle electron microscopy (EM) is a powerful tool for studying the structures of large biological molecules. However, the achievable resolution does not always allow for direct recognition of individual protein domains. Labels that can be visualized by EM have been developed for protein termini, but tagging internal domains remains a challenge. We describe a robust strategy for determining the position of internal sites within EM maps, termed domain localization by RCT sampling (DOLORS). DOLORS uses monovalent streptavidin added posttranslationally to tagged sites in the target protein. Internal labels generally display less conformational flexibility than terminal labels, providing more precise positional information. Automated methods are used to rapidly generate assemblies of unique 3D models allowing the attachment sites of labeled domains to be accurately identified and thus provide an overall architectural map of the molecule. PMID:23217681

  10. Local structure of ZnO micro flowers and nanoparticles obtained by micro segmented flow synthesis

    SciTech Connect

    Li, Shuning; Roy, Amitava; Lichtenberg, Henning; Merchan, Gregory; Kumar, Challa S.S.R.; Köhler, J. Michael

    2012-03-07

    The micro-segmented flow technique was applied for continuous synthesis of ZnO micro- and nanoparticles with short residence times of 9.4 s and 21.4 s, respectively. The obtained particles were characterized by scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Small angle X-ray scattering (SAXS) and photoluminescence spectroscopy were used to determine the size and optical properties of ZnO nanoparticles. In addition, extended X-ray absorption fine structure (EXAFS) spectroscopy was employed to investigate local structural properties. The EXAFS measurements reveal a larger degree of structural disorder in the nanoparticles than the microparticles. These structural changes should be taken into consideration while evaluating the size-dependent visible emission of ZnO nanoparticles.

  11. Dramatic changes in electronic structure revealed by fractionally charged nuclei

    SciTech Connect

    Cohen, Aron J.; Mori-Sánchez, Paula

    2014-01-28

    Discontinuous changes in the electronic structure upon infinitesimal changes to the Hamiltonian are demonstrated. These are revealed in one and two electron molecular systems by full configuration interaction (FCI) calculations when the realm of the nuclear charge is extended to be fractional. FCI electron densities in these systems show dramatic changes in real space and illustrate the transfer, hopping, and removal of electrons. This is due to the particle nature of electrons seen in stretched systems and is a manifestation of an energy derivative discontinuity at constant number of electrons. Dramatic errors of density functional theory densities are seen in real space as this physics is missing from currently used approximations. The movements of electrons in these simple systems encapsulate those in real physical processes, from chemical reactions to electron transport and pose a great challenge for the development of new electronic structure methods.

  12. Electronic structure imperfections and chemical bonding at graphene interfaces

    NASA Astrophysics Data System (ADS)

    Schultz, Brian Joseph

    nanomaterial with lateral dimensions in the hundreds of microns if not larger, with a corresponding atomic vertical thickness poses significant difficulties. Graphene's unique structure is dominated by surface area or potentially hybridized interfaces; consequently, the true realization of this remarkable nanomaterial in device constructs relies on engineering graphene interfaces at the surface in order to controllably mold the electronic structure. Near-edge X-ray absorption fine-structure (NEXAFS) spectroscopy and the transmission mode analogue scanning transmission X-ray microscopy (STXM) are particularly useful tools to study the unoccupied states of graphene and graphene interfaces. In addition, polarized NEXAFS and STXM studies provide information on surface orientation, bond sterics, and the extent of substrate alignment before and after interfacial hybridization. The work presented in this dissertation is fundamentally informed by NEXAFS and STXM measurements on graphene/metal, graphene/dielectric, and graphene/organic interfaces. We start with a general review of the electronic structure of freestanding graphene and graphene interfaces in Chapter 1. In Chapter 2, we investigate freestanding single-layer graphene via STXM and NEXAFS demonstrating that electronic structure heterogeneities from synthesis and processing are ubiquitous in 2-dimensional graphene. We show the mapping of discrete charge transfer regions as a result of doped impurities that decorate the surfaces of graphene and that transfer processing imparts local electronic corrugations or ripples. In corroboration with density functional theory, definitive assignments to the spectral features, global steric orientations of the localized domains, and quantitative charge transfer schemes are evidenced. In the following chapters, we deliberately (Chapter 3) incorporate substitutional nitrogen into reduced graphene oxide to induce C--N charge redistribution and improve global conductivity, (Chapter 4

  13. Studies of local electron heat transport on TFTR

    SciTech Connect

    Fredrickson, E.D.; Chang, Z.Y.; Janos, A.; McGuire, K.M.; Scott, S.; Taylor, G.

    1993-08-16

    The anomalously fast relaxation of the perturbations to the electron temperature profile caused by a sawtooth crash has been studied extensively on TFTR. We will show that on a short timescale the heat pulse is not simply diffusive as has been generally assumed, but that modeling of the heat pulse requires a transient enhancement in {chi}{sub e} following the sawtooth crash. It will be shown that the time-dependent enhancement in {chi}{sub e} predicted by non-linear thermal transport models, i.e., incremental {chi} models or the Rebut-Lallia-Watkins transport model, is much smaller than that required to explain the anomalies in the heat pulse propagation.

  14. Tracking Coherent Structures and Source Localization in Geophysical Flows

    NASA Astrophysics Data System (ADS)

    Forgoston, Eric; Hsieh, Ani; Schwartz, Ira; Yecko, Philip

    There has been a steady increase in the deployment of autonomous underwater and surface vehicles for applications such as ocean monitoring, tracking of marine processes, and forecasting contaminant transport. The underwater environment poses unique challenges since robots must operate in a communication and localization-limited environment where their dynamics are tightly coupled with the environmental dynamics. This work presents current efforts in understanding the impact of geophysical fluid dynamics on underwater vehicle control and autonomy. The focus of the talk is on the use of collaborative vehicles to track Lagrangian coherent structures and to localize contaminant spills. Research supported by the National Science Foundation and the Office of Naval Research.

  15. Binding-activated localization microscopy of DNA structures.

    PubMed

    Schoen, Ingmar; Ries, Jonas; Klotzsch, Enrico; Ewers, Helge; Vogel, Viola

    2011-09-14

    Many nucleic acid stains show a strong fluorescence enhancement upon binding to double-stranded DNA. Here we exploit this property to perform superresolution microscopy based on the localization of individual binding events. The dynamic labeling scheme and the optimization of fluorophore brightness yielded a resolution of ∼14 nm (fwhm) and a spatial sampling of 1/nm. We illustrate our approach with two different DNA-binding dyes and apply it to visualize the organization of the bacterial chromosome in fixed Escherichia coli cells. In general, the principle of binding-activated localization microscopy (BALM) can be extended to other dyes and targets such as protein structures. PMID:21838238

  16. Effect of local coordination of Mn on Mn-L2,3 edge electron energy loss spectrum

    NASA Astrophysics Data System (ADS)

    Nishida, Shuji; Kobayashi, Shunsuke; Kumamoto, Akihito; Ikeno, Hidekazu; Mizoguchi, Teruyasu; Tanaka, Isao; Ikuhara, Yuichi; Yamamoto, Takahisa

    2013-08-01

    The effects of the local coordination environment of Mn ions in perovskite manganese oxides on the Mn-L2,3 edge electron energy loss (EEL) spectra was experimentally and theoretically investigated. The Mn-L2,3 edge EEL spectra were observed for various perovskite manganese oxides, including YMnO3, LaMnO3, BaMnO3, SrMnO3, and CaMnO3, in which the Mn ions have different valence states and local coordination. The experiment revealed that the Mn L3/L2 ratio is influenced not only by the valence state but also by the local environment of the Mn ions. Furthermore, compared to the Mn L3/L2 ratios of Mn3+ compounds, the Mn L3/L2 ratios of the Mn4+ compounds are found to be much more sensitive to local distortions. The ab-initio multiplet calculation of the Mn-L2,3 edge EEL spectra revealed that the effects of local coordination on the spectral features are dependent on the local electronic structures of the Mn ions. These findings indicate that the valence state as well as the local environments of the Mn ions can be unraveled by combining experimental and theoretical investigations of Mn-L2,3 edge EEL spectra.

  17. Characterizing the Locality of Diabatic States forElectronic Excitation Transfer By Decomposing theDiabatic Coupling

    SciTech Connect

    Newton, M.D.; Vura-Weis, J.; Wasielewski, M.R.; Subotnik, J.E.

    2010-10-19

    A common strategy to calculate electronic coupling matrix elements for charge or energy transfer is to take the adiabatic states generated by electronic structure computations and rotate them to form localized diabatic states. In this paper, we show that, for intermolecular transfer of singlet electronic excitation, usually we cannot fully localize the electronic excitations in this way. Instead, we calculate putative initial and final states with small excitation tails caused by weak interactions with high energy excited states in the electronic manifold. These tails do not lead to substantial changes in the total diabatic coupling between states, but they do lead to a different partitioning of the total coupling between Coulomb (Forster), exchange (Dexter), and one-electron components. The tails may be reduced by using a multistate diabatic model or eliminated entirely by truncation (denoted as 'chopping'). Without more information, we are unable to conclude with certainty whether the observed diabatic tails are a physical reality or a computational artifact. This research suggests that decomposition of the diabatic coupling between chromophores into Coulomb, exchange, and one-electron components may depend strongly on the number of states considered, and such results should be treated with caution.

  18. Fluctuations and local ice structure in model supercooled water

    NASA Astrophysics Data System (ADS)

    Overduin, S. D.; Patey, G. N.

    2015-09-01

    Large-scale simulations (up to 32 000 molecules) are used to analyze local structures and fluctuations for the TIP4P/2005 and TIP5P water models, under deeply supercooled conditions, near previously proposed liquid-liquid critical points. Bulk freezing does not occur in our simulations, but correlations between molecules with local ice-like structure (ice-like molecules) are strong and long ranged (˜4 nm), exceeding the shortest dimension of smaller simulation cells at the lowest temperatures considered. Correlations between ice-like molecules decay slowly at low temperature, on the order of a hundred nanoseconds. Local ice-like structure is strongly correlated with highly tetrahedral liquid structure at all times, both structures contribute to density fluctuations, and to the associated anomalous scattering. For the TIP4P/2005 and TIP5P models, we show that the apparent spontaneous liquid-liquid phase separations, recently reported [T. Yagasaki, M. Matsumoto, and H. Tanaka, Phys. Rev. E 89, 020301 (2014)] for small rectangular simulation cells below the proposed critical points, exhibit strong system size dependence and do not occur at all in the largest systems we consider. Furthermore, in the smaller rectangular systems where layers of different densities do occur, we find that the appearance of a region of low density is always accompanied simultaneously by an excess of local ice density, with no separation in time. Our results suggest that the density differences observed in direct simulations for the two models considered here are likely due to long-range correlations between ice-like molecules and do not provide strong evidence of liquid-liquid phase separation.

  19. Study of structural and electronic properties of Mn{sub 3}O{sub 4}

    SciTech Connect

    Kaur, Ramandeep Maitra, Tulika Nautiyal, Tashi

    2014-04-24

    Using density functional theory calculations we have examined the structural and electronic properties of magnetic spinel Mn{sub 3}O{sub 4}. We have optimized the structure (both volume and c/a ratio) within GGA. Then Coulomb correlations are included in the calculations to study the electronic properties. We observe that both the band gap and magnetic moment increase with the increase in Coulomb correlation due to the increased Jahn-Teller splitting and localization of the single e{sub g} electron of Mn{sup 3+}.

  20. One- and many-electron self-interaction error in local and global hybrid functionals

    NASA Astrophysics Data System (ADS)

    Schmidt, Tobias; Kümmel, Stephan

    2016-04-01

    Electronic self-interaction poses a fundamental challenge in density-functional theory. It greatly limits, e.g., the physical interpretation of eigenvalues as electron removal energies. We here investigate whether local hybrid functionals that are designed to be free from one-electron self-interaction lead to occupied Kohn-Sham eigenvalues and orbitals that approximate photoemission observables well. We compare the local hybrid results to the ones from global hybrid functionals that only partially counteract the self-interaction, and to the results that are obtained with a Perdew-Zunger-type self-interaction correction. Furthermore, we check whether being nominally free from one-electron self-interaction translates into a reduced many-electron self-interaction error. Our findings show that this is not the case for the local hybrid functionals that we studied: In practice they are similar to global hybrids in many respects, despite being formally superior. This finding indicates that there is a conceptual difference between the Perdew-Zunger way and the local hybrid way of translating the one-electron condition to a many-electron system. We also point out and solve some difficulties that occur when using local hybrid functionals in combination with pseudopotentials.

  1. Local structure in BaTi O3-BiSc O3 dipole glasses

    NASA Astrophysics Data System (ADS)

    Levin, I.; Krayzman, V.; Woicik, J. C.; Bridges, F.; Sterbinsky, G. E.; Usher, T.-M.; Jones, J. L.; Torrejon, D.

    2016-03-01

    Local structures in cubic perovskite-type (B a0.6B i0.4) (T i0.6S c0.4) O3 solid solutions that exhibit reentrant dipole glass behavior have been studied with variable-temperature x-ray/neutron total scattering, extended x-ray absorption fine structure, and electron diffraction methods. Simultaneous fitting of these data using a reverse Monte Carlo algorithm provided instantaneous atomic configurations, which have been used to extract local displacements of the constituent species. The smaller Bi and Ti atoms exhibit probability density distributions that consist of 14 and 8 split sites, respectively. In contrast, Ba and Sc feature single-site distributions. The multisite distributions arise from large and strongly anisotropic off-center displacements of Bi and Ti. The cation displacements are correlated over a short range, with a correlation length limited by chemical disorder. The magnitudes of these displacements and their anisotropy, which are largely determined by local chemistry, change relatively insignificantly on cooling from room temperature. The structure features a nonrandom distribution of local polarization with low-dimensional polar clusters that are several unit cells in size. In situ measurements of atomic pair-distribution function under applied electric field were used to study field-induced changes in the local structure; however, no significant effects besides lattice expansion in the direction of the field could be observed up to electric-field values of 4 kV m m-1 .

  2. Electronic structure of proteins and DNA: solid-state aspects.

    PubMed

    Ladik, J J

    1978-01-01

    The generalization of the Hartree-Fock method to periodic systems (polymers or crystals) using a linear combination of atomic orbitals (LCAO) makes it possible to calculate ab initio self-consistent-field LCAO band structures of periodic protein and DNA models. The results obtained for polyglycine, polyalanine, and for the mixed poly(Gly-Ala) periodic chain, as well as for the four homopolynucleotides, are presented. The correction of these band structures for excitonic effects (in the excited state) and for long-range correlation effects is shown also. Furthermore, it is outlined how the short-range correlation in insulator biopolymers and correlation effects in proteins with a partially filled valence band (for instance, due to charge transfer) can be calculated. The Coherent Potential Approximation is outlined and its possible application to aperiodic proteins and DNA is pointed out. Finally the effect of an electron acceptor on proteins or of a chemical carcinogen bound to DNA is discussed as a local perturbation of the band structures of these systems on the basis of the self-consistent resolvent method. PMID:259504

  3. Electronic band structure and photoemission: A review and projection

    SciTech Connect

    Falicov, L.M.

    1987-09-01

    A brief review of electronic-structure calculations in solids, as a means of interpreting photoemission spectra, is presented. The calculations are, in general, of three types: ordinary one-electron-like band structures, which apply to bulk solids and are the basis of all other calculations; surface modified calculations, which take into account, self-consistently if at all possible, the presence of a vacuum-solid interface and of the electronic modifications caused thereby; and many-body calculations, which go beyond average-field approximations and consider dynamic rearrangement effects caused by electron-electron correlations during the photoemission process. 44 refs.

  4. Spatial and electron structure of substituted gold clusters

    NASA Astrophysics Data System (ADS)

    Yarzhemsky, V. G.; Kazaryan, M. A.; Bulychev, N. A.; Dyakov, Y. A.; Kosheleva, O. K.; Chen, C. H.

    2015-12-01

    The structure of intermetallic clusters Au12M (M=Hf, Ta, W, Re, Os) and features of their interaction with electron donors and acceptor atoms, i.e. H and F, were investigated making use computer calculation based of density functional theory. In was found that metal clusters with effective electron number equal to 18 have more symmetrical shape then that with a number of electrons differing from 18. The interaction of gold nanoparticles with silica was modeled by attachment of SiO4H groups and the connection of the electronic structure with electronic transitions in spaser is discussed.

  5. Electronic Resources in a Next-Generation Catalog: The Case of WorldCat Local

    ERIC Educational Resources Information Center

    Shadle, Steve

    2009-01-01

    In April 2007, the University of Washington Libraries debuted WorldCat Local (WCL), a localized version of the WorldCat database that interoperates with a library's integrated library system and fulfillment services to provide a single-search interface for a library's physical and electronic content. This brief will describe how WCL incorporates a…

  6. Interlibrary Service Requests for Locally and Electronically Available Items: Patterns of Use, Users, and Canceled Requests

    ERIC Educational Resources Information Center

    Page, Jessica R.; Kuehn, Jennifer

    2009-01-01

    As the use of the Ohio State University Libraries interlibrary services has increased, there have been more requests to borrow items that are already available to patrons locally, often in electronic format. Patterns relating to why patrons could not find locally available materials were identified in the record of canceled interlibrary requests…

  7. Strong impact of lattice vibrations on electronic and magnetic properties of paramagnetic Fe revealed by disordered local moments molecular dynamics

    NASA Astrophysics Data System (ADS)

    Alling, B.; Körmann, F.; Grabowski, B.; Glensk, A.; Abrikosov, I. A.; Neugebauer, J.

    2016-06-01

    We study the impact of lattice vibrations on magnetic and electronic properties of paramagnetic bcc and fcc iron at finite temperature, employing the disordered local moments molecular dynamics (DLM-MD) method. Vibrations strongly affect the distribution of local magnetic moments at finite temperature, which in turn correlates with the local atomic volumes. Without the explicit consideration of atomic vibrations, the mean local magnetic moment and mean field derived magnetic entropy of paramagnetic bcc Fe are larger compared to paramagnetic fcc Fe, which would indicate that the magnetic contribution stabilizes the bcc phase at high temperatures. In the present study we show that this assumption is not valid when the coupling between vibrations and magnetism is taken into account. At the γ -δ transition temperature (1662 K), the lattice distortions cause very similar magnetic moments of both bcc and fcc structures and hence magnetic entropy contributions. This finding can be traced back to the electronic densities of states, which also become increasingly similar between bcc and fcc Fe with increasing temperature. Given the sensitive interplay of the different physical excitation mechanisms, our results illustrate the need for an explicit consideration of vibrational disorder and its impact on electronic and magnetic properties to understand paramagnetic Fe. Furthermore, they suggest that at the γ -δ transition temperature electronic and magnetic contributions to the Gibbs free energy are extremely similar in bcc and fcc Fe.

  8. Monaural sound localization based on structure-induced acoustic resonance.

    PubMed

    Kim, Keonwook; Kim, Youngwoong

    2015-01-01

    A physical structure such as a cylindrical pipe controls the propagated sound spectrum in a predictable way that can be used to localize the sound source. This paper designs a monaural sound localization system based on multiple pyramidal horns around a single microphone. The acoustic resonance within the horn provides a periodicity in the spectral domain known as the fundamental frequency which is inversely proportional to the radial horn length. Once the system accurately estimates the fundamental frequency, the horn length and corresponding angle can be derived by the relationship. The modified Cepstrum algorithm is employed to evaluate the fundamental frequency. In an anechoic chamber, localization experiments over azimuthal configuration show that up to 61% of the proper signal is recognized correctly with 30% misfire. With a speculated detection threshold, the system estimates direction 52% in positive-to-positive and 34% in negative-to-positive decision rate, on average. PMID:25668214

  9. Monaural Sound Localization Based on Structure-Induced Acoustic Resonance

    PubMed Central

    Kim, Keonwook; Kim, Youngwoong

    2015-01-01

    A physical structure such as a cylindrical pipe controls the propagated sound spectrum in a predictable way that can be used to localize the sound source. This paper designs a monaural sound localization system based on multiple pyramidal horns around a single microphone. The acoustic resonance within the horn provides a periodicity in the spectral domain known as the fundamental frequency which is inversely proportional to the radial horn length. Once the system accurately estimates the fundamental frequency, the horn length and corresponding angle can be derived by the relationship. The modified Cepstrum algorithm is employed to evaluate the fundamental frequency. In an anechoic chamber, localization experiments over azimuthal configuration show that up to 61% of the proper signal is recognized correctly with 30% misfire. With a speculated detection threshold, the system estimates direction 52% in positive-to-positive and 34% in negative-to-positive decision rate, on average. PMID:25668214

  10. Effect of potassium doping on electronic structure and thermoelectric properties of topological crystalline insulator

    NASA Astrophysics Data System (ADS)

    Roychowdhury, Subhajit; Sandhya Shenoy, U.; Waghmare, Umesh V.; Biswas, Kanishka

    2016-05-01

    Topological crystalline insulator (TCI), Pb0.6Sn0.4Te, exhibits metallic surface states protected by crystal mirror symmetry with negligibly small band gap. Enhancement of its thermoelectric performances needs tuning of its electronic structure particularly through engineering of its band gap. While physical perturbations tune the electronic structure of TCI by breaking of the crystal mirror symmetry, chemical means such as doping have been more attractive recently as they result in better thermoelectric performance in TCIs. Here, we demonstrate that K doping in TCI, Pb0.6Sn0.4Te, breaks the crystal mirror symmetry locally and widens electronic band gap, which is confirmed by direct electronic absorption spectroscopy and electronic structure calculations. K doping in Pb0.6Sn0.4Te increases p-type carrier concentration and suppresses the bipolar conduction via widening a band gap, which collectively boosts the thermoelectric figure of merit (ZT) to 1 at 708 K.

  11. A local average distance descriptor for flexible protein structure comparison

    PubMed Central

    2014-01-01

    Background Protein structures are flexible and often show conformational changes upon binding to other molecules to exert biological functions. As protein structures correlate with characteristic functions, structure comparison allows classification and prediction of proteins of undefined functions. However, most comparison methods treat proteins as rigid bodies and cannot retrieve similarities of proteins with large conformational changes effectively. Results In this paper, we propose a novel descriptor, local average distance (LAD), based on either the geodesic distances (GDs) or Euclidean distances (EDs) for pairwise flexible protein structure comparison. The proposed method was compared with 7 structural alignment methods and 7 shape descriptors on two datasets comprising hinge bending motions from the MolMovDB, and the results have shown that our method outperformed all other methods regarding retrieving similar structures in terms of precision-recall curve, retrieval success rate, R-precision, mean average precision and F1-measure. Conclusions Both ED- and GD-based LAD descriptors are effective to search deformed structures and overcome the problems of self-connection caused by a large bending motion. We have also demonstrated that the ED-based LAD is more robust than the GD-based descriptor. The proposed algorithm provides an alternative approach for blasting structure database, discovering previously unknown conformational relationships, and reorganizing protein structure classification. PMID:24694083

  12. Localization of carriers in a one-dimensional electron system over liquid helium

    NASA Astrophysics Data System (ADS)

    Gladchenko, S. P.; Kovdrya, Yu. Z.; Nikolaenko, V. A.

    2000-07-01

    The mobility of carriers in a one-dimensional electron system over liquid helium has been measured at the temperature 0.5-1.7 K and for different values of linear electron density. Profiled nylon substrates with some quantity of charge deposited were used for the realization of a one-dimensional electron system. It is shown that electron mobility is dependent on the quantity of the charge on a substrate. Effects observed are explained by the localization of electrons moving in the random potential created by the substrates charge. It is supposed that at low temperatures the movement of carriers is determined by quantum effects.

  13. Weak localization and electron–electron interactions in few layer black phosphorus devices

    NASA Astrophysics Data System (ADS)

    Shi, Yanmeng; Gillgren, Nathaniel; Espiritu, Timothy; Tran, Son; Yang, Jiawei; Watanabe, Kenji; Taniguchi, Takahashi; Lau, Chun Ning

    2016-09-01

    Few layer phosphorene (FLP) devices are extensively studied due to their unique electronic properties and potential applications on nano-electronics. Here we present magnetotransport studies which reveal electron–electron interactions as the dominant scattering mechanism in hexagonal boron nitride-encapsulated FLP devices. From weak localization measurements, we estimate the electron dephasing length to be 30 to 100 nm at low temperatures, which exhibits a strong dependence on carrier density n and a power-law dependence on temperature (∼T ‑0.4). These results establish that the dominant scattering mechanism in FLP is electron–electron interactions.

  14. Electronic structure of cuprate superconductors in a full charge-spin recombination scheme

    NASA Astrophysics Data System (ADS)

    Feng, Shiping; Kuang, Lülin; Zhao, Huaisong

    2015-10-01

    A long-standing unsolved problem is how a microscopic theory of superconductivity in cuprate superconductors based on the charge-spin separation can produce a large electron Fermi surface. Within the framework of the kinetic-energy driven superconducting mechanism, a full charge-spin recombination scheme is developed to fully recombine a charge carrier and a localized spin into a electron, and then is employed to study the electronic structure of cuprate superconductors in the superconducting-state. In particular, it is shown that the underlying electron Fermi surface fulfills Luttinger's theorem, while the superconducting coherence of the low-energy quasiparticle excitations is qualitatively described by the standard d-wave Bardeen-Cooper-Schrieffer formalism. The theory also shows that the observed peak-dip-hump structure in the electron spectrum and Fermi arc behavior in the underdoped regime are mainly caused by the strong energy and momentum dependence of the electron self-energy.

  15. Earth Structure, Ice Mass Changes, and the Local Dynamic Geoid

    NASA Astrophysics Data System (ADS)

    Harig, C.; Simons, F. J.

    2014-12-01

    Spherical Slepian localization functions are a useful method for studying regional mass changes observed by satellite gravimetry. By projecting data onto a sparse basis set, the local field can be estimated more easily than with the full spherical harmonic basis. We have used this method previously to estimate the ice mass change in Greenland from GRACE data, and it can also be applied to other planetary problems such as global magnetic fields. Earth's static geoid, in contrast to the time-variable field, is in large part related to the internal density and rheological structure of the Earth. Past studies have used dynamic geoid kernels to relate this density structure and the internal deformation it induces to the surface geopotential at large scales. These now classical studies of the eighties and nineties were able to estimate the mantle's radial rheological profile, placing constraints on the ratio between upper and lower mantle viscosity. By combining these two methods, spherical Slepian localization and dynamic geoid kernels, we have created local dynamic geoid kernels which are sensitive only to density variations within an area of interest. With these kernels we can estimate the approximate local radial rheological structure that best explains the locally observed geoid on a regional basis. First-order differences of the regional mantle viscosity structure are accessible to this technique. In this contribution we present our latest, as yet unpublished results on the geographical and temporal pattern of ice mass changes in Antarctica over the past decade, and we introduce a new approach to extract regional information about the internal structure of the Earth from the static global gravity field. Both sets of results are linked in terms of the relevant physics, but also in being developed from the marriage of Slepian functions and geoid kernels. We make predictions on the utility of our approach to derive fully three-dimensional rheological Earth models, to

  16. Dynamics of Localized Structures in Systems with Broken Parity Symmetry

    NASA Astrophysics Data System (ADS)

    Javaloyes, J.; Camelin, P.; Marconi, M.; Giudici, M.

    2016-04-01

    A great variety of nonlinear dissipative systems are known to host structures having a correlation range much shorter than the size of the system. The dynamics of these localized structures (LSs) has been investigated so far in situations featuring parity symmetry. In this Letter we extend this analysis to systems lacking this property. We show that the LS drifting speed in a parameter varying landscape is not simply proportional to the parameter gradient, as found in parity preserving situations. The symmetry breaking implies a new contribution to the velocity field which is a function of the parameter value, thus leading to a new paradigm for LSs manipulation. We illustrate this general concept by studying the trajectories of the LSs found in a passively mode-locked laser operated in the localization regime. Moreover, the lack of parity affects significantly LSs interactions which are governed by asymmetrical repulsive forces.

  17. Local structure co-occurrence pattern for image retrieval

    NASA Astrophysics Data System (ADS)

    Zhang, Ke; Zhang, Fan; Lu, Jia; Lu, Yinghua; Kong, Jun; Zhang, Ming

    2016-03-01

    Image description and annotation is an active research topic in content-based image retrieval. How to utilize human visual perception is a key approach to intelligent image feature extraction and representation. This paper has proposed an image feature descriptor called the local structure co-occurrence pattern (LSCP). LSCP extracts the whole visual perception for an image by building a local binary structure, and it is represented by a color-shape co-occurrence matrix which explores the relationship of multivisual feature spaces according to visual attention mechanism. As a result, LSCP not only describes low-level visual features integrated with texture feature, color feature, and shape feature but also bridges high-level semantic comprehension. Extensive experimental results on an image retrieval task on the benchmark datasets, corel-10,000, MIT VisTex, and INRIA Holidays, have demonstrated the usefulness, effectiveness, and robustness of the proposed LSCP.

  18. Electron-beam-induced deposition and post-treatment processes to locally generate clean titanium oxide nanostructures on Si(100).

    PubMed

    Schirmer, M; Walz, M-M; Vollnhals, F; Lukasczyk, T; Sandmann, A; Chen, C; Steinrück, H-P; Marbach, H

    2011-02-25

    We have investigated the lithographic generation of TiO(x) nanostructures on Si(100) via electron-beam-induced deposition (EBID) of titanium tetraisopropoxide (TTIP) in ultra-high vacuum (UHV) by scanning electron microscopy (SEM) and local Auger electron spectroscopy (AES). In addition, the fabricated nanostructures were also characterized ex situ via atomic force microscopy (AFM) under ambient conditions. In EBID, a highly focused electron beam is used to locally decompose precursor molecules and thereby to generate a deposit. A drawback of this nanofabrication technique is the unintended deposition of material in the vicinity of the impact position of the primary electron beam due to so-called proximity effects. Herein, we present a post-treatment procedure to deplete the unintended deposits by moderate sputtering after the deposition process. Moreover, we were able to observe the formation of pure titanium oxide nanocrystals (<100 nm) in situ upon heating the sample in a well-defined oxygen atmosphere. While the nanocrystal growth for the as-deposited structures also occurs in the surroundings of the irradiated area due to proximity effects, it is limited to the pre-defined regions, if the sample was sputtered before heating the sample under oxygen atmosphere. The described two-step post-treatment procedure after EBID presents a new pathway for the fabrication of clean localized nanostructures. PMID:21242619

  19. Electron-beam-induced deposition and post-treatment processes to locally generate clean titanium oxide nanostructures on Si(100)

    NASA Astrophysics Data System (ADS)

    Schirmer, M.; Walz, M.-M.; Vollnhals, F.; Lukasczyk, T.; Sandmann, A.; Chen, C.; Steinrück, H.-P.; Marbach, H.

    2011-02-01

    We have investigated the lithographic generation of TiOx nanostructures on Si(100) via electron-beam-induced deposition (EBID) of titanium tetraisopropoxide (TTIP) in ultra-high vacuum (UHV) by scanning electron microscopy (SEM) and local Auger electron spectroscopy (AES). In addition, the fabricated nanostructures were also characterized ex situ via atomic force microscopy (AFM) under ambient conditions. In EBID, a highly focused electron beam is used to locally decompose precursor molecules and thereby to generate a deposit. A drawback of this nanofabrication technique is the unintended deposition of material in the vicinity of the impact position of the primary electron beam due to so-called proximity effects. Herein, we present a post-treatment procedure to deplete the unintended deposits by moderate sputtering after the deposition process. Moreover, we were able to observe the formation of pure titanium oxide nanocrystals (<100 nm) in situ upon heating the sample in a well-defined oxygen atmosphere. While the nanocrystal growth for the as-deposited structures also occurs in the surroundings of the irradiated area due to proximity effects, it is limited to the pre-defined regions, if the sample was sputtered before heating the sample under oxygen atmosphere. The described two-step post-treatment procedure after EBID presents a new pathway for the fabrication of clean localized nanostructures.

  20. Dynamic modulation of electronic properties of graphene by localized carbon doping using focused electron beam induced deposition.

    PubMed

    Kim, S; Russell, M; Henry, M; Kim, S S; Naik, R R; Voevodin, A A; Jang, S S; Tsukruk, V V; Fedorov, A G

    2015-09-28

    We report on the first demonstration of controllable carbon doping of graphene to engineer local electronic properties of a graphene conduction channel using focused electron beam induced deposition (FEBID). Electrical measurements indicate that an "n-p-n" junction on graphene conduction channel is formed by partial carbon deposition near the source and drain metal contacts by low energy (<50 eV) secondary electrons due to inelastic collisions of long range backscattered primary electrons generated from a low dose of high energy (25 keV) electron beam (1 × 10(18) e(-) per cm(2)). Detailed AFM imaging provides direct evidence of the new mechanism responsible for dynamic evolution of the locally varying graphene doping. The FEBID carbon atoms, which are physisorbed and weakly bound to graphene, diffuse towards the middle of graphene conduction channel due to their surface chemical potential gradient, resulting in negative shift of Dirac voltage. Increasing a primary electron dose to 1 × 10(19) e(-) per cm(2) results in a significant increase of carbon deposition, such that it covers the entire graphene conduction channel at high surface density, leading to n-doping of graphene channel. Collectively, these findings establish a unique capability of FEBID technique to dynamically modulate the doping state of graphene, thus enabling a new route to resist-free, "direct-write" functional patterning of graphene-based electronic devices with potential for on-demand re-configurability. PMID:26302897

  1. Local and near surface structure from diffraction (Preface)

    SciTech Connect

    Barabash, Rozaliya; Ice, Gene E

    2010-01-01

    This special topic of Materials Science and Engineering A highlights novel applications of X-ray and neutron diffraction for the analysis of a range of materials, including conventional and nanostructured materials, thin films, bio-inspired materials, and superalloys. The development of ultra-brilliant synchrotron X-ray sources and recent advances in neutron diffraction provide important new opportunities for the analysis of local and near surface material structures at multiple length scales.

  2. Atomic structure and electronic properties of Ni3Al(111) and (011) surfaces

    NASA Astrophysics Data System (ADS)

    Jurczyszyn, L.; Krupski, A.; Degen, S.; Pieczyrak, B.; Kralj, M.; Becker, C.; Wandelt, K.

    2007-07-01

    We present results of theoretical studies of the structural and electronic properties of (111) and (011) surfaces of paramagnetic Ni3Al alloy. Atomic and electronic structures of these surfaces have been obtained from the density-functional calculations performed with the use of plane wave basis set. Our ab initio calculations show that for all considered surfaces, the topmost Al atoms are located above Ni atoms, and the structural parameters of relaxed surface systems well correspond to experimental data provided by earlier low-energy electron-diffraction measurements. The details of the calculated electronic structure of Ni3Al(111) in the vicinity of the Fermi level were compared with the results of scanning tunneling spectroscopy (STS) measurements which we have performed for this system, and a good agreement has been found between the calculated local-density-of-states distributions and the shape of obtained STS spectra.

  3. Electronic structure of BaO/W cathode surfaces

    NASA Technical Reports Server (NTRS)

    Muller, Wolfgang

    1989-01-01

    The local electronic structure of the emissive layer of barium dispenser thermionic cathodes is investigated theoretically using the relativistic scattered-wave approach. The interaction of Ba and O with W, Os, and W-Os alloy surfaces is studied with atomic clusters modeling different absorption environments representative of B- and M-type cathodes. Ba is found to be strongly oxidized, while O and the metal substrate are in a reduced chemical state. The presence of O enhances the surface dipole and Ba binding energy relative to Ba on W. Model results for W-Os alloy substrates show only relatively small changes in Ba and O for identical geometries, but very large charge redistributions inside the substrate, which are attributed to the electronegativity difference between Os and W. If Os is present in the surface layer, the charge transfer from Ba to the substrate and the Ba binding energy increase relative to W. Explanations are offered for the improved electron emission from alloy surfaces and the different emission enhancement for different alloy substrates.

  4. Electronic and magnetic structure of the Cr(001) surface.

    PubMed

    Habibi, P; Barreteau, C; Smogunov, A

    2013-04-10

    Density functional theory (DFT) calculations are carried out to study the electronic and magnetic structure of the (001) surface of chromium. Our aim is to identify and characterize the most prominent electronic surface states and make the connection with the main experimental results. We show that a low dispersive minority spin surface state at the center of the surface Brillouin zone plays a crucial role. This surface state of Δ1 symmetry at 0.58 eV above the Fermi level exhibits a predominantly dz(2) as well as pz orbital character. Local density of states (LDOS) analysis in the vacuum above the surface shows that the sharp feature originating from this surface state persists far away above the surface because of the slow decay rate of the pz wavefunction. Finally, by artificially lowering the surface magnetic moment [Formula: see text] on the outermost surface layer we find excellent agreement with experiments for [Formula: see text]. In addition, we propose that some extra spin polarized scanning tunneling spectroscopy (SP-STS) experiments should be made at smaller tip-surface distances to reveal additional features originating from the majority spin dz(2) surface state. PMID:23478357

  5. Current driven due to localized electron power deposition in DIII-D

    SciTech Connect

    Harvey, R.W.; Lin-Liu, Y.R.; Luce, T.C.; Prater, R.; Sauter, O.; Smirnov, A.P.

    1999-05-01

    Due to spatial localization of electron cyclotron wave injection in DIII-D, electrons heated in an off-axis region must toroidally transit the tokamak 25--50 times before re-entering the heating region. This distance is of the order of the mean free path. The effect of such RF localization is simulated with a time-dependent Fokker-Planck code which is 2D-in-velocity, 1D-in-space-along-B, and periodic in space. An effective parallel electric field arises to maintain continuity of the driven current. Somewhat surprisingly, the localized current drive efficiency remains equal to that for a uniform medium.

  6. Local spin torque induced by electron electric dipole moment in the Ybf molecule

    NASA Astrophysics Data System (ADS)

    Fukuda, Masahiro; Senami, Masato; Ogiso, Yoji; Tachibana, Akitomo

    2014-10-01

    In this study, we show the modification of the equation of motion of the electronic spin, which is derived by the quantum electron spin vorticity principle, by the effect of the electron electric dipole moment (EDM). To investigate the new contribution to spin torque by EDM, using first principle calculations, we visualize distributions of the local spin angular momentum density and local spin torque density of the YbF molecule on which the static electric field and magnetic field are applied at t = 0.

  7. Local spin torque induced by electron electric dipole moment in the YbF molecule

    SciTech Connect

    Fukuda, Masahiro; Senami, Masato; Ogiso, Yoji; Tachibana, Akitomo

    2014-10-06

    In this study, we show the modification of the equation of motion of the electronic spin, which is derived by the quantum electron spin vorticity principle, by the effect of the electron electric dipole moment (EDM). To investigate the new contribution to spin torque by EDM, using first principle calculations, we visualize distributions of the local spin angular momentum density and local spin torque density of the YbF molecule on which the static electric field and magnetic field are applied at t = 0.

  8. Local atomic structure inheritance in Ag{sub 50}Sn{sub 50} melt

    SciTech Connect

    Bai, Yanwen; Bian, Xiufang Qin, Jingyu; Hu, Lina; Yang, Jianfei; Zhang, Kai; Zhao, Xiaolin; Yang, Chuncheng; Zhang, Shuo; Huang, Yuying

    2014-01-28

    Local structure inheritance signatures were observed during the alloying process of the Ag{sub 50}Sn{sub 50} melt, using high-temperature X-ray diffraction and ab initio molecular dynamics simulations. The coordination number N{sub m} around Ag atom is similar in the alloy and in pure Ag melts (N{sub m} ∼ 10), while, during the alloying process, the local structure around Sn atoms rearranges. Sn-Sn covalent bonds were substituted by Ag-Sn chemical bonds, and the total coordination number around Sn increases by about 70% as compared with those in the pure Sn melt. Changes in the electronic structure of the alloy have been studied by Ag and Sn K-edge X-ray absorption spectroscopy, as well as by calculations of the partial density of states. We propose that a leading mechanism for local structure inheritance in Ag{sub 50}Sn{sub 50} is due to s-p dehybridization of Sn and to the interplay between Sn-s and Ag-d electrons.

  9. Electronic structure of CoPt based systems: from bulk to nanoalloys

    NASA Astrophysics Data System (ADS)

    Zosiak, L.; Goyhenex, C.; Kozubski, R.; Tréglia, G.

    2015-11-01

    An accurate description of the local electronic structure is necessary for guiding the design of materials with targeted properties in a controlled way. For complex materials like nanoalloys, self-consistent tight-binding calculations should be a good alternative to ab initio methods, for handling the most complex and large systems (hundreds to thousands of atoms), provided that these parameterized method is well founded from ab initio ones that they intend to replace. Ab initio calculations (density functional theory) enabled us to derive rules for charge distribution as a function of structural change and alloying effects in Co and Pt based systems, from bulk to nanoalloys. A general local neutrality rule per site, orbital and species was found. Based on it, self-consistent tight-binding calculations could be implemented and applied to CoPt nanoalloys. A very good agreement is obtained between tight-binding and DFT calculations in terms of local electronic structure.

  10. In situ KPFM imaging of local photovoltaic characteristics of structured organic photovoltaic devices.

    PubMed

    Watanabe, Satoshi; Fukuchi, Yasumasa; Fukasawa, Masako; Sassa, Takafumi; Kimoto, Atsushi; Tajima, Yusuke; Uchiyama, Masanobu; Yamashita, Takashi; Matsumoto, Mutsuyoshi; Aoyama, Tetsuya

    2014-02-12

    Here, we discuss the local photovoltaic characteristics of a structured bulk heterojunction, organic photovoltaic devices fabricated with a liquid carbazole, and a fullerene derivative based on analysis by scanning kelvin probe force microscopy (KPFM). Periodic photopolymerization induced by an interference pattern from two laser beams formed surface relief gratings (SRG) in the structured films. The surface potential distribution in the SRGs indicates the formation of donor and acceptor spatial distribution. Under illumination, the surface potential reversibly changed because of the generation of fullerene anions and hole transport from the films to substrates, which indicates that we successfully imaged the local photovoltaic characteristics of the structured photovoltaic devices. Using atomic force microscopy, we confirmed the formation of the SRG because of the material migration to the photopolymerized region of the films, which was induced by light exposure through photomasks. The structuring technique allows for the direct fabrication and the control of donor and acceptor spatial distribution in organic photonic and electronic devices with minimized material consumption. This in situ KPFM technique is indispensable to the fabrication of nanoscale electron donor and electron acceptor spatial distribution in the devices. PMID:24450927

  11. Atomistic modeling of electronic structure and transport in disordered nanostructures

    NASA Astrophysics Data System (ADS)

    Kharche, Neerav

    As the Si-CMOS technology approaches the end of the International Technology Roadmap for Semiconductors (ITRS), the semiconductor industry faces a formidable challenge to continue the transistor scaling according to Moore's law. To continue the scaling of classical devices, alternative channel materials such as SiGe, carbon nanotubes, nanowires, and III-V based materials are being investigated along with novel 3D device geometries. Researchers are also investigating radically new quantum computing devices, which are expected to perform calculations faster than the existing classical Si-CMOS based structures. Atomic scale disorders such as interface roughness, alloy randomness, non-uniform strain, and dopant fluctuations are routinely present in the experimental realization of such devices. These disorders now play an increasingly important role in determining the electronic structure and transport properties as device sizes enter the nanometer regime. This work employs the atomistic tight-binding technique, which is ideally suited for modeling systems with local disorders on an atomic scale. High-precision multi-million atom electronic structure calculations of (111) Si surface quantum wells and (100) SiGe/Si/SiGe heterostructure quantum wells are performed to investigate the modulation of valley splitting induced by atomic scale disorders. The calculations presented here resolve the existing discrepancies between theoretically predicted and experimentally measured valley splitting, which is an important design parameter in quantum computing devices. Supercell calculations and the zone-unfolding method are used to compute the bandstructures of inhomogeneous nanowires made of AlGaAs and SiGe and their connection with the transmission coefficients computed using non-equilibrium Green's function method is established. A unified picture of alloy nanowires emerges, in which the nanodevice (transmission) and nanomaterials (bandstructure) viewpoints complement each other

  12. Ab-initio study of structural, mechanical and electronic properties of functionalized carbon nanotubes

    SciTech Connect

    Milowska, Karolina Z.; Birowska, Magdalena; Majewski, Jacek A.

    2013-12-04

    We present exemplary results of extensive studies of structural, mechanical and electronic properties of covalent functionalization of carbon nanotubes (CNTs). We report new results for metallic (9,0), and semiconducting (10,0) single-wall carbon nanotubes (CNT) functionalized with -COOH, -OH, and both groups with concentration up to 12.5%. Our studies are performed in the framework of the density functional theory (DFT). We discuss here the stability, local and global changes in structure, elastic moduli (Young's, Shear, and Bulk), electronic structure and resulting band gaps, as a function of the density of the adsorbed molecules.

  13. Analyzing the sequence-structure relationship of a library of local structural prototypes.

    PubMed

    Benros, Cristina; de Brevern, Alexandre G; Hazout, Serge

    2009-01-21

    We present a thorough analysis of the relation between amino acid sequence and local three-dimensional structure in proteins. A library of overlapping local structural prototypes was built using an unsupervised clustering approach called "hybrid protein model" (HPM). The HPM carries out a multiple structural alignment of local folds from a non-redundant protein structure databank encoded into a structural alphabet composed of 16 protein blocks (PBs). Following previous research focusing on the HPM protocol, we have considered gaps in the local structure prototype. This methodology allows to have variable length fragments. Hence, 120 local structure prototypes were obtained. Twenty-five percent of the protein fragments learnt by HPM had gaps. An investigation of tight turns suggested that they are mainly derived from three PB series with precise locations in the HPM. The amino acid information content of the whole conformational classes was tackled by multivariate methods, e.g., canonical correlation analysis. It points out the presence of seven amino acid equivalence classes showing high propensities for preferential local structures. In the same way, definition of "contrast factors" based on sequence-structure properties underline the specificity of certain structural prototypes, e.g., the dependence of Gly or Asn-rich turns to a limited number of PBs, or, the opposition between Pro-rich coils to those enriched in Ser, Thr, Asn and Glu. These results are so useful to analyze the sequence-structure relationships, but could also be used to improve fragment-based method for protein structure prediction from sequence. PMID:18977232

  14. Electronic-structure calculations of praseodymium metal by means of modified density-functional theory

    SciTech Connect

    Svane, A.; Trygg, J.; Johansson, B.; Eriksson, O. |

    1997-09-01

    Electronic-structure calculations of elemental praseodymium are presented. Several approximations are used to describe the Pr f electrons. It is found that the low-pressure, trivalent phase is well described using either the self-interaction corrected (SIC) local-spin-density (LSD) approximation or the generalized-gradient approximation (GGA) with spin and orbital polarization (OP). In the SIC-LSD approach the Pr f electrons are treated explicitly as localized with a localization energy given by the self-interaction of the f orbital. In the GGA+OP scheme the f-electron localization is described by the onset of spin and orbital polarization, the energetics of which is described by spin-moment formation energy and a term proportional to the total orbital moment, L{sub z}{sup 2}. The high-pressure phase is well described with the f electrons treated as band electrons, in either the LSD or the GGA approximations, of which the latter describes more accurately the experimental equation of state. The calculated pressure of the transition from localized to delocalized behavior is 280 kbar in the SIC-LSD approximation and 156 kbar in the GGA+OP approach, both comparing favorably with the experimentally observed transition pressure of 210 kbar. {copyright} {ital 1997} {ital The American Physical Society}

  15. Examination of the local structure in composite and lowdimensional semiconductor by X-ray Absorption Spectroscopy

    SciTech Connect

    Lawniczak-Jablonska, K.; Demchenko, I.N.; Piskorska, E.; Wolska,A.; Talik, E.; Zakharov, D.N.; Liliental-Weber, Z.

    2006-09-25

    X-ray absorption methods have been successfully used to obtain quantitative information about local atomic composition of two different materials. X-ray Absorption Near Edge Structure analysis and X-Ray Photoelectron Spectroscopy allowed us to determine seven chemical compounds and their concentrations in c-BN composite. Use of Extended X-ray Absorption Fine Structure in combination with Transmission Electron Microscopy enabled us to determine the composition and size of buried Ge quantum dots. It was found that the quantum dots consisted out of pure Ge core covered by 1-2 monolayers of a layer rich in Si.

  16. Trends in the properties and structures of the simple metals from a universal local pseudopotential

    NASA Astrophysics Data System (ADS)

    Nogueira, Fernando; Fiolhais, Carlos; Perdew, John P.

    1999-01-01

    The properties of simple metals are fixed primarily by the equilibrium average valence-electron density parameter rs, and secondarily by the valence z. The simplest level of theory that can account quantitatively for these trends invokes a ``universal'' local electron-ion pseudopotential, defined for each pair (rs,z) and treated as a second-order perturbation. We construct this pseudopotential from two conditions: (1) The total energy should minimize at the equilibrium Wigner-Seitz radius z1/3rs. (2) The bulk modulus should equal the realistic rs-dependent prediction of the stabilized jellium model with effective valence z*=1. These conditions can be satisfied by an analytic local pseudopotential depending upon two parameters other than z; we show that the choice of the two-parameter form (evanescent core vs Heine-Abarenkov) is not important. Our universal local pseudopotential is applied to calculate realistic bulk binding energies, pressure derivatives of bulk moduli, Voigt shear moduli, and interstitial electron numbers, revealing their trends as functions of rs and z. Equilibrium crystal structures are mapped in the rs-z plane, where the Hume-Rothery rules for substitutional alloys are manifest. The effect of pressure on crystal structure is also examined.

  17. Local Structure of Cerium in Aluminophosphate and Silicophosphate Glasses

    SciTech Connect

    J Rygel; Y Chen; C Pantano; T Shibata; J Du; L Kokou; R Woodman; J Belcher

    2011-12-31

    The local structure of cerium in two systematic compositional series of glasses, nominally CeP{sub 3}O{sub 9}-AlP{sub 3}O{sub 9} and CeP{sub 3}O{sub 9}-SiP{sub 2}O{sub 7}, was interrogated using X-ray photoelectron spectroscopy (XPS) and X-ray absorption fine structure (XAFS) spectroscopy. XPS revealed that, for glasses melted in air, {>=}95% of cerium ions are Ce{sup 3+}. This was independently confirmed using X-ray absorption near edge spectroscopy (XANES). Ce K-edge extended X-ray absorption fine structure (EXAFS) has been used to determine the local structure of Ce{sup 3+}. Near the metaphosphate composition, cerium was found to have an average cerium coordination number of {approx}7.0 and an average cerium-oxygen bond length of 2.41 {angstrom}. The average cerium coordination number and average cerium-oxygen bond distance were found to increase with decreasing cerium concentration in both compositional series. Rare-earth clustering is suggested based on numerical calculations for glasses containing {>=}14 and {>=}15 mol% Ce{sub 2}O{sub 3} for the aluminophosphate and silicophosphate series, respectively.

  18. Local Structure of Cerium in Aluminophosphate and Silicophosphate Glasses

    SciTech Connect

    Rygel, Jennifer L.; Chen, Yongsheng; Pantano, Carlo G.; Shibata, Tomohiro; Du, Jincheng; Kokou, Leopold; Woodman, Robert; Belcher, James

    2011-09-20

    The local structure of cerium in two systematic compositional series of glasses, nominally CeP{sub 3}O{sub 9}-AlP{sub 3}O{sub 9} and CeP{sub 3}O{sub 9}-SiP{sub 2}O{sub 7}, was interrogated using X-ray photoelectron spectroscopy (XPS) and X-ray absorption fine structure (XAFS) spectroscopy. XPS revealed that, for glasses melted in air, {>=}95% of cerium ions are Ce{sup 3+}. This was independently confirmed using X-ray absorption near edge spectroscopy (XANES). Ce K-edge extended X-ray absorption fine structure (EXAFS) has been used to determine the local structure of Ce{sup 3+}. Near the metaphosphate composition, cerium was found to have an average cerium coordination number of {approx}7.0 and an average cerium-oxygen bond length of 2.41 {angstrom}. The average cerium coordination number and average cerium-oxygen bond distance were found to increase with decreasing cerium concentration in both compositional series. Rare-earth clustering is suggested based on numerical calculations for glasses containing {>=}14 and {>=}15 mol% Ce{sub 2}O{sub 3} for the aluminophosphate and silicophosphate series, respectively.

  19. Assessing the local identifiability of probabilistic knowledge structures.

    PubMed

    Stefanutti, Luca; Heller, Jürgen; Anselmi, Pasquale; Robusto, Egidio

    2012-12-01

    Given a collection Q of problems, in knowledge space theory Doignon & Falmagne, (International Journal of Man-Machine Studies 23:175-196, 1985) the knowledge state of a student is the collection K ⊆ Q of all problems that this student is capable of solving. A knowledge structure is a pair (Q, ), where is a collection of knowledge states that contains at least the empty set and Q. A probabilistic knowledge structure (PKS) is a knowledge structure (Q, , π), where π is a probability distribution on the knowledge states. The PKS that has received the most attention is the basic local independence model BLIM; Falmagne & Doignon, (British Journal of Mathematical and Statistical Psychology 41:1-23, 1988a, Journal of Mathematical Psychology 32:232-258, 1988b). To the best of our knowledge, systematic investigations in the literature concerning the identifiability of the BLIM are totally missing. Based on the theoretical work of Bamber and van Santen (Journal of Mathematical Psychology 29:443-473, 1985), the present article is aimed to present a method and a corresponding computerized procedure for assessing the local identifiability of the BLIM, which is applicable to any finite knowledge structure of moderate size. PMID:22588988

  20. Imaging doped silicon test structures using low energy electron microscopy.

    SciTech Connect

    Nakakura, Craig Yoshimi; Anderson, Meredith Lynn; Kellogg, Gary Lee

    2010-01-01

    This document is the final SAND Report for the LDRD Project 105877 - 'Novel Diagnostic for Advanced Measurements of Semiconductor Devices Exposed to Adverse Environments' - funded through the Nanoscience to Microsystems investment area. Along with the continuous decrease in the feature size of semiconductor device structures comes a growing need for inspection tools with high spatial resolution and high sample throughput. Ideally, such tools should be able to characterize both the surface morphology and local conductivity associated with the structures. The imaging capabilities and wide availability of scanning electron microscopes (SEMs) make them an obvious choice for imaging device structures. Dopant contrast from pn junctions using secondary electrons in the SEM was first reported in 1967 and more recently starting in the mid-1990s. However, the serial acquisition process associated with scanning techniques places limits on the sample throughput. Significantly improved throughput is possible with the use of a parallel imaging scheme such as that found in photoelectron emission microscopy (PEEM) and low energy electron microscopy (LEEM). The application of PEEM and LEEM to device structures relies on contrast mechanisms that distinguish differences in dopant type and concentration. Interestingly, one of the first applications of PEEM was a study of the doping of semiconductors, which showed that the PEEM contrast was very sensitive to the doping level and that dopant concentrations as low as 10{sup 16} cm{sup -3} could be detected. More recent PEEM investigations of Schottky contacts were reported in the late 1990s by Giesen et al., followed by a series of papers in the early 2000s addressing doping contrast in PEEM by Ballarotto and co-workers and Frank and co-workers. In contrast to PEEM, comparatively little has been done to identify contrast mechanisms and assess the capabilities of LEEM for imaging semiconductor device strictures. The one exception is the

  1. Local structure and spin transition in Fe2O3 hematite at high pressure

    NASA Astrophysics Data System (ADS)

    Sanson, Andrea; Kantor, Innokenty; Cerantola, Valerio; Irifune, Tetsuo; Carnera, Alberto; Pascarelli, Sakura

    2016-07-01

    The pressure evolution of the local structure of Fe2O3 hematite has been determined by extended x-ray absorption fine structure up to ˜79 GPa. Below the phase-transition pressure at ˜50 GPa, no increasing of FeO6 octahedra distortion is observed as pressure is applied. Above the phase transition, an abrupt decrease of the nearest-neighbor Fe-O distance is observed concomitantly with a strong reduction in the FeO6 distortion. This information on the local structure, used as a test-bench for the different high-pressure forms proposed in the literature, suggests that the orthorhombic structure with space group A b a 2 , recently proposed by Bykova et al. [Nat. Commun. 7, 10661 (2016), 10.1038/ncomms10661], is the most probable, but puts into question the presence of the P 21 /n form in the pressure range 54-67 GPa. Finally, the crossover from Fe high-spin to low-spin states with pressure increase has been monitored from the pre-edge region of the Fe K -edge absorption spectra. Its "simultaneous" comparison with the local structural changes allows us to conclude that it is the electronic transition that drives the structural transition and not vice versa.

  2. Localized conductive patterning via focused electron beam reduction of graphene oxide

    NASA Astrophysics Data System (ADS)

    Kim, Songkil; Kulkarni, Dhaval D.; Henry, Mathias; Zackowski, Paul; Jang, Seung Soon; Tsukruk, Vladimir V.; Fedorov, Andrei G.

    2015-03-01

    We report on a method for "direct-write" conductive patterning via reduction of graphene oxide (GO) sheets using focused electron beam induced deposition (FEBID) of carbon. FEBID treatment of the intrinsically dielectric graphene oxide between two metal terminals opens up the conduction channel, thus enabling a unique capability for nanoscale conductive domain patterning in GO. An increase in FEBID electron dose results in a significant increase of the domain electrical conductivity with improving linearity of drain-source current vs. voltage dependence, indicative of a change of graphene oxide electronic properties from insulating to semiconducting. Density functional theory calculations suggest a possible mechanism underlying this experimentally observed phenomenon, as localized reduction of graphene oxide layers via interactions with highly reactive intermediates of electron-beam-assisted dissociation of surface-adsorbed hydrocarbon molecules. These findings establish an unusual route for using FEBID as nanoscale lithography and patterning technique for engineering carbon-based nanomaterials and devices with locally tailored electronic properties.

  3. Localized conductive patterning via focused electron beam reduction of graphene oxide

    SciTech Connect

    Kim, Songkil; Henry, Mathias; Kulkarni, Dhaval D.; Zackowski, Paul; Jang, Seung Soon; Tsukruk, Vladimir V.; Fedorov, Andrei G.

    2015-03-30

    We report on a method for “direct-write” conductive patterning via reduction of graphene oxide (GO) sheets using focused electron beam induced deposition (FEBID) of carbon. FEBID treatment of the intrinsically dielectric graphene oxide between two metal terminals opens up the conduction channel, thus enabling a unique capability for nanoscale conductive domain patterning in GO. An increase in FEBID electron dose results in a significant increase of the domain electrical conductivity with improving linearity of drain-source current vs. voltage dependence, indicative of a change of graphene oxide electronic properties from insulating to semiconducting. Density functional theory calculations suggest a possible mechanism underlying this experimentally observed phenomenon, as localized reduction of graphene oxide layers via interactions with highly reactive intermediates of electron-beam-assisted dissociation of surface-adsorbed hydrocarbon molecules. These findings establish an unusual route for using FEBID as nanoscale lithography and patterning technique for engineering carbon-based nanomaterials and devices with locally tailored electronic properties.

  4. Communication: Near-locality of exchange and correlation density functionals for 1- and 2-electron systems.

    PubMed

    Sun, Jianwei; Perdew, John P; Yang, Zenghui; Peng, Haowei

    2016-05-21

    The uniform electron gas and the hydrogen atom play fundamental roles in condensed matter physics and quantum chemistry. The former has an infinite number of electrons uniformly distributed over the neutralizing positively charged background, and the latter only one electron bound to the proton. The uniform electron gas was used to derive the local spin density approximation to the exchange-correlation functional that undergirds the development of the Kohn-Sham density functional theory. We show here that the ground-state exchange-correlation energies of the hydrogen atom and many other 1- and 2-electron systems are modeled surprisingly well by a different local spin density approximation (LSDA0). LSDA0 is constructed to satisfy exact constraints but agrees surprisingly well with the exact results for a uniform two-electron density in a finite, curved three-dimensional space. We also apply LSDA0 to excited or noded 1-electron densities, where it works less well. Furthermore, we show that the localization of the exact exchange hole for a 1- or 2-electron ground state can be measured by the ratio of the exact exchange energy to its optimal lower bound. PMID:27208927

  5. Communication: Near-locality of exchange and correlation density functionals for 1- and 2-electron systems

    NASA Astrophysics Data System (ADS)

    Sun, Jianwei; Perdew, John P.; Yang, Zenghui; Peng, Haowei

    2016-05-01

    The uniform electron gas and the hydrogen atom play fundamental roles in condensed matter physics and quantum chemistry. The former has an infinite number of electrons uniformly distributed over the neutralizing positively charged background, and the latter only one electron bound to the proton. The uniform electron gas was used to derive the local spin density approximation to the exchange-correlation functional that undergirds the development of the Kohn-Sham density functional theory. We show here that the ground-state exchange-correlation energies of the hydrogen atom and many other 1- and 2-electron systems are modeled surprisingly well by a different local spin density approximation (LSDA0). LSDA0 is constructed to satisfy exact constraints but agrees surprisingly well with the exact results for a uniform two-electron density in a finite, curved three-dimensional space. We also apply LSDA0 to excited or noded 1-electron densities, where it works less well. Furthermore, we show that the localization of the exact exchange hole for a 1- or 2-electron ground state can be measured by the ratio of the exact exchange energy to its optimal lower bound.

  6. Local structural excitations in model glass systems under applied load

    NASA Astrophysics Data System (ADS)

    Swayamjyoti, S.; Löffler, J. F.; Derlet, P. M.

    2016-04-01

    The potential-energy landscape of a model binary Lennard-Jones structural glass is investigated as a function of applied external strain, in terms of how local structural excitations (LSEs) respond to the load. Using the activation relaxation technique and nudged elastic band methods, the evolving structure and barrier energy of such LSEs are studied in detail. For the case of a tensile/compressive strain, the LSE barrier energies generally decrease/increase, whereas under pure shear, it may either increase or decrease resulting in a broadening of the barrier energy distribution. It is found that how a particular LSE responds to an applied strain is strongly controlled by the LSE's far-field internal stress signature prior to loading.

  7. Syntheses and electronic structures of decamethylmetallocenes

    SciTech Connect

    Robbins, J.L.

    1981-04-01

    The synthesis of decamethylmanganocene ((eta-C/sub 5/(CH/sub 3/)/sub 5/)/sub 2/Mn or (Me/sub 5/Cp)/sub 2/Mn)) is described. Magnetic susceptibility and electron paramagnetic resonance (EPR) studies show that (Me/sub 5/Cp)/sub 2/Mn is a low-spin, 17-electron compound with an orbitally degenerate, /sup 2/E/sub 2g/ (e/sub 2g//sup 3/ a/sub 1g//sup 2/) ground state. An x-ray crystallographic study of (Me/sub 5/Cp)/sub 2/Mn shows that it is a monomeric, D/sub 5d/ decamethylmetallocene with metal to ring carbon distances that are about 0.3 A shorter than those determined for high-spin manganocenes. The syntheses of new (Me/sub 5/Cp)/sub 2/M (M = Mg,V,Cr,Co, and Ni) and ((Me/sub 5/Cp)/sub 2/M)PF/sub 6/ (M = Cr,Co, and Ni) compounds are described. In addition, a preparative route to a novel, dicationic decamethylmetallocene, ((Me/sub 5/Cp)/sub 2/Ni)(PF/sub 6/)/sub 2/ is reported. Infrared, nuclear magnetic resonance, magnetic susceptibility, and/or x-ray crystallographic studies indicate that all the above compounds are D/sub 5d/ or D/sub 5h/ decamethylmetallocenes with low-spin electronic configurations. Cyclic voltammetry studies verify the reversibility and the one-electron nature of the (Me/sub 5/Cp)/sub 2/M ..-->.. ((Me/sub 5/Cp)/sub 2/M)/sup +/ (M = Cr,Mn,Fe,Co,Ni), ((Me/sub 5/Cp)/sub 2/Mn)/sup -/ ..-->.. (Me/sub 5/Cp)/sub 2/Mn and ((Me/sub 5/Cp)/sub 2/Ni)/sup +/ ..-->.. (Me/sub 5/Cp)/sub 2/Ni)/sup 2 +/ redox reactions. These studies reveal that the neutral decamethylmetallocenes are much more easily oxidized than their metallocene counterparts. This result attests to the electron-donating properties of the ten substituent methyl groups. Proton and carbon-13 NMR data are reported for the diamagnetic Mg(II), Mn(I), Fe(II), Co(III), and Ni(IV) decamethylmetallocenes and for ((Me/sub 5/Cp)/sub 2/V(CO)/sub 2/)/sup +/. The uv-visible absorption spectra of the 15-, 18- and 20- electron decamethylmetallocenes are also reported.

  8. Phase behavior and local structure of liquid crystalline polymers

    NASA Astrophysics Data System (ADS)

    Fynewever, Herb

    In this work we use a combination of theory and computer simulation to study the phase behavior of liquid crystalline polymers and the local structure of polymer melts. We review experimental and simulation evidence which shows that long and stiff molecules form orientationally ordered phases at packing fractions intermediate between the liquid and the solid. With the aid of a two-molecule simulation, we are able to apply Onsager's theory [Ann. N. Y. Acad. Sci. 51, 627 (1949)] for liquid crystal formation to flexible molecules without any additional approximations. Our results have a quantitative advantage over other theories in comparison with computer simulation data such as for the liquid-liquid crystal phase diagram. We also study the local structure of polymer melts using a two-molecule simulation to apply the density functional theories of Donley, Curro, and McCoy [J. Chem. Phys. 101 , 3205 (1994)1; and Yethiraj and Woodward [J. Chem. Phys 102 , 5499 (1995)]. The accuracy of these methods rivals that of integral equation theories in their predictions of local order. Further, the two-molecule simulation facilitates a more direct calculation of the equation of state via the monitoring of orientational correlations.

  9. Role of nonlinear localized structures and turbulence in magnetized plasma

    NASA Astrophysics Data System (ADS)

    Pathak, Neha; Yadav, Nitin; Uma, R.; Sharma, R. P.

    2016-09-01

    In the present study, we have analyzed the field localization of kinetic Alfvén wave (KAW) due to the presence of background density perturbation, which are assumed to be originated by the three dimensionally propagating low frequency KAW. These localized structures play an important role for energy transportation at smaller scales in the dispersion range of magnetic power spectrum. For the present model, governing dynamic equations of high frequency pump KAW and low frequency KAW has been derived by considering ponderomotive nonlinearity. Further, these coupled equations have been numerically solved to analyze the resulting localized structures of pump KAW and magnetic power spectrum in the magnetopause regime. Numerically calculated spectrum exhibits inertial range having spectral index of -3/2 followed by steeper scaling; this steepening in the turbulent spectrum is a signature of energy transportation from larger to smaller scales. In this way, the proposed mechanism, which is based on nonlinear wave-wave interaction, may be useful for understanding the particle acceleration and turbulence in magnetopause.

  10. High Resolution Local Structure-Constrained Image Upsampling.

    PubMed

    Zhao, Yang; Wang, Ronggang; Wang, Wenmin; Gao, Wen

    2015-11-01

    With the development of ultra-high-resolution display devices, the visual perception of fine texture details is becoming more and more important. A method of high-quality image upsampling with a low cost is greatly needed. In this paper, we propose a fast and efficient image upsampling method that makes use of high-resolution local structure constraints. The average local difference is used to divide a bicubic-interpolated image into a sharp edge area and a texture area, and these two areas are reconstructed separately with specific constraints. For reconstruction of the sharp edge area, a high-resolution gradient map is estimated as an extra constraint for the recovery of sharp and natural edges; for the reconstruction of the texture area, a high-resolution local texture structure map is estimated as an extra constraint to recover fine texture details. These two reconstructed areas are then combined to obtain the final high-resolution image. The experimental results demonstrated that the proposed method recovered finer pixel-level texture details and obtained top-level objective performance with a low time cost compared with state-of-the-art methods. PMID:26186777

  11. Local atomic arrangements and lattice distortions in layered Ge-Sb-Te crystal structures

    PubMed Central

    Lotnyk, Andriy; Ross, Ulrich; Bernütz, Sabine; Thelander, Erik; Rauschenbach, Bernd

    2016-01-01

    Insights into the local atomic arrangements of layered Ge-Sb-Te compounds are of particular importance from a fundamental point of view and for data storage applications. In this view, a detailed knowledge of the atomic structure in such alloys is central to understanding the functional properties both in the more commonly utilized amorphous–crystalline transition and in recently proposed interfacial phase change memory based on the transition between two crystalline structures. Aberration-corrected scanning transmission electron microscopy allows direct imaging of local arrangement in the crystalline lattice with atomic resolution. However, due to the non-trivial influence of thermal diffuse scattering on the high-angle scattering signal, a detailed examination of the image contrast requires comparison with theoretical image simulations. This work reveals the local atomic structure of trigonal Ge-Sb-Te thin films by using a combination of direct imaging of the atomic columns and theoretical image simulation approaches. The results show that the thin films are prone to the formation of stacking disorder with individual building blocks of the Ge2Sb2Te5, Ge1Sb2Te4 and Ge3Sb2Te6 crystal structures intercalated within randomly oriented grains. The comparison with image simulations based on various theoretical models reveals intermixed cation layers with pronounced local lattice distortions, exceeding those reported in literature. PMID:27220411

  12. Local atomic arrangements and lattice distortions in layered Ge-Sb-Te crystal structures.

    PubMed

    Lotnyk, Andriy; Ross, Ulrich; Bernütz, Sabine; Thelander, Erik; Rauschenbach, Bernd

    2016-01-01

    Insights into the local atomic arrangements of layered Ge-Sb-Te compounds are of particular importance from a fundamental point of view and for data storage applications. In this view, a detailed knowledge of the atomic structure in such alloys is central to understanding the functional properties both in the more commonly utilized amorphous-crystalline transition and in recently proposed interfacial phase change memory based on the transition between two crystalline structures. Aberration-corrected scanning transmission electron microscopy allows direct imaging of local arrangement in the crystalline lattice with atomic resolution. However, due to the non-trivial influence of thermal diffuse scattering on the high-angle scattering signal, a detailed examination of the image contrast requires comparison with theoretical image simulations. This work reveals the local atomic structure of trigonal Ge-Sb-Te thin films by using a combination of direct imaging of the atomic columns and theoretical image simulation approaches. The results show that the thin films are prone to the formation of stacking disorder with individual building blocks of the Ge2Sb2Te5, Ge1Sb2Te4 and Ge3Sb2Te6 crystal structures intercalated within randomly oriented grains. The comparison with image simulations based on various theoretical models reveals intermixed cation layers with pronounced local lattice distortions, exceeding those reported in literature. PMID:27220411

  13. Local atomic arrangements and lattice distortions in layered Ge-Sb-Te crystal structures

    NASA Astrophysics Data System (ADS)

    Lotnyk, Andriy; Ross, Ulrich; Bernütz, Sabine; Thelander, Erik; Rauschenbach, Bernd

    2016-05-01

    Insights into the local atomic arrangements of layered Ge-Sb-Te compounds are of particular importance from a fundamental point of view and for data storage applications. In this view, a detailed knowledge of the atomic structure in such alloys is central to understanding the functional properties both in the more commonly utilized amorphous–crystalline transition and in recently proposed interfacial phase change memory based on the transition between two crystalline structures. Aberration-corrected scanning transmission electron microscopy allows direct imaging of local arrangement in the crystalline lattice with atomic resolution. However, due to the non-trivial influence of thermal diffuse scattering on the high-angle scattering signal, a detailed examination of the image contrast requires comparison with theoretical image simulations. This work reveals the local atomic structure of trigonal Ge-Sb-Te thin films by using a combination of direct imaging of the atomic columns and theoretical image simulation approaches. The results show that the thin films are prone to the formation of stacking disorder with individual building blocks of the Ge2Sb2Te5, Ge1Sb2Te4 and Ge3Sb2Te6 crystal structures intercalated within randomly oriented grains. The comparison with image simulations based on various theoretical models reveals intermixed cation layers with pronounced local lattice distortions, exceeding those reported in literature.

  14. Protein structure prediction with local adjust tabu search algorithm

    PubMed Central

    2014-01-01

    Background Protein folding structure prediction is one of the most challenging problems in the bioinformatics domain. Because of the complexity of the realistic protein structure, the simplified structure model and the computational method should be adopted in the research. The AB off-lattice model is one of the simplification models, which only considers two classes of amino acids, hydrophobic (A) residues and hydrophilic (B) residues. Results The main work of this paper is to discuss how to optimize the lowest energy configurations in 2D off-lattice model and 3D off-lattice model by using Fibonacci sequences and real protein sequences. In order to avoid falling into local minimum and faster convergence to the global minimum, we introduce a novel method (SATS) to the protein structure problem, which combines simulated annealing algorithm and tabu search algorithm. Various strategies, such as the new encoding strategy, the adaptive neighborhood generation strategy and the local adjustment strategy, are adopted successfully for high-speed searching the optimal conformation corresponds to the lowest energy of the protein sequences. Experimental results show that some of the results obtained by the improved SATS are better than those reported in previous literatures, and we can sure that the lowest energy folding state for short Fibonacci sequences have been found. Conclusions Although the off-lattice models is not very realistic, they can reflect some important characteristics of the realistic protein. It can be found that 3D off-lattice model is more like native folding structure of the realistic protein than 2D off-lattice model. In addition, compared with some previous researches, the proposed hybrid algorithm can more effectively and more quickly search the spatial folding structure of a protein chain. PMID:25474708

  15. Electronic structure and magnetic coupling in copper oxide superconductors

    SciTech Connect

    Wang, Y.J. ); Newton, M.D. ); Davenport, J.W. )

    1992-11-01

    The electronic structure and magnetic coupling in La{sub 2}CuO{sub 4} and Nd{sub 2}CuO{sub 4} have been analyzed using the results of all-valence-electron calculations for (Cu{sub 2}O{sub 11}){sup 18{minus}}, (Cu{sub 4}O{sub 12}){sup 16{minus}}, and (Cu{sub 4}O{sub 20}){sup 32{minus}} clusters, and their {ital p}- and {ital n}-doped variants, embedded in a Madelung potential to represent the crystal environment. The calculations employ the semiempirical incomplete neglect of differential overlap (INDO) method, which is parametrized on the basis of atomic and molecular spectroscopic data, but which makes use of no data from copper oxide materials. The energies of the low-lying cluster spin states are fitted to a Heisenberg Hamiltonian and yield values of {ital J} (134 meV for La{sub 2}CuO{sub 4} and 117 meV for Nd{sub 2}CuO{sub 4}) in close agreement with experiment. The evaluation of {ital J} can be compactly represented in terms of the parameters ({ital t}, {ital U}, and {ital V}) of a one-band Hamiltonian that controls resonance among covalent and ionic valence-bond structures. The resonance mixing is achieved by configuration interaction (CI) among valence-band structures defined in terms of localized molecular orbitals (LMO's) obtained from self-consistent field (SCF) INDO calculations. {ital P} doping is found to involve strong hybridization of the 2{ital p}{sigma} orbitals of the in-plane oxygen ions and the 3{ital d}{sub {ital x}}{sup 2}{minus}{ital y}{sup 2} orbitals of the Cu ions, and the resulting holes are predominantly ({similar to}60%) located in the 2{ital p}{sigma} orbitals. The lowest-energy {ital n}-doped cluster states involve addition of electrons to the 4{ital s}/4{ital p} Cu atom manifolds. However, the separation of these states from low-spin (3{ital d}{sup 10}) alternatives is uncertain because of apparent sensitivity to the representation of the crystal potential, as found by Martin.

  16. Electron Precipitation Associated with Small-Scale Auroral Structures

    NASA Astrophysics Data System (ADS)

    Michell, R.; Samara, M.; Grubbs, G. A., II; Hampton, D. L.; Bonnell, J. W.; Ogasawara, K.

    2014-12-01

    We present results from the Ground-to-Rocket Electrons Electrodynamics Correlative Experiment (GREECE) sounding rocket mission, where we combined high-resolution ground-based auroral imaging with high time-resolution precipitating electron measurements. The GREECE payload successfully launched from Poker Flat, Alaska on 03 March 2014 and reached an apogee of approximately 335 km. The narrow field-of-view auroral imaging was taken from Venetie, AK, which is directly under apogee. This enabled the small-scale auroral features at the magnetic footpoint of the rocket payload to be imaged in detail. The electron precipitation was measured with the Acute Precipitating Electron Spectrometer (APES) onboard the payload. Features in the electron data are matched up with their corresponding auroral structures and boundaries, enabling measurement of the exact electron distributions responsible for the specific small-scale auroral features. These electron distributions will then be used to infer what the potential electron acceleration processes were.

  17. Curly arrows meet electron density transfers in chemical reaction mechanisms: from electron localization function (ELF) analysis to valence-shell electron-pair repulsion (VSEPR) inspired interpretation.

    PubMed

    Andrés, Juan; Berski, Sławomir; Silvi, Bernard

    2016-07-01

    Probing the electron density transfers during a chemical reaction can provide important insights, making possible to understand and control chemical reactions. This aim has required extensions of the relationships between the traditional chemical concepts and the quantum mechanical ones. The present work examines the detailed chemical insights that have been generated through 100 years of work worldwide on G. N. Lewis's ground breaking paper on The Atom and the Molecule (Lewis, G. N. The Atom and the Molecule, J. Am. Chem. Soc. 1916, 38, 762-785), with a focus on how the determination of reaction mechanisms can be reached applying the bonding evolution theory (BET), emphasizing how curly arrows meet electron density transfers in chemical reaction mechanisms and how the Lewis structure can be recovered. BET that combines the topological analysis of the electron localization function (ELF) and Thom's catastrophe theory (CT) provides a powerful tool providing insight into molecular mechanisms of chemical rearrangements. In agreement with physical laws and quantum theoretical insights, BET can be considered as an appropriate tool to tackle chemical reactivity with a wide range of possible applications. Likewise, the present approach retrieves the classical curly arrows used to describe the rearrangements of chemical bonds for a given reaction mechanism, providing detailed physical grounds for this type of representation. The ideas underlying the valence-shell-electron pair-repulsion (VSEPR) model applied to non-equilibrium geometries provide simple chemical explanations of density transfers. For a given geometry around a central atom, the arrangement of the electronic domain may comply or not with the VSEPR rules according with the valence shell population of the considered atom. A deformation yields arrangements which are either VSEPR defective (at least a domain is missing to match the VSEPR arrangement corresponding to the geometry of the ligands), VSEPR compliant

  18. Local measurement of optically induced photocurrent in semiconductor structures

    NASA Astrophysics Data System (ADS)

    Benesova, Marketa; Dobis, Pavel; Tomanek, Pavel; Uhdeova, Nadezda

    2003-07-01

    Photocurrent (PC) spectroscopic techniques have demonstrated to be helpful experimental method to investigate the local properties of bulk semiconductors, microstructures, surfaces and interfaces. We have measured locally induced PC of semiconductor quantum structures using a technique of reflection Scanning Near-field Optical Microscope (r-SNOM) in combination with Ti:Sapphire laser and tuning dye laser and with He-Ne laser. The r-SNOM employs an uncoated and/or Au-metalized single-mode fiber tip both in illumination and collection mode. Taking opportunity of the high lateral resolution of the microscope and combining it with fast micro-PL, it is possible to locate e.g. defects in a multiple quantum well grown by molecular beam epitaxy. Near-field characteristics of measured quantities are also discussed.

  19. Measuring capital market efficiency: Global and local correlations structure

    NASA Astrophysics Data System (ADS)

    Kristoufek, Ladislav; Vosvrda, Miloslav

    2013-01-01

    We introduce a new measure for capital market efficiency. The measure takes into consideration the correlation structure of the returns (long-term and short-term memory) and local herding behavior (fractal dimension). The efficiency measure is taken as a distance from an ideal efficient market situation. The proposed methodology is applied to a portfolio of 41 stock indices. We find that the Japanese NIKKEI is the most efficient market. From a geographical point of view, the more efficient markets are dominated by the European stock indices and the less efficient markets cover mainly Latin America, Asia and Oceania. The inefficiency is mainly driven by a local herding, i.e. a low fractal dimension.

  20. Correlating Electronic Transport to Atomic Structures in Self-Assembled Quantum Wires

    SciTech Connect

    Li, An-Ping; Qin, Shengyong; Kim, Tae Hwan; Ouyang, Wenjie; Zhang, Yanning; Weitering, Harm H; Shih, Chih-Kang; Baddorf, Arthur P; Wu, Ruiqian

    2012-01-01

    Quantum wires, as a smallest electronic conductor, are expected to be a fundamental component in all quantum architectures. The electronic conductance in quantum wires, however, is often dictated by structural instabilities and electron localization at the atomic scale. Here we report on the evolutions of electronic transport as a function of temperature and interwire coupling as the quantum wires of GdSi{sub 2} are self-assembled on Si(100) wire-by-wire. The correlation between structure, electronic properties, and electronic transport are examined by combining nanotransport measurements, scanning tunneling microscopy, and density functional theory calculations. A metal-insulator transition is revealed in isolated nanowires, while a robust metallic state is obtained in wire bundles at low temperature. The atomic defects lead to electron localizations in isolated nanowire, and interwire coupling stabilizes the structure and promotes the metallic states in wire bundles. This illustrates how the conductance nature of a one-dimensional system can be dramatically modified by the environmental change on the atomic scale.

  1. Electronic structure and stability of some silicon compounds

    NASA Astrophysics Data System (ADS)

    Novak, Igor; Abu-Izneid, Tareq; Kovač, Branka

    2010-05-01

    The electronic structures of N,1,3-tris(1,1-dimethylethyl)-cyclodisilazan-2-amine ( I) and 2,3,5,5-tetrakis(trimethylsilyl)cyclopentadiene ( II) have been investigated by HeI and HeII UV photoelectron spectroscopy (UPS) and quantum chemical calculations. We discuss the influence of substituent effects on their electronic structure and thermodynamic stability. Our study shows that trimethylsilyl substituents have strong influence on the electronic structure of cyclopentadiene via inductive effect. Their influence on thermodynamic stability is also pronounced. In substituted cyclodisilazanes hyperconjugative influence of alkylsilyl groups was shown to cause relative thermodynamic stabilization of the cyclodisilazane system.

  2. Electronic Structure Contributions to Reactivity in Xanthine Oxidase Family Enzymes

    PubMed Central

    Stein, Benjamin W.; Kirk, Martin L.

    2016-01-01

    We review the xanthine oxidase (XO) family of pyranopterin molybdenum enzymes with a specific emphasis on electronic structure contributions to reactivity. In addition to xanthine and aldehyde oxidoreductases, which catalyze the 2-electron oxidation of aromatic heterocycles and aldehyde substrates, this mini-review highlights recent work on the closely related carbon monoxide dehydrogenase (CODH) that catalyzes the oxidation of CO using a unique Mo-Cu heterobimetallic active site. A primary focus of this mini-review relates to how spectroscopy and computational methods have been used to develop an understanding of critical relationships between geometric structure, electronic structure, and catalytic function. PMID:25425163

  3. Spectral differences in real-space electronic structure calculations

    NASA Astrophysics Data System (ADS)

    Jordan, D. K.; Mazziotti, D. A.

    2004-01-01

    Real-space grids for electronic structure calculations are efficient because the potential is diagonal while the second derivative in the kinetic energy may be sparsely evaluated with finite differences or finite elements. In applications to vibrational problems in chemical physics a family of methods known as spectral differences has improved finite differences by several orders of magnitude. In this paper the use of spectral differences for electronic structure is studied. Spectral differences are implemented in two electronic structure programs PARSEC and HARES which currently employ finite differences. Applications to silicon clusters and lattices indicate that spectral differences achieve the same accuracy as finite differences with less computational work.

  4. Unimodal biometric system based on local topology structure preserving projections

    NASA Astrophysics Data System (ADS)

    Liu, Huanxi; Lv, Xiaowei; Li, Xiong; Liu, Yuncai

    2009-11-01

    We propose a unified unimodal biometric system that is suitable for most individual modalities, e.g., face and gait. The proposed system consists of three steps: (1) preprocessing raw biometric data, (2) determining the intrinsic low-dimensional subspace of preprocessed data by local topology structure preserving projections (LTSPP), and (3) performing the classification in the determined subspace using the intraclass distance sum. In the proposed system, LTSPP is a novel subspace algorithm that focuses not only on the class information but also on the local topology structure. In terms of representing the separability of different classes, LTSPP projects the interclass margin data far apart. Meanwhile, LTSPP preserves the intraclass topology structures by using linear reconstruction coefficients. Compared with other subspace methods, LTSPP possesses more discriminant abilities and is more suitable for biometric recognition. In addition, both preprocessing each raw datum into unit and performing the classification using the intraclass distance sum are helpful to improve the recognition rates. We carry out various recognition experiments using the Yale and HumanID gait databases. The encouraging experimental results demonstrate the effectiveness of our unified unimodal biometric system, and the proposed LTSPP algorithm for this system can yield the best recognition rates compared to the other algorithms.

  5. Electronic structure of fluorides: general trends for ground and excited state properties

    NASA Astrophysics Data System (ADS)

    Cadelano, E.; Cappellini, G.

    2011-05-01

    The electronic structure of fluorite crystals are studied by means of density functional theory within the local density approximation for the exchange correlation energy. The ground-state electronic properties, which have been calculated for the cubic structures CaF2, SrF2, BaF2, CdF2, HgF2, β-PbF2, using a plane waves expansion of the wave functions, show good comparison with existing experimental data and previous theoretical results. The electronic density of states at the gap region for all the compounds and their energy-band structure have been calculated and compared with the existing data in the literature. General trends for the ground-state parameters, the electronic energy-bands and transition energies for all the fluorides considered are given and discussed in details. Moreover, for the first time results for HgF2 have been presented.

  6. Structural, electronic and thermal properties of Mo{sub 3}Ir superconductors

    SciTech Connect

    Subhashree, G. Sankar, S.; Krithiga, R.; Devi, L. Vimala

    2015-06-24

    Self consistent first principle calculations on superconducting material Mo{sub 3}Ir of A15 phase have been performed to understand their fundamental characteristics of the structural, electronic and thermal properties. The bulk modulus (B{sub 0}), Debye temperature (θ{sub D}), density of states (N (E{sub F})) and electronic specific heat coefficient (γ) have been computed in terms of the electronic structure results obtained by using the tight-binding linear muffin tin orbital (TB-LMTO) method based on the density functional theory (DFT) within the local density approximation (LDA). Structural, electronic and thermal properties calculated here are found to corroborate well with the experimental and theoretical results of literature.

  7. Dynamic modulation of electronic properties of graphene by localized carbon doping using focused electron beam induced deposition

    NASA Astrophysics Data System (ADS)

    Kim, S.; Russell, M.; Henry, M.; Kim, S. S.; Naik, R. R.; Voevodin, A. A.; Jang, S. S.; Tsukruk, V. V.; Fedorov, A. G.

    2015-09-01

    We report on the first demonstration of controllable carbon doping of graphene to engineer local electronic properties of a graphene conduction channel using focused electron beam induced deposition (FEBID). Electrical measurements indicate that an ``n-p-n'' junction on graphene conduction channel is formed by partial carbon deposition near the source and drain metal contacts by low energy (<50 eV) secondary electrons due to inelastic collisions of long range backscattered primary electrons generated from a low dose of high energy (25 keV) electron beam (1 × 1018 e- per cm2). Detailed AFM imaging provides direct evidence of the new mechanism responsible for dynamic evolution of the locally varying graphene doping. The FEBID carbon atoms, which are physisorbed and weakly bound to graphene, diffuse towards the middle of graphene conduction channel due to their surface chemical potential gradient, resulting in negative shift of Dirac voltage. Increasing a primary electron dose to 1 × 1019 e- per cm2 results in a significant increase of carbon deposition, such that it covers the entire graphene conduction channel at high surface density, leading to n-doping of graphene channel. Collectively, these findings establish a unique capability of FEBID technique to dynamically modulate the doping state of graphene, thus enabling a new route to resist-free, ``direct-write'' functional patterning of graphene-based electronic devices with potential for on-demand re-configurability.We report on the first demonstration of controllable carbon doping of graphene to engineer local electronic properties of a graphene conduction channel using focused electron beam induced deposition (FEBID). Electrical measurements indicate that an ``n-p-n'' junction on graphene conduction channel is formed by partial carbon deposition near the source and drain metal contacts by low energy (<50 eV) secondary electrons due to inelastic collisions of long range backscattered primary electrons generated

  8. Presolvated Electron Reaction with Methylacetoacetate: Electron Localization, Proton-Deuteron Exchange, and H-atom Abstraction

    PubMed Central

    Petrovici, Alex; Adhikary, Amitava; Kumar, Anil; Sevilla, Michael D.

    2015-01-01

    Radiation-produced electrons initiate various reaction processes that are important to radiation damage to biomolecules. In this work, the site of attachment of the prehydrated electrons with methylacetoacetate (MAA, CH3-CO-CH2-CO-OCH3) at 77 K and subsequent reactions of the anion radical (CH3-CO•−-CH2-CO-OCH3) in the temperature range (77 to ca. 170 K) have been investigated in homogeneous H2O and D2O aqueous glasses by electron spin resonance (ESR) spectroscopy. At 77 K, the prehydrated electron attaches to MAA forming the anion radical in which the electron is delocalized over the two carbonyl groups. This species readily protonates to produce the protonated electron adduct radical CH3-C(•)OH-CH2-CO-OCH3. The ESR spectrum of CH3-C(•)OH-CH2-CO-OCH3 in H2O shows line components due to proton hyperfine couplings of the methyl and methylene groups. Whereas, the ESR spectrum of CH3-C(•)OH-CH2-CO-OCH3 in D2O glass shows only the line components due to proton hyperfine couplings of CH3 group. This is expected since the methylen protons in MAA are readily exchangeable in D2O. On stepwise annealing to higher temperatures (ca. 150 to 170 K), CH3-C(•)OH-CH2-CO-OCH3 undergoes bimolecular H-atom abstraction from MAA to form the more stable radical, CH3-CO-CH•-CO-OCH3. Theoretical calculations using density functional theory (DFT) support the radical assignments. PMID:25255751

  9. Electronic structure and spectral-luminescent properties of 1,2,4,6-tetrasubstituted pyridinium salts

    SciTech Connect

    Korunova, A.F.; Krainov, I.P.; Protsenko, E.G.

    1985-09-01

    The structure of the electronic excitation of 1,2,4,6-tetrasubstituted pyridinium salts was studied by quantum-chemical calculations carried out by the SCF PPP CI method, using excitation-localization numbers on the atoms and fragments, and interfragmentary charge transfer numbers. The nature of the absorption bands observed in the spectra and certain structural factors causing the spectral-luminescent properties were established.

  10. Characterization of small thermal structures in RFX-mod electron temperature profiles

    NASA Astrophysics Data System (ADS)

    Fassina, A.; Gobbin, M.; Spagnolo, S.; Franz, P.; Terranova, D.

    2016-05-01

    In the RFX-mod reverse field pinch (RFP) experiment, electron temperature profiles often feature structures and fluctuations at fine scale. The present work aims at characterizing their occurrence and their localization, in particular by linking them to underlying tearing modes magnetic islands. The confinement characteristics are discussed, identifying analogies with respect to high scale T e structures. Finally, high frequency magnetic activity (i.e. microtearing instabilities) is confirmed to be closely correlated to the presence and proximity of temperature gradients.

  11. Structure and electronic properties of mixed (a + c) dislocation cores in GaN

    SciTech Connect

    Horton, M. K.; Rhode, S. L.; Moram, M. A.

    2014-08-14

    Classical atomistic models and atomic-resolution scanning transmission electron microscopy studies of GaN films reveal that mixed (a + c)-type dislocations have multiple different core structures, including a dissociated structure consisting of a planar fault on one of the (12{sup ¯}10) planes terminated by two different partial dislocations. Density functional theory calculations show that all cores introduce localized states into the band gap, which affects device performance.

  12. Recent advances in electronic structure theory

    NASA Astrophysics Data System (ADS)

    Piecuch, Piotr; Kowalski, Karol; Pimienta, Ian S. O.; McGuire, Michael J.

    The recently developed new approach to the many-electron correlation problem in atoms and molecules, termed the method of moments of coupled-cluster (CC) equations (MMCC), is reviewed. The ground-state MMCC formalism and its extension to excited electronic states via the equation-of-motion coupled-cluster (EOMCC) approach are discussed. The main principle of all MMCC methods is that of the non-iterative energy corrections which, when added to the ground- and excited-state energies obtained in the standard CC calculations, such as CCSD or EOMCCSD, recover the exact, full configuration interaction (CI) energies. Three types of the MMCC approximations are reviewed in detail: (i) the CI-corrected MMCC methods, which can be applied to ground and excited states; (ii) the renormalized and completely renormalized CC methods for ground states; and (iii) the quasi-variational MMCC approaches for the ground-state problem, including the quadratic MMCC models. It is demonstrated that the MMCC formalism provides a new theoretical framework for designing 'black-box' CC approaches that lead to an excellent description of entire potential energy surfaces of ground- and excited-state molecular systems with an ease of use of the standard single-reference methods. The completely renormalized (CR) CCSD(T) and CCSD(TQ) methods and their quadratic and excited-state MMCC analogues remove the failing of the standard CCSD, CCSD(T), EOMCCSD and similar methods at larger internuclear separations and for states that normally require a genuine multireference description. All theoretical ideas are illustrated by numerical examples involving bond breaking, excited vibrational states, reactive potential energy surfaces and difficult cases of excited electronic states. The description of the existing and well-established variants of the MMCC theory, such as CR-CCSD(T), is augmented by the discussion of future prospects and potentially useful recent developments, including the extension of the black

  13. Advancing Efficient All-Electron Electronic Structure Methods Based on Numeric Atom-Centered Orbitals for Energy Related Materials

    NASA Astrophysics Data System (ADS)

    Blum, Volker

    This talk describes recent advances of a general, efficient, accurate all-electron electronic theory approach based on numeric atom-centered orbitals; emphasis is placed on developments related to materials for energy conversion and their discovery. For total energies and electron band structures, we show that the overall accuracy is on par with the best benchmark quality codes for materials, but scalable to large system sizes (1,000s of atoms) and amenable to both periodic and non-periodic simulations. A recent localized resolution-of-identity approach for the Coulomb operator enables O (N) hybrid functional based descriptions of the electronic structure of non-periodic and periodic systems, shown for supercell sizes up to 1,000 atoms; the same approach yields accurate results for many-body perturbation theory as well. For molecular systems, we also show how many-body perturbation theory for charged and neutral quasiparticle excitation energies can be efficiently yet accurately applied using basis sets of computationally manageable size. Finally, the talk highlights applications to the electronic structure of hybrid organic-inorganic perovskite materials, as well as to graphene-based substrates for possible future transition metal compound based electrocatalyst materials. All methods described here are part of the FHI-aims code. VB gratefully acknowledges contributions by numerous collaborators at Duke University, Fritz Haber Institute Berlin, TU Munich, USTC Hefei, Aalto University, and many others around the globe.

  14. Local intelligent electronic device (IED) rendering templates over limited bandwidth communication link to manage remote IED

    DOEpatents

    Bradetich, Ryan; Dearien, Jason A; Grussling, Barry Jakob; Remaley, Gavin

    2013-11-05

    The present disclosure provides systems and methods for remote device management. According to various embodiments, a local intelligent electronic device (IED) may be in communication with a remote IED via a limited bandwidth communication link, such as a serial link. The limited bandwidth communication link may not support traditional remote management interfaces. According to one embodiment, a local IED may present an operator with a management interface for a remote IED by rendering locally stored templates. The local IED may render the locally stored templates using sparse data obtained from the remote IED. According to various embodiments, the management interface may be a web client interface and/or an HTML interface. The bandwidth required to present a remote management interface may be significantly reduced by rendering locally stored templates rather than requesting an entire management interface from the remote IED. According to various embodiments, an IED may comprise an encryption transceiver.

  15. Localized structures in dissipative media: from optics to plant ecology

    PubMed Central

    Tlidi, M.; Staliunas, K.; Panajotov, K.; Vladimirov, A. G.; Clerc, M. G.

    2014-01-01

    Localized structures (LSs) in dissipative media appear in various fields of natural science such as biology, chemistry, plant ecology, optics and laser physics. The proposal for this Theme Issue was to gather specialists from various fields of nonlinear science towards a cross-fertilization among active areas of research. This is a cross-disciplinary area of research dominated by nonlinear optics due to potential applications for all-optical control of light, optical storage and information processing. This Theme Issue contains contributions from 18 active groups involved in the LS field and have all made significant contributions in recent years. PMID:25246688

  16. Localization-Based Super-Resolution Imaging of Cellular Structures

    PubMed Central

    Kanchanawong, Pakorn; Waterman, Clare M.

    2013-01-01

    Fluorescence microscopy allows direct visualization of fluorescently tagged proteins within cells. However, the spatial resolution of conventional fluorescence microscopes is limited by diffraction to ~250 nm, prompting the development of super-resolution microscopy which offers resolution approaching the scale of single proteins, i.e., ~20 nm. Here, we describe protocols for single molecule localization-based super-resolution imaging, using focal adhesion proteins as an example and employing either photoswitchable fluorophores or photoactivatable fluorescent proteins. These protocols should also be easily adaptable to imaging a broad array of macromolecular assemblies in cells whose components can be fluorescently tagged and assemble into high density structures. PMID:23868582

  17. Modeling Polymorphic Molecular Crystals with Electronic Structure Theory.

    PubMed

    Beran, Gregory J O

    2016-05-11

    Interest in molecular crystals has grown thanks to their relevance to pharmaceuticals, organic semiconductor materials, foods, and many other applications. Electronic structure methods have become an increasingly important tool for modeling molecular crystals and polymorphism. This article reviews electronic structure techniques used to model molecular crystals, including periodic density functional theory, periodic second-order Møller-Plesset perturbation theory, fragment-based electronic structure methods, and diffusion Monte Carlo. It also discusses the use of these models for predicting a variety of crystal properties that are relevant to the study of polymorphism, including lattice energies, structures, crystal structure prediction, polymorphism, phase diagrams, vibrational spectroscopies, and nuclear magnetic resonance spectroscopy. Finally, tools for analyzing crystal structures and intermolecular interactions are briefly discussed. PMID:27008426

  18. Fabrication of nano ion-electron sources and nano-probes by local electron bombardment

    NASA Astrophysics Data System (ADS)

    Rezeq, Moh'd.; Ali, Ahmed; Barada, Hassan

    2015-04-01

    A new method for fabricating nano ion-electron sources and nano probes with an apex in the range of 1 nm is introduced. The method is based on bombarding a regular tip apex with electrons extracted and accelerated from a nearby source by the electric field. This can be achieved by placing a metal ring around a precursor metal tip at a level below the tip apex in a field ion microscope (FIM). The metal ring is then heated, by a grounded DC power source, to a temperature below the thermionic emission value. The electric field between the tip and the hot ring is high enough to cause electrons to be extracted from the metal ring, i.e. Schottky field emission, and then accelerated to the shank with energy sufficient to dislodge atoms from the shank. An atomic scale apex with a single atom end can be obtained by monitoring the evolution of the tip apex due to the movement of mobile atoms while adjusting the tip electric field and the temperature of the metal ring. As this method depends only on the electron bombardment mechanism, this makes it a clean process that can be applied to any metal or heavily doped semiconductor materials appropriate for generating a high electric field for FIM applications.

  19. Electron structure: Shape, size, and generalized parton distributions in QED

    NASA Astrophysics Data System (ADS)

    Miller, Gerald A.

    2014-12-01

    The shape of the electron is studied using lowest-order perturbation theory. Quantities used to probe the structure of the proton—form factors, generalized parton distributions, transverse densities, Wigner distributions and the angular momentum content—are computed for the electron-photon component of the electron wave function. The influence of longitudinally polarized photons, demanded by the need for infrared regularization via a nonzero photon mass, is included. The appropriate value of the photon mass depends on experimental conditions, and consequently the size of the electron (as defined by the slope of its Dirac form factor) bound in a hydrogen atom is found to be about four times larger than when the electron is in a continuum scattering state. The shape of the electron, as determined from the transverse density and generalized parton distributions, is shown not to be round, and the continuum electron is shown to be far less round than the bound electron. An electron distribution function (analogous to the quark distribution function) is defined, and that of the bound electron is shown to be suppressed compared to that of the continuum electron. If the relative transverse momentum of the virtual electron and photon is large compared with the electron mass, the virtual electron and photon each carry nearly the total angular momentum of the physical electron (1 /2 ), with the orbital angular momentum being nearly (-1 /2 ). Including the nonzero photon mass leads to the suppression of end-point contributions to form factors. Implications for proton structure and color transparency are discussed.

  20. XAFS study on the impact of local structure on electrochemical performance for Co3O4 nanowire arrays

    NASA Astrophysics Data System (ADS)

    Jiang, Shan; Cheng, Weiren; He, Jingfu; Huang, Junheng; Liu, Qinghua; Jiang, Yong; Wei, Shiqiang

    2016-05-01

    Determining the local structure of catalyst materials is critical for understanding the mechanism of enhanced electrochemical activity in semiconductor electrode. Here, using X-ray absorption fine structure (XAFS) spectra, we reveal that the local disorder structure is formed for the mixed-phase Co3O4 nanowire arrays due to the interaction between the phases of Co3O4 and Co2(OH)2CO3. Comparing to pure Co3O4 nanowire arrays, the mixed phase sample is richer in Co2+ and the electronic structure is changed by the local structure, which are demonstrated by the X-ray absorption near-edge structure (XANES) spectra. It is deduced that the mixed-phase Co3O4 nanowire arrays with abundant Co2+ sites provide more redox centres in electrochemical reaction than the pure Co3O4 nanowire arrays.

  1. Electron Diffraction Determination of Nanoscale Structures

    SciTech Connect

    Parks, Joel H

    2013-03-01

    Dominant research results on adsorption on gold clusters are reviewed, including adsorption of H{sub 2}O and O{sub 2} on gold cluster cations and anions, kinetics of CO adsorption to middle sized gold cluster cations, adsorption of CO on Au{sub n}{sup +} with induced changes in structure, and H{sub 2}O enhancement of CO adsorption.

  2. Local probing of structure and property in dimensionally confined amorphous and crystalline structures by S/TEM

    NASA Astrophysics Data System (ADS)

    Yan, Aiming

    The characterization of materials' microstructure has been brought up to a new level since the invention and broad application of transmission electron microscope (TEM) thanks to the high-energy electron beam source which guarantees an unsurpassable spatial resolution and theoretical study of interaction between electron and matter. The advent of nano-world has imposed an urgent request to characterize nano-assemblies in nano- or even sub-nano-scale and scanning transmission electron microscopy (STEM) which typically utilizes an electron probe with a size of 1nm or even smaller has found its unique advantage to unravel the local structure, chemical and physical properties of these emerging nanostructures. Dimensionally constrained nanostructures such as thin films and nanopatterned systems have attracted people's attention for decades due to their novel chemical and physical properties and popularity in energy storage, biological integration and etc. This dissertation focuses on the unique characterization capability of S/TEM to study the local order in amorphous transparent conducting oxide thin films, disordering in 2-D layered materials, localized surface plasmons in nanoporous gold patterns on 2-D layered structures and crystallization process in dimensionally and spatially constrained oxide nanopatterns observed by in-situ TEM. Electron diffraction and x-ray diffraction are commonly used techniques to study the crystallinity in a certain material - crystalline or amorphous. In amorphous materials which lack long-range order, normal electron diffraction and x-ray diffraction techniques won't be able to extract any useful information regarding the ordering or disordering in the materials. We have developed a unique set of electron diffraction methods in both TEM and STEM, combined with density functional theory molecular dynamics of liquid quench to study the short-range (< 1 nm) and medium-range order (between 1 nm and 3 nm) in amorphous transparent oxide films

  3. Local structure study of Fe dopants in Ni-deficit Ni3Al alloys

    DOE PAGESBeta

    V. N. Ivanovski; Umicevic, A.; Belosevic-Cavor, J.; Lei, Hechang; Li, Lijun; Cekic, B.; Koteski, V.; Petrovic, C.

    2015-08-24

    We found that the local electronic and magnetic structure, hyperfine interactions, and phase composition of polycrystalline Ni–deficient Ni 3-x FexAl (x = 0.18 and 0.36) were investigated by means of 57 Fe Mössbauer spectroscopy. The samples were characterized by X–ray diffraction and magnetization measurements. The ab initio calculations performed with the projector augmented wave method and the calculations of the energies of iron point defects were done to elucidate the electronic structure and site preference of Fe doped Ni 3 Al. Moreover, the value of calculated electric field gradient tensor Vzz=1.6 1021Vm-2 matches well with the results of Mössbauer spectroscopymore » and indicates that the Fe atoms occupy Ni sites.« less

  4. Electronic structure of CrAs and FeAs

    NASA Astrophysics Data System (ADS)

    Podloucky, Raimund

    1984-08-01

    As in a recent study for MnAs a two centre tight binding model consisting of itinerant metal d-states hybridizing with non-metal p-states was applied for CrAs and FeAs to calculate unpolarized and spin polarized local densities of states, ferromagnetic moments and band energies. The factor for the change of the d-band width relative to MnAs was estimated to be 1.3 for CrAs and 0.8 for FeAs. The self-consistent separation of the p- and d-band centres amounts to -1.3 eV for CrAs and -0.5 eV for FeAs providing a charge transfer of 0.8 and 0.6 electrons from the metal to the As atoms, correspondingly. One B8 1 structure and two B31 structures according to low and high temperature phases were studied for each compound. For CrAs self-consistent magnetic moments of 1.58 and 1.2μ B were obtained, respectively. For FeAs no ferromagnetic moment could be stabilized unless the d-band width was substantially reduced. The results are discussed with respect to MnAs. The model is able to reproduce the increase and breakdown of the magnetic moment for the series CrAs-MnAs-FeAs. Furthermore, the correct structural trend B31-B8 1-B31 is obtained if the band energy differences are corrected by a constant of 0.3 eV. This correction is attributed to the failure of the model to provide absolute differences of total energies.

  5. Linear Scaling Electronic Structure Methods with Periodic Boundary Conditions

    SciTech Connect

    Gustavo E. Scuseria

    2008-02-08

    The methodological development and computational implementation of linear scaling quantum chemistry methods for the accurate calculation of electronic structure and properties of periodic systems (solids, surfaces, and polymers) and their application to chemical problems of DOE relevance.

  6. Revealing the hidden correlated electronic structure of strained graphene

    NASA Astrophysics Data System (ADS)

    Craco, L.; Selli, D.; Seifert, G.; Leoni, S.

    2015-05-01

    We explore the effect of isotropic strain on the electronic structure of graphene. It is shown that the interplay between one-particle band narrowing and sizable multiorbital Coulomb interactions induces a transition from a Dirac-liquid semimetal to an orbital selective metal characterized by narrow π -orbital Kondo clouds and abrupt downshift of σ* states. The correlated electronic structure we derive is promising in the sense that it leads to results that might explain the reshaped electronic structure of graphene nanobubbles probed in scanning tunneling microscopy. Our proposal is a key step in understanding the intricate and interdependent changes in orbital and electronic degrees of freedom of strained materials with hexagonal lattice structure.

  7. Secondary electron emission from surfaces with small structure

    NASA Astrophysics Data System (ADS)

    Dzhanoev, A. R.; Spahn, F.; Yaroshenko, V.; Lühr, H.; Schmidt, J.

    2015-09-01

    It is found that for objects possessing small surface structures with differing radii of curvature the secondary electron emission (SEE) yield may be significantly higher than for objects with smooth surfaces of the same material. The effect is highly pronounced for surface structures of nanometer scale, often providing a more than 100 % increase of the SEE yield. The results also show that the SEE yield from surfaces with structure does not show a universal dependence on the energy of the primary, incident electrons as it is found for flat surfaces in experiments. We derive conditions for the applicability of the conventional formulation of SEE using the simplifying assumption of universal dependence. Our analysis provides a basis for studying low-energy electron emission from nanometer structured surfaces under a penetrating electron beam important in many technological applications.

  8. Stacking dependent electronic structures of transition metal dichalcogenides heterobilayer

    NASA Astrophysics Data System (ADS)

    Lee, Yea-Lee; Park, Cheol-Hwan; Ihm, Jisoon

    The systematic study of the electronic structures and optical properties of the transition metal dichalcogenides (TMD) heterobilayers can significantly improve the designing of new electronic and optoelectronic devices. Here, we theoretically study the electronic structures and optical properties of TMD heterobilayers using the first-principles methods. The band structures of TMD heterobilayer are shown to be determined by the band alignments of the each layer, the weak interlayer interactions, and angle dependent stacking patterns. The photoluminescence spectra are investigated using the calculated band structures, and the optical absorption spectra are examined by the GW approximations including the electron-hole interaction through the solution of the Bethe-Salpeter equation. It is expected that the weak interlayer interaction gives rise to the substantial interlayer optical transition which will be corresponding to the interlayer exciton.

  9. Interfacial valence electron localization and the corrosion resistance of Al-SiC nanocomposite

    NASA Astrophysics Data System (ADS)

    Mosleh-Shirazi, Sareh; Hua, Guomin; Akhlaghi, Farshad; Yan, Xianguo; Li, Dongyang

    2015-12-01

    Microstructural inhomogeneity generally deteriorates the corrosion resistance of materials due to the galvanic effect and interfacial issues. However, the situation may change for nanostructured materials. This article reports our studies on the corrosion behavior of SiC nanoparticle-reinforced Al6061 matrix composite. It was observed that the corrosion resistance of Al6061 increased when SiC nanoparticles were added. Overall electron work function (EWF) of the Al-SiC nanocomposite increased, along with an increase in the corrosion potential. The electron localization function of the Al-SiC nanocomposite was calculated and the results revealed that valence electrons were localized in the region of SiC-Al interface, resulting in an increase in the overall work function and thus building a higher barrier to hinder electrons in the nano-composite to participate in corrosion reactions.

  10. Interfacial valence electron localization and the corrosion resistance of Al-SiC nanocomposite

    PubMed Central

    Mosleh-Shirazi, Sareh; Hua, Guomin; Akhlaghi, Farshad; Yan, Xianguo; Li, Dongyang

    2015-01-01

    Microstructural inhomogeneity generally deteriorates the corrosion resistance of materials due to the galvanic effect and interfacial issues. However, the situation may change for nanostructured materials. This article reports our studies on the corrosion behavior of SiC nanoparticle-reinforced Al6061 matrix composite. It was observed that the corrosion resistance of Al6061 increased when SiC nanoparticles were added. Overall electron work function (EWF) of the Al-SiC nanocomposite increased, along with an increase in the corrosion potential. The electron localization function of the Al-SiC nanocomposite was calculated and the results revealed that valence electrons were localized in the region of SiC-Al interface, resulting in an increase in the overall work function and thus building a higher barrier to hinder electrons in the nano-composite to participate in corrosion reactions. PMID:26667968

  11. Local structure studies of materials using pair distribution function analysis

    NASA Astrophysics Data System (ADS)

    Peterson, Joseph W.

    A collection of pair distribution function studies on various materials is presented in this dissertation. In each case, local structure information of interest pushes the current limits of what these studies can accomplish. The goal is to provide insight into the individual material behaviors as well as to investigate ways to expand the current limits of PDF analysis. Where possible, I provide a framework for how PDF analysis might be applied to a wider set of material phenomena. Throughout the dissertation, I discuss 0 the capabilities of the PDF method to provide information pertaining to a material's structure and properties, ii) current limitations in the conventional approach to PDF analysis, iii) possible solutions to overcome certain limitations in PDF analysis, and iv) suggestions for future work to expand and improve the capabilities PDF analysis.

  12. Topological band order, structural, electronic and optical properties of XPdBi (X = Lu, Sc) compounds

    NASA Astrophysics Data System (ADS)

    Narimani, M.; Nourbakhsh, Z.

    2016-05-01

    In this paper, the structural, electronic and optical properties of LuPdBi and ScPdBi compounds are investigated using the density functional theory by WIEN2K package within the generalized gradient approximation, local density approximation, Engel-Vosco generalized gradient approximations and modified Becke-Johnson potential approaches. The topological phases and band orders of these compounds are studied. The effect of pressure on band inversion strength, electron density of states and the linear coefficient of the electronic specific heat of these compounds is investigated. Furthermore, the effect of pressure on real and imaginary parts of dielectric function, absorption and reflectivity coefficients of these compounds is studied.

  13. Density Functional Theory of Structural and Electronic Properties of III-N Semiconductors

    SciTech Connect

    Guerel, H. Hakan; Akinci, Oezden; Uenlue, Hilmi

    2010-11-01

    In this wok, we present the density functional theory (DFT) calculations of cubic III-N based semiconductors by using the full potential linear augmented plane-wave method plus local orbitals as implemented in the WIEN2k code. Our aim is to predict the pressure effect on structural and electronic properties of III-N binaries and ternaries. Results are given for structural properties (e.g., lattice constant, elastic constants, bulk modulus, and its pressure derivative) and electronic properties (e.g., band structure, density of states, band gaps and band widths) of GaAs, GaN, AlN, and InN binaries and GaAsN ternaries. The proposed model uses GGA exchange-correlation potential to determine band gaps of semiconductors at {Gamma}, L and X high symmetry points of Brillouin zone. The results are found in good agreement with available experimental data for structural and electronic properties of these semiconductors.

  14. Electronic structure of small silicon clusters

    SciTech Connect

    Wales, D.J.

    1994-03-01

    Predictions of Stone`s tensor-surface-harmonic theory [Mol. Phys. 41, 1339 (1980)] for bonding in small silicon clusters are tested by {ital ab} {ital initio} calculations. Stable geometries, along with the energies and symmetries of the occupied molecular orbitals, may all be rationalized within the model. For example, local energy minima for Si{sub {ital n}}{sup 2{minus}} clusters are found which are isostructural to the borane and carborane clusters B{sub {ital n}}H{sub {ital n}}{sup 2{minus}} and C{sub 2}B{sub {ital n}{minus}2}H{sub {ital n}}. In particular, both Si{sub 12}{sup 2{minus}} and Si{sub 13}{sup 2+} exhibit icosahedral geometries which are true minima.

  15. Fundamental limitations of the local approximation for electron distribution function and fluid model in bounded plasmas

    SciTech Connect

    Krasilnikov, M. B. Kudryavtsev, A. A.; Kapustin, K. D.

    2014-12-15

    It is shown that the local approximation for computing the electron distribution function depends both on the ratio between the energy relaxation length and a characteristic plasma length and on the ratio between heating and ambipolar electric fields. In particular, the local approximation is not valid at the discharge periphery even at high pressure due to the fact that the ambipolar electric field practically always is larger than the heating electric field.

  16. Non-rigid registration and non-local principle component analysis to improve electron microscopy spectrum images

    NASA Astrophysics Data System (ADS)

    Yankovich, Andrew B.; Zhang, Chenyu; Oh, Albert; Slater, Thomas J. A.; Azough, Feridoon; Freer, Robert; Haigh, Sarah J.; Willett, Rebecca; Voyles, Paul M.

    2016-09-01

    Image registration and non-local Poisson principal component analysis (PCA) denoising improve the quality of characteristic x-ray (EDS) spectrum imaging of Ca-stabilized Nd2/3TiO3 acquired at atomic resolution in a scanning transmission electron microscope. Image registration based on the simultaneously acquired high angle annular dark field image significantly outperforms acquisition with a long pixel dwell time or drift correction using a reference image. Non-local Poisson PCA denoising reduces noise more strongly than conventional weighted PCA while preserving atomic structure more faithfully. The reliability of and optimal internal parameters for non-local Poisson PCA denoising of EDS spectrum images is assessed using tests on phantom data.

  17. Pre-embedding Method of Electron Microscopy for Glycan Localization in Mammalian Tissues and Cells Using Lectin Probes.

    PubMed

    Akimoto, Yoshihiro; Takata, Kuniaki; Kawakami, Hayato

    2016-01-01

    In recent years, the study of glycans is progressing remarkably by the development of glycan analysis systems using mass spectrometry, glycan profiling systems using lectin microarrays, and glycoprotein analysis by the isotope-coded glycosylation site-specific tagging method. With these methodologies, glycan structures and biological functions are being elucidated. In the study of glycan function as well as disease diagnosis, it is important to examine the localization of glycans in tissues and cells. Histochemical methods using lectin probes can localize glycans in the tissues and cells. This chapter describes a pre-embedding electron microscopic method for glycan localization in which tissue sections and cells are incubated with lectin prior to embedding in resin. PMID:27515086

  18. Global functions in global-local finite-element analysis of localized stresses in prismatic structures

    NASA Technical Reports Server (NTRS)

    Dong, Stanley B.

    1989-01-01

    An important consideration in the global local finite-element method (GLFEM) is the availability of global functions for the given problem. The role and mathematical requirements of these global functions in a GLFEM analysis of localized stress states in prismatic structures are discussed. A method is described for determining these global functions. Underlying this method are theorems due to Toupin and Knowles on strain energy decay rates, which are related to a quantitative expression of Saint-Venant's principle. It is mentioned that a mathematically complete set of global functions can be generated, so that any arbitrary interface condition between the finite element and global subregions can be represented. Convergence to the true behavior can be achieved with increasing global functions and finite-element degrees of freedom. Specific attention is devoted to mathematically two-dimensional and three-dimensional prismatic structures. Comments are offered on the GLFEM analysis of NASA flat panel with a discontinuous stiffener. Methods for determining global functions for other effects are also indicated, such as steady-state dynamics and bodies under initial stress.

  19. Electron and Hole States in Low Dimensional Structures

    NASA Astrophysics Data System (ADS)

    Edwards, Gerard

    Available from UMI in association with The British Library. In this thesis results from microscopic calculations for the electron and hole states in low dimensional heterostructures are presented. The basis for the calculation is the local empirical pseudopotential technique which is used to generate the bulk semiconductor bandstructure. Then an S matrix approach, which is numerically stable, is employed to propagate the solution through the layered structure. The technique is essentially a scattering approach and hence is suitable to describe the experimental situation of finite samples. The fact that a finite system is treated allows the formalism to be naturally extended to include an external E field. The calculations that have been done are for the (001) growth direction. In chapter 1 the basic concepts of semiconductor physics relevant to the material of this thesis are introduced. In Chapter 2 the theoretical technique used in this thesis, for conduction band states, is reviewed and compared and contrasted with alternative methods. The emergence of miniband states and Stark ladders in coupled GaAs/AlAs quantum well structures are dealt with in chapter 3. In Chapter 4 the bound state problem, relevant to optical properties, of the energy versus k_parallel subband dispersion of a AlGaAs-GaAs-AlGaAs quantum well is examined. Chapter 5 contains the extension of the theoretical technique to incorporate the spin-orbit interaction so that heterostructure hole states can be tackled. The validity of the effective mass theory treatment of the semiconductor interface and the Luttinger model of the bulk valence band is questioned and the microscopic nature of the GaAs-AlAs interface scattering investigated. In chapter 6 hole states in GaAs/AlAs double barrier structures and coupled multiple quantum well (MQW) structures are calculated. The anomalous formation of contact interface states instead of heavy hole minibands is observed in MQW structures. In chapter 7 In

  20. Local structures surrounding Zr in nanostructurally stabilized cubic zirconia: Structural origin of phase stability

    SciTech Connect

    Soo, Y. L.; Chen, P. J.; Huang, S. H.; Shiu, T. J.; Tsai, T. Y.; Chow, Y. H.; Lin, Y. C.; Weng, S. C.; Chang, S. L.; Wang, G.; Cheung, C. L.; Sabirianov, R. F.; Mei, W. N.; Namavar, F.; Haider, H.; Garvin, K. L.; Lee, J. F.; Lee, H. Y.; Chu, P. P.

    2008-12-01

    Local environment surrounding Zr atoms in the thin films of nanocrystalline zirconia (ZrO{sub 2}) has been investigated by using the extended x-ray absorption fine structure (EXAFS) technique. These films prepared by the ion beam assisted deposition exhibit long-range structural order of cubic phase and high hardness at room temperature without chemical stabilizers. The local structure around Zr probed by EXAFS indicates a cubic Zr sublattice with O atoms located on the nearest tetragonal sites with respect to the Zr central atoms, as well as highly disordered locations. Similar Zr local structure was also found in a ZrO{sub 2} nanocrystal sample prepared by a sol-gel method. Variations in local structures due to thermal annealing were observed and analyzed. Most importantly, our x-ray results provide direct experimental evidence for the existence of oxygen vacancies arising from local disorder and distortion of the oxygen sublattice in nanocrystalline ZrO{sub 2}. These oxygen vacancies are regarded as the essential stabilizing factor for the nanostructurally stabilized cubic zirconia.