Local structural and chemical ordering of nanosized Pt3±δCo probed by multiple-scattering x-ray absorption spectroscopy

NASA Astrophysics Data System (ADS)

Greco, Giorgia; Witkowska, Agnieszka; Principi, Emiliano; Minicucci, Marco; di Cicco, Andrea

2011-04-01

This work reports a detailed investigation of the local structure and chemical disorder of a Pt3±δCo thin film and Pt3±δCo nanoparticles. We have used a combination of techniques including x-ray absorption spectroscopy (XAS), x-ray diffraction (XRD), and high-resolution transmission electron microscopy (TEM). High-quality XAS spectra at the Co K edge and Pt L3 edge have been analyzed using double-edge multiple-scattering data analysis. Structural extended x-ray absorption fine structure (EXAFS) refinements have been performed accounting for the reduction of the coordination numbers and degeneracy of three-atom configurations, resulting from the measured size distribution and stoichiometry. The important effect of chemical ordering on pair and three-atom configurations has been studied using computer simulations based on a simple model accounting for substitutional disorder, defined by an order parameter s. It has been found that individual EXAFS signals related to the minority species (Co) are extremely sensitive to substitutional disorder so their intensities, especially those of the collinear three-atom configurations, can be used as a measure of the ordering level. The thin film has been found to be chemically disordered (s⩽0.4), in agreement with previous estimates. The Pt3±δCo nanoalloy has been found to be partially ordered (s=0.6±0.1) while the local structure around Co atoms is characterized by a higher level of structural disorder as compared to the bulk-like thin film. The robust approach for nanomaterial characterization used in this work combining different techniques can, in principle, be applied for structural refinements of any binary nanocrystalline functional system.

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.

SGO: A fast engine for ab initio atomic structure global optimization by differential evolution

NASA Astrophysics Data System (ADS)

Chen, Zhanghui; Jia, Weile; Jiang, Xiangwei; Li, Shu-Shen; Wang, Lin-Wang

2017-10-01

As the high throughout calculations and material genome approaches become more and more popular in material science, the search for optimal ways to predict atomic global minimum structure is a high research priority. This paper presents a fast method for global search of atomic structures at ab initio level. The structures global optimization (SGO) engine consists of a high-efficiency differential evolution algorithm, accelerated local relaxation methods and a plane-wave density functional theory code running on GPU machines. The purpose is to show what can be achieved by combining the superior algorithms at the different levels of the searching scheme. SGO can search the global-minimum configurations of crystals, two-dimensional materials and quantum clusters without prior symmetry restriction in a relatively short time (half or several hours for systems with less than 25 atoms), thus making such a task a routine calculation. Comparisons with other existing methods such as minima hopping and genetic algorithm are provided. One motivation of our study is to investigate the properties of magnetic systems in different phases. The SGO engine is capable of surveying the local minima surrounding the global minimum, which provides the information for the overall energy landscape of a given system. Using this capability we have found several new configurations for testing systems, explored their energy landscape, and demonstrated that the magnetic moment of metal clusters fluctuates strongly in different local minima.

Controlling the delocalization-localization transition of light via electromagnetically induced transparency

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cheng Jing; Huang Guoxiang; State Key Laboratory of Precision Spectroscopy, East China Normal University, Shanghai 200062

2011-05-15

We propose a scheme to realize a transition from delocalization to localization of light waves via electromagnetically induced transparency. The system we suggested is a resonant cold atomic ensemble having N configuration, with a control field consisting of two pairs of laser beams with different cross angles, which produce an electromagnetically induced quasiperiodic waveguide (EIQPW) for the propagation of a signal field. By appropriately tuning the incommensurate rate or relative modulation strength between the two pairs of control-field components, the signal field can exhibit the delocalization-localization transition as it transports inside the atomic ensemble. The delocalization-localization transition point is determinedmore » and the propagation property of the signal field is studied in detail. Our work provides a way of realizing wave localization via atomic coherence, which is quite different from the conventional, off-resonant mechanism-based Aubry-Andre model, and the great controllability of the EIQPW also allows an easy manipulation of the delocalization-localization transition.« less

Interactive Web-based Visualization of Atomic Position-time Series Data

NASA Astrophysics Data System (ADS)

Thapa, S.; Karki, B. B.

2017-12-01

Extracting and interpreting the information contained in large sets of time-varying three dimensional positional data for the constituent atoms of simulated material is a challenging task. We have recently implemented a web-based visualization system to analyze the position-time series data extracted from the local or remote hosts. It involves a pre-processing step for data reduction, which involves skipping uninteresting parts of the data uniformly (at full atomic configuration level) or non-uniformly (at atomic species level or individual atom level). Atomic configuration snapshot is rendered using the ball-stick representation and can be animated by rendering successive configurations. The entire atomic dynamics can be captured as the trajectories by rendering the atomic positions at all time steps together as points. The trajectories can be manipulated at both species and atomic levels so that we can focus on one or more trajectories of interest, and can be also superimposed with the instantaneous atomic structure. The implementation was done using WebGL and Three.js for graphical rendering, HTML5 and Javascript for GUI, and Elasticsearch and JSON for data storage and retrieval within the Grails Framework. We have applied our visualization system to the simulation datatsets for proton-bearing forsterite (Mg2SiO4) - an abundant mineral of Earths upper mantle. Visualization reveals that protons (hydrogen ions) incorporated as interstitials are much more mobile than protons substituting the host Mg and Si cation sites. The proton diffusion appears to be anisotropic with high mobility along the x-direction, showing limited discrete jumps in other two directions.

Electron Localization States in Asymmetric Shape Carbon Nanotubes Caused by Hydrogen Adsorption

NASA Astrophysics Data System (ADS)

Pan, L. J.; Chen, W. G.

2017-12-01

In this paper, we presented pseudopotential-based density functional theory studies on energy, structure, energy band structure of hydrogenated single-walled carbon nanotube. The stability of the configuration mainly depends on hydrogen coverage. According to the adsorption energies, the stability deteriorates with the increase of the hydrogen adsorption. The cross section of configurations become various shapes such as “beetle” or “lip” appearance without the balanced effects of hydrogen atoms. We also explored the energy band structures of configurations in three typical adsorption patterns, showing that the disparate trends of energy band gap as the hydrogen atoms concentrate. For C32H24, the band gap may reach the large value of 2.79 eV for the adsorption pattern A configuration and reduce to be zero for the adsorption pattern C case, the values of band gap for pattern A configurations decrease, which is opposite of the pattern B configurations as the adsorption hydrogen becomes more disperse. It is deduced that the hydrogen adsorption has significant effect on the electrical properties of the carbon nanotube.

Atomic structure considerations for the low-temperature opacity of Sn

DOE PAGES

Colgan, J.; Kilcrease, D. P.; Abdallah, J.; ...

2017-03-31

Here, we have begun a preliminary investigation into the opacity of Sn at low temperatures (< 50 eV). The emissivity and opacity of Sn is a crucial factor in determining the utility of Sn in EUV lithography, with numerous industrial implications. To this end, we have been exploring the accuracy of some approximations used in opacity models for the relevant ion stages of Sn (neutral through ~ 18 times ionized). We also find that the use of intermediate-coupling, as compared to full configuration-interaction, is not adequate to obtain accurate line positions of the important bound-bound transitions in Sn. One requiresmore » full configuration-interaction to properly describe the strong mixing between the various n=4 sub-shells that give rise to the Δn= 0 transitions that dominate the opacity spectrum at low temperatures. Furthermore, since calculations that include full configuration-interaction for large numbers of configurations quickly become computationally prohibitive, we have explored hybrid calculations, in which full configuration-interaction is retained for the most important transitions, while intermediate-coupling is employed for all other transitions. After extensive exploration of the atomic structure properties, local-thermodynamic-equilibrium (LTE) opacities are generated using the ATOMIC code at selected temperatures and densities and compared to experiment.« less

Atomic structure considerations for the low-temperature opacity of Sn

DOE Office of Scientific and Technical Information (OSTI.GOV)

Colgan, J.; Kilcrease, D. P.; Abdallah, J.

Here, we have begun a preliminary investigation into the opacity of Sn at low temperatures (< 50 eV). The emissivity and opacity of Sn is a crucial factor in determining the utility of Sn in EUV lithography, with numerous industrial implications. To this end, we have been exploring the accuracy of some approximations used in opacity models for the relevant ion stages of Sn (neutral through ~ 18 times ionized). We also find that the use of intermediate-coupling, as compared to full configuration-interaction, is not adequate to obtain accurate line positions of the important bound-bound transitions in Sn. One requiresmore » full configuration-interaction to properly describe the strong mixing between the various n=4 sub-shells that give rise to the Δn= 0 transitions that dominate the opacity spectrum at low temperatures. Furthermore, since calculations that include full configuration-interaction for large numbers of configurations quickly become computationally prohibitive, we have explored hybrid calculations, in which full configuration-interaction is retained for the most important transitions, while intermediate-coupling is employed for all other transitions. After extensive exploration of the atomic structure properties, local-thermodynamic-equilibrium (LTE) opacities are generated using the ATOMIC code at selected temperatures and densities and compared to experiment.« less

Effect of gradual ordering of Ge/Sb atoms on chemical bonding: A proposed mechanism for the formation of crystalline Ge2Sb2Te5

NASA Astrophysics Data System (ADS)

Singh, Janpreet; Singh, Gurinder; Kaura, Aman; Tripathi, S. K.

2018-04-01

Using first principle calculations, we study the atomic arrangement and bonding mechanism in the crystalline phase of Ge2Sb2Te5 (GST). It is found that the stability of GST depends on the gradual ordering of Ge/Sb atoms. The configurations with different concentration of Ge/Sb in layers have been analyzed by the partial density of state, electron localization function and Bader charge distribution. The s and p-states of Ge atom alter with different stacking configurations but there is no change in Sb and Te atom states. Our findings show that the bonding between Ge-Te is not only responsible for the stability of GST alloy but can also predict which composition can show generic features of phase change material. As the number of Ge atoms near to vacancy layer decreases, Ge donates more charge. A growth model has been proposed for the formation of crystalline phase which justifies the structure models proposed in the literature.

Learning molecular energies using localized graph kernels.

PubMed

Ferré, Grégoire; Haut, Terry; Barros, Kipton

2017-03-21

Recent machine learning methods make it possible to model potential energy of atomic configurations with chemical-level accuracy (as calculated from ab initio calculations) and at speeds suitable for molecular dynamics simulation. Best performance is achieved when the known physical constraints are encoded in the machine learning models. For example, the atomic energy is invariant under global translations and rotations; it is also invariant to permutations of same-species atoms. Although simple to state, these symmetries are complicated to encode into machine learning algorithms. In this paper, we present a machine learning approach based on graph theory that naturally incorporates translation, rotation, and permutation symmetries. Specifically, we use a random walk graph kernel to measure the similarity of two adjacency matrices, each of which represents a local atomic environment. This Graph Approximated Energy (GRAPE) approach is flexible and admits many possible extensions. We benchmark a simple version of GRAPE by predicting atomization energies on a standard dataset of organic molecules.

Learning molecular energies using localized graph kernels

NASA Astrophysics Data System (ADS)

Ferré, Grégoire; Haut, Terry; Barros, Kipton

2017-03-01

Recent machine learning methods make it possible to model potential energy of atomic configurations with chemical-level accuracy (as calculated from ab initio calculations) and at speeds suitable for molecular dynamics simulation. Best performance is achieved when the known physical constraints are encoded in the machine learning models. For example, the atomic energy is invariant under global translations and rotations; it is also invariant to permutations of same-species atoms. Although simple to state, these symmetries are complicated to encode into machine learning algorithms. In this paper, we present a machine learning approach based on graph theory that naturally incorporates translation, rotation, and permutation symmetries. Specifically, we use a random walk graph kernel to measure the similarity of two adjacency matrices, each of which represents a local atomic environment. This Graph Approximated Energy (GRAPE) approach is flexible and admits many possible extensions. We benchmark a simple version of GRAPE by predicting atomization energies on a standard dataset of organic molecules.

Atomic fountain clock with very high frequency stability employing a pulse-tube-cryocooled sapphire oscillator.

PubMed

Takamizawa, Akifumi; Yanagimachi, Shinya; Tanabe, Takehiko; Hagimoto, Ken; Hirano, Iku; Watabe, Ken-ichi; Ikegami, Takeshi; Hartnett, John G

2014-09-01

The frequency stability of an atomic fountain clock was significantly improved by employing an ultra-stable local oscillator and increasing the number of atoms detected after the Ramsey interrogation, resulting in a measured Allan deviation of 8.3 × 10(-14)τ(-1/2)). A cryogenic sapphire oscillator using an ultra-low-vibration pulse-tube cryocooler and cryostat, without the need for refilling with liquid helium, was applied as a local oscillator and a frequency reference. High atom number was achieved by the high power of the cooling laser beams and optical pumping to the Zeeman sublevel m(F) = 0 employed for a frequency measurement, although vapor-loaded optical molasses with the simple (001) configuration was used for the atomic fountain clock. The resulting stability is not limited by the Dick effect as it is when a BVA quartz oscillator is used as the local oscillator. The stability reached the quantum projection noise limit to within 11%. Using a combination of a cryocooled sapphire oscillator and techniques to enhance the atom number, the frequency stability of any atomic fountain clock, already established as primary frequency standard, may be improved without opening its vacuum chamber.

First-principles study of structure, electronic properties and stability of tungsten adsorption on TiC(111) surface with disordered vacancies

NASA Astrophysics Data System (ADS)

Ilyasov, Victor V.; Pham, Khang D.; Zhdanova, Tatiana P.; Phuc, Huynh V.; Hieu, Nguyen N.; Nguyen, Chuong V.

2017-12-01

In this paper, we systematically investigate the atomic structure, electronic and thermodynamic properties of adsorbed W atoms on the polar Ti-terminated TixCy (111) surface with different configurations of adsorptions using first principle calculations. The bond length, adsorption energy, and formation energy for different reconstructions of the atomic structure of the W/TixCy (111) systems were established. The effect of the tungsten coverage on the electronic structure and the adsorption mechanism of tungsten atom on the TixCy (111) are also investigated. We also suggest the possible mechanisms of W nucleation on the TixCy (111) surface. The effective charges on W atoms and nearest-neighbor atoms in the examined reconstructions were identified. Additionally, we have established the charge transfer from titanium atom to tungsten and carbon atoms which determine by the reconstruction of the local atomic and electronic structures. Our calculations showed that the charge transfer correlates with the electronegativity of tungsten and nearest-neighbor atoms. We also determined the effective charge per atom of titanium, carbon atoms, and neighboring adsorbed tungsten atom in different binding configurations. We found that, with reduction of the lattice symmetry associated with titanium and carbon vacancies, the adsorption energy increases by 1.2 times in the binding site A of W/TixCy systems.

Interaction between benzenedithiolate and gold: Classical force field for chemical bonding

NASA Astrophysics Data System (ADS)

Leng, Yongsheng; Krstić, Predrag S.; Wells, Jack C.; Cummings, Peter T.; Dean, David J.

2005-06-01

We have constructed a group of classical potentials based on ab initio density-functional theory (DFT) calculations to describe the chemical bonding between benzenedithiolate (BDT) molecule and gold atoms, including bond stretching, bond angle bending, and dihedral angle torsion involved at the interface between the molecule and gold clusters. Three DFT functionals, local-density approximation (LDA), PBE0, and X3LYP, have been implemented to calculate single point energies (SPE) for a large number of molecular configurations of BDT-1, 2 Au complexes. The three DFT methods yield similar bonding curves. The variations of atomic charges from Mulliken population analysis within the molecule/metal complex versus different molecular configurations have been investigated in detail. We found that, except for bonded atoms in BDT-1, 2 Au complexes, the Mulliken partial charges of other atoms in BDT are quite stable, which significantly reduces the uncertainty in partial charge selections in classical molecular simulations. Molecular-dynamics (MD) simulations are performed to investigate the structure of BDT self-assembled monolayer (SAM) and the adsorption geometry of S adatoms on Au (111) surface. We found that the bond-stretching potential is the most dominant part in chemical bonding. Whereas the local bonding geometry of BDT molecular configuration may depend on the DFT functional used, the global packing structure of BDT SAM is quite independent of DFT functional, even though the uncertainty of some force-field parameters for chemical bonding can be as large as ˜100%. This indicates that the intermolecular interactions play a dominant role in determining the BDT SAMs global packing structure.

Interaction between benzenedithiolate and gold: classical force field for chemical bonding.

PubMed

Leng, Yongsheng; Krstić, Predrag S; Wells, Jack C; Cummings, Peter T; Dean, David J

2005-06-22

We have constructed a group of classical potentials based on ab initio density-functional theory (DFT) calculations to describe the chemical bonding between benzenedithiolate (BDT) molecule and gold atoms, including bond stretching, bond angle bending, and dihedral angle torsion involved at the interface between the molecule and gold clusters. Three DFT functionals, local-density approximation (LDA), PBE0, and X3LYP, have been implemented to calculate single point energies (SPE) for a large number of molecular configurations of BDT-1, 2 Au complexes. The three DFT methods yield similar bonding curves. The variations of atomic charges from Mulliken population analysis within the molecule/metal complex versus different molecular configurations have been investigated in detail. We found that, except for bonded atoms in BDT-1, 2 Au complexes, the Mulliken partial charges of other atoms in BDT are quite stable, which significantly reduces the uncertainty in partial charge selections in classical molecular simulations. Molecular-dynamics (MD) simulations are performed to investigate the structure of BDT self-assembled monolayer (SAM) and the adsorption geometry of S adatoms on Au (111) surface. We found that the bond-stretching potential is the most dominant part in chemical bonding. Whereas the local bonding geometry of BDT molecular configuration may depend on the DFT functional used, the global packing structure of BDT SAM is quite independent of DFT functional, even though the uncertainty of some force-field parameters for chemical bonding can be as large as approximately 100%. This indicates that the intermolecular interactions play a dominant role in determining the BDT SAMs global packing structure.

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

DOE PAGES

Belianinov, Alex; Panchapakesan, G.; Lin, Wenzhi; ...

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 signaturemore » 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.« less

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Belianinov, Alex, E-mail: belianinova@ornl.gov; Ganesh, Panchapakesan; Lin, Wenzhi

2014-12-01

Atomic level spatial variability of electronic structure in Fe-based superconductor FeTe{sub 0.55}Se{sub 0.45} (T{sub c} = 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 FeTe{sub 1−x}Se{sub x} structures further confirms that the two types of chalcogens, i.e., Te and Se, can be identified bymore » 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.« less

Atomic scale imaging of magnetic circular dichroism by achromatic electron microscopy.

PubMed

Wang, Zechao; Tavabi, Amir H; Jin, Lei; Rusz, Ján; Tyutyunnikov, Dmitry; Jiang, Hanbo; Moritomo, Yutaka; Mayer, Joachim; Dunin-Borkowski, Rafal E; Yu, Rong; Zhu, Jing; Zhong, Xiaoyan

2018-03-01

In order to obtain a fundamental understanding of the interplay between charge, spin, orbital and lattice degrees of freedom in magnetic materials and to predict and control their physical properties 1-3 , experimental techniques are required that are capable of accessing local magnetic information with atomic-scale spatial resolution. Here, we show that a combination of electron energy-loss magnetic chiral dichroism 4 and chromatic-aberration-corrected transmission electron microscopy, which reduces the focal spread of inelastically scattered electrons by orders of magnitude when compared with the use of spherical aberration correction alone, can achieve atomic-scale imaging of magnetic circular dichroism and provide element-selective orbital and spin magnetic moments atomic plane by atomic plane. This unique capability, which we demonstrate for Sr 2 FeMoO 6 , opens the door to local atomic-level studies of spin configurations in a multitude of materials that exhibit different types of magnetic coupling, thereby contributing to a detailed understanding of the physical origins of magnetic properties of materials at the highest spatial resolution.

Three-Dimensional Localized-Delocalized Anderson Transition in the Time Domain

NASA Astrophysics Data System (ADS)

Delande, Dominique; Morales-Molina, Luis; Sacha, Krzysztof

2017-12-01

Systems which can spontaneously reveal periodic evolution are dubbed time crystals. This is in analogy with space crystals that display periodic behavior in configuration space. While space crystals are modeled with the help of space periodic potentials, crystalline phenomena in time can be modeled by periodically driven systems. Disorder in the periodic driving can lead to Anderson localization in time: the probability for detecting a system at a fixed point of configuration space becomes exponentially localized around a certain moment in time. We here show that a three-dimensional system exposed to a properly disordered pseudoperiodic driving may display a localized-delocalized Anderson transition in the time domain, in strong analogy with the usual three-dimensional Anderson transition in disordered systems. Such a transition could be experimentally observed with ultracold atomic gases.

Crafting ferromagnetism in Mn-doped MgO surfaces with p-type defects

PubMed Central

Panigrahi, Puspamitra; Araujo, C Moyses; Hussen, Tanveer; Ahuja, Rajeev

2014-01-01

We have employed first-principles calculations based on density functional theory (DFT) to investigate the underlying physics of unusual magnetism in Mn-doped MgO surface. We have studied two distinct scenarios. In the first one, two Mn atoms are substitutionally added to the surface, occupying the Mg sites. Both are stabilized in the Mn valence state carrying a local moment of 4.3 having a high-spin configuration. The magnetic interaction between the local moments display a very short-ranged characteristic, decaying very quickly with distance, and having antiferromagnetic ordering lower in energy. The energetics analysis also indicates that the Mn ions prefer to stay close to each other with an oxygen atom bridging the local interaction. In the second scenario, we started exploring the effect of native defects on the magnetism by crafting both Mg and O vacancies, which are p- and n-type defects, respectively. It is found that the electrons and holes affect the magnetic interaction between Mn ions in a totally different manner. The n-type defect leads to very similar magnetism, with the AFM configuration being energetically preferred. However, in the presence of Mg vacancy, the situation is quite different. The Mn atoms are further oxidized, giving rise to mixed Mn(d) ionic states. As a consequence, the Mn atoms couple ferromagnetically, when placed in the close configuration, and the obtained electronic structure is coherent with the double-exchange type of magnetic interaction. To guarantee the robustness of our results, we have benchmarked our calculations with three distinct theory levels, namely DFT-GGA, DFT-GGA+U and DFT-hybrid functionals. On the surface, the Mg vacancy displays lower formation energy occurring at higher concentrations. Therefore, our model systems can be the basis to explain a number of controversial results regarding transition metal doped oxides. PMID:27877684

Optimal atomic structure of amorphous silicon obtained from density functional theory calculations

NASA Astrophysics Data System (ADS)

Pedersen, Andreas; Pizzagalli, Laurent; Jónsson, Hannes

2017-06-01

Atomic structure of amorphous silicon consistent with several reported experimental measurements has been obtained from annealing simulations using electron density functional theory calculations and a systematic removal of weakly bound atoms. The excess energy and density with respect to the crystal are well reproduced in addition to radial distribution function, angular distribution functions, and vibrational density of states. No atom in the optimal configuration is locally in a crystalline environment as deduced by ring analysis and common neighbor analysis, but coordination defects are present at a level of 1%-2%. The simulated samples provide structural models of this archetypal disordered covalent material without preconceived notion of the atomic ordering or fitting to experimental data.

Electronic Structures of Silicene Nanoribbons: Two-Edge-Chemistry Modification and First-Principles Study.

PubMed

Yao, Yin; Liu, Anping; Bai, Jianhui; Zhang, Xuanmei; Wang, Rui

2016-12-01

In this paper, we investigate the structural and electronic properties of zigzag silicene nanoribbons (ZSiNRs) with edge-chemistry modified by H, F, OH, and O, using the ab initio density functional theory method and local spin-density approximation. Three kinds of spin polarized configurations are considered: nonspin polarization (NM), ferromagnetic spin coupling for all electrons (FM), ferromagnetic ordering along each edge, and antiparallel spin orientation between the two edges (AFM). The H, F, and OH groups modified 8-ZSiNRs have the AFM ground state. The directly edge oxidized (O1) ZSiNRs yield the same energy and band structure for NM, FM, and AFM configurations, owning to the same s p (2) hybridization. And replacing the Si atoms on the two edges with O atoms (O2) yields FM ground state. The edge-chemistry-modified ZSiNRs all exhibit metallic band structures. And the modifications introduce special edge state strongly localized at the Si atoms in the edge, except for the O1 form. The modification of the zigzag edges of silicene nanoribbons is a key issue to apply the silicene into the field effect transistors (FETs) and gives more necessity to better understand the experimental findings.

Global and local approaches to population analysis: Bonding patterns in superheavy element compounds

NASA Astrophysics Data System (ADS)

Oleynichenko, Alexander; Zaitsevskii, Andréi; Romanov, Stepan; Skripnikov, Leonid V.; Titov, Anatoly V.

2018-03-01

Relativistic effective atomic configurations of superheavy elements Cn, Nh and Fl and their lighter homologues (Hg, Tl and Pb) in their simple compounds with fluorine and oxygen are determined using the analysis of local properties of molecular Kohn-Sham density matrices in the vicinity of heavy nuclei. The difference in populations of atomic spinors with the same orbital angular momentum and different total angular momenta is demonstrated to be essential for understanding the peculiarities of chemical bonding in superheavy element compounds. The results are fully compatible with those obtained by the relativistic iterative version of conventional projection analysis of global density matrices.

Learning molecular energies using localized graph kernels

DOE PAGES

Ferré, Grégoire; Haut, Terry Scot; Barros, Kipton Marcos

2017-03-21

We report that recent machine learning methods make it possible to model potential energy of atomic configurations with chemical-level accuracy (as calculated from ab initio calculations) and at speeds suitable for molecular dynamics simulation. Best performance is achieved when the known physical constraints are encoded in the machine learning models. For example, the atomic energy is invariant under global translations and rotations; it is also invariant to permutations of same-species atoms. Although simple to state, these symmetries are complicated to encode into machine learning algorithms. In this paper, we present a machine learning approach based on graph theory that naturallymore » incorporates translation, rotation, and permutation symmetries. Specifically, we use a random walk graph kernel to measure the similarity of two adjacency matrices, each of which represents a local atomic environment. This Graph Approximated Energy (GRAPE) approach is flexible and admits many possible extensions. Finally, we benchmark a simple version of GRAPE by predicting atomization energies on a standard dataset of organic molecules.« less

Learning molecular energies using localized graph kernels

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ferré, Grégoire; Haut, Terry Scot; Barros, Kipton Marcos

We report that recent machine learning methods make it possible to model potential energy of atomic configurations with chemical-level accuracy (as calculated from ab initio calculations) and at speeds suitable for molecular dynamics simulation. Best performance is achieved when the known physical constraints are encoded in the machine learning models. For example, the atomic energy is invariant under global translations and rotations; it is also invariant to permutations of same-species atoms. Although simple to state, these symmetries are complicated to encode into machine learning algorithms. In this paper, we present a machine learning approach based on graph theory that naturallymore » incorporates translation, rotation, and permutation symmetries. Specifically, we use a random walk graph kernel to measure the similarity of two adjacency matrices, each of which represents a local atomic environment. This Graph Approximated Energy (GRAPE) approach is flexible and admits many possible extensions. Finally, we benchmark a simple version of GRAPE by predicting atomization energies on a standard dataset of organic molecules.« less

Heralded entangling quantum gate via cavity-assisted photon scattering

NASA Astrophysics Data System (ADS)

Borges, Halyne S.; Rossatto, Daniel Z.; Luiz, Fabrício S.; Villas-Boas, Celso J.

2018-01-01

We theoretically investigate the generation of heralded entanglement between two identical atoms via cavity-assisted photon scattering in two different configurations, namely, either both atoms confined in the same cavity or trapped into locally separated ones. Our protocols are given by a very simple and elegant single-step process, the key mechanism of which is a controlled-phase-flip gate implemented by impinging a single photon on single-sided cavities. In particular, when the atoms are localized in remote cavities, we introduce a single-step parallel quantum circuit instead of the serial process extensively adopted in the literature. We also show that such parallel circuit can be straightforwardly applied to entangle two macroscopic clouds of atoms. Both protocols proposed here predict a high entanglement degree with a success probability close to unity for state-of-the-art parameters. Among other applications, our proposal and its extension to multiple atom-cavity systems step toward a suitable route for quantum networking, in particular for quantum state transfer, quantum teleportation, and nonlocal quantum memory.

Identifying local structural states in atomic imaging by computer vision

DOE Office of Scientific and Technical Information (OSTI.GOV)

Laanait, Nouamane; Ziatdinov, Maxim; He, Qian

The availability of atomically resolved imaging modalities enables an unprecedented view into the local structural states of materials, which manifest themselves by deviations from the fundamental assumptions of periodicity and symmetry. Consequently, approaches that aim to extract these local structural states from atomic imaging data with minimal assumptions regarding the average crystallographic configuration of a material are indispensable to advances in structural and chemical investigations of materials. Here, we present an approach to identify and classify local structural states that is rooted in computer vision. This approach introduces a definition of a structural state that is composed of both localmore » and non-local information extracted from atomically resolved images, and is wholly untethered from the familiar concepts of symmetry and periodicity. Instead, this approach relies on computer vision techniques such as feature detection, and concepts such as scale-invariance. We present the fundamental aspects of local structural state extraction and classification by application to simulated scanning transmission electron microscopy images, and analyze the robustness of this approach in the presence of common instrumental factors such as noise, limited spatial resolution, and weak contrast. Finally, we apply this computer vision-based approach for the unsupervised detection and classification of local structural states in an experimental electron micrograph of a complex oxides interface, and a scanning tunneling micrograph of a defect engineered multilayer graphene surface.« less

Identifying local structural states in atomic imaging by computer vision

DOE PAGES

Laanait, Nouamane; Ziatdinov, Maxim; He, Qian; ...

2016-11-02

The availability of atomically resolved imaging modalities enables an unprecedented view into the local structural states of materials, which manifest themselves by deviations from the fundamental assumptions of periodicity and symmetry. Consequently, approaches that aim to extract these local structural states from atomic imaging data with minimal assumptions regarding the average crystallographic configuration of a material are indispensable to advances in structural and chemical investigations of materials. Here, we present an approach to identify and classify local structural states that is rooted in computer vision. This approach introduces a definition of a structural state that is composed of both localmore » and non-local information extracted from atomically resolved images, and is wholly untethered from the familiar concepts of symmetry and periodicity. Instead, this approach relies on computer vision techniques such as feature detection, and concepts such as scale-invariance. We present the fundamental aspects of local structural state extraction and classification by application to simulated scanning transmission electron microscopy images, and analyze the robustness of this approach in the presence of common instrumental factors such as noise, limited spatial resolution, and weak contrast. Finally, we apply this computer vision-based approach for the unsupervised detection and classification of local structural states in an experimental electron micrograph of a complex oxides interface, and a scanning tunneling micrograph of a defect engineered multilayer graphene surface.« less

Chemical Bonding: The Orthogonal Valence-Bond View

PubMed Central

Sax, Alexander F.

2015-01-01

Chemical bonding is the stabilization of a molecular system by charge- and spin-reorganization processes in chemical reactions. These processes are said to be local, because the number of atoms involved is very small. With multi-configurational self-consistent field (MCSCF) wave functions, these processes can be calculated, but the local information is hidden by the delocalized molecular orbitals (MO) used to construct the wave functions. The transformation of such wave functions into valence bond (VB) wave functions, which are based on localized orbitals, reveals the hidden information; this transformation is called a VB reading of MCSCF wave functions. The two-electron VB wave functions describing the Lewis electron pair that connects two atoms are frequently called covalent or neutral, suggesting that these wave functions describe an electronic situation where two electrons are never located at the same atom; such electronic situations and the wave functions describing them are called ionic. When the distance between two atoms decreases, however, every covalent VB wave function composed of non-orthogonal atomic orbitals changes its character from neutral to ionic. However, this change in the character of conventional VB wave functions is hidden by its mathematical form. Orthogonal VB wave functions composed of orthonormalized orbitals never change their character. When localized fragment orbitals are used instead of atomic orbitals, one can decide which local information is revealed and which remains hidden. In this paper, we analyze four chemical reactions by transforming the MCSCF wave functions into orthogonal VB wave functions; we show how the reactions are influenced by changing the atoms involved or by changing their local symmetry. Using orthogonal instead of non-orthogonal orbitals is not just a technical issue; it also changes the interpretation, revealing the properties of wave functions that remain otherwise undetected. PMID:25906476

Atomic structure and glass forming ability of Cu46Zr46Al8 bulk metallic glass

NASA Astrophysics Data System (ADS)

Wang, X. D.; Jiang, Q. K.; Cao, Q. P.; Bednarcik, J.; Franz, H.; Jiang, J. Z.

2008-11-01

By using a combination of state-of-the-art experimental and computational methods, the high glass forming ability (GFA) of Cu46Zr46Al8 alloy is studied from the view of its atomic packing. Three-dimensional atomic configuration is well established. It is found that Al atoms almost homogeneously distribute around Cu and Zr atoms without segregation, causing the local environment around Cu and Zr atoms in Cu46Zr46Al8 bulk metallic glass different from that of the major competing phase of Cu10Zr7. Furthermore, the addition of Al not only increases the amount of icosahedronlike clusters but also makes them more homogeneous distribution, which can enhance the GFA by increasing the structural incompatibility with the competing crystalline phases.

A reactive, scalable, and transferable model for molecular energies from a neural network approach based on local information

NASA Astrophysics Data System (ADS)

Unke, Oliver T.; Meuwly, Markus

2018-06-01

Despite the ever-increasing computer power, accurate ab initio calculations for large systems (thousands to millions of atoms) remain infeasible. Instead, approximate empirical energy functions are used. Most current approaches are either transferable between different chemical systems, but not particularly accurate, or they are fine-tuned to a specific application. In this work, a data-driven method to construct a potential energy surface based on neural networks is presented. Since the total energy is decomposed into local atomic contributions, the evaluation is easily parallelizable and scales linearly with system size. With prediction errors below 0.5 kcal mol-1 for both unknown molecules and configurations, the method is accurate across chemical and configurational space, which is demonstrated by applying it to datasets from nonreactive and reactive molecular dynamics simulations and a diverse database of equilibrium structures. The possibility to use small molecules as reference data to predict larger structures is also explored. Since the descriptor only uses local information, high-level ab initio methods, which are computationally too expensive for large molecules, become feasible for generating the necessary reference data used to train the neural network.

Anisotropic polaron localization and spontaneous symmetry breaking: Comparison of cation-site acceptors in GaN and ZnO

NASA Astrophysics Data System (ADS)

Sun, Y. Y.; Abtew, Tesfaye A.; Zhang, Peihong; Zhang, S. B.

2014-10-01

The behavior of cation substitutional hole doping in GaN and ZnO is investigated using hybrid density functional calculations. Our results reveal that Mg substitution for Ga (MgGa) in GaN can assume three different configurations. Two of the configurations are characterized by the formation of defect-bound small polaron (i.e., a large structural distortion accompanied by hole localization on one of the neighboring N atoms). The third one has a relatively small but significant distortion that is characterized by highly anisotropic polaron localization. In this third configuration, MgGa exhibits both effective-mass-like and noneffective-mass-like characters. In contrast, a similar defect in ZnO, LiZn, cannot sustain the anisotropic polaron in the hybrid functional calculation, but undergoes spontaneous breaking of a mirror symmetry through a mechanism driven by the hole localization. Finally, using NaZn in ZnO as an example, we show that the deep acceptor levels of the small-polaron defects could be made shallower by applying compressive strain to the material.

Atomic-Resolution Spectrum Imaging of Semiconductor Nanowires.

PubMed

Zamani, Reza R; Hage, Fredrik S; Lehmann, Sebastian; Ramasse, Quentin M; Dick, Kimberly A

2018-03-14

Over the past decade, III-V heterostructure nanowires have attracted a surge of attention for their application in novel semiconductor devices such as tunneling field-effect transistors (TFETs). The functionality of such devices critically depends on the specific atomic arrangement at the semiconductor heterointerfaces. However, most of the currently available characterization techniques lack sufficient spatial resolution to provide local information on the atomic structure and composition of these interfaces. Atomic-resolution spectrum imaging by means of electron energy-loss spectroscopy (EELS) in the scanning transmission electron microscope (STEM) is a powerful technique with the potential to resolve structure and chemical composition with sub-angstrom spatial resolution and to provide localized information about the physical properties of the material at the atomic scale. Here, we demonstrate the use of atomic-resolution EELS to understand the interface atomic arrangement in three-dimensional heterostructures in semiconductor nanowires. We observed that the radial interfaces of GaSb-InAs heterostructure nanowires are atomically abrupt, while the axial interface in contrast consists of an interfacial region where intermixing of the two compounds occurs over an extended spatial region. The local atomic configuration affects the band alignment at the interface and, hence, the charge transport properties of devices such as GaSb-InAs nanowire TFETs. STEM-EELS thus represents a very promising technique for understanding nanowire physical properties, such as differing electrical behavior across the radial and axial heterointerfaces of GaSb-InAs nanowires for TFET applications.

Ab initio calculation of diffusion barriers for Cu adatom hopping on Cu(1 0 0) surface and evolution of atomic configurations

NASA Astrophysics Data System (ADS)

Zhang, Wei; Gan, Jie; Li, Qian; Gao, Kun; Sun, Jian; Xu, Ning; Ying, Zhifeng; Wu, Jiada

2011-06-01

The self-diffusion dynamics of Cu adatoms on Cu(1 0 0) surface has been studied based on the calculation of the energy barriers for various hopping events using lattice-gas based approach and a modified model. To simplify the description of the interactions and the calculation of the energy barrier, a three-tier hierarchy of description of atomic configurations was conceived in which the active adatom and its nearest atoms were chosen to constitute basic configuration and taken as a whole to study many-body interactions of the atoms in various atomic configurations, whereas the impacts of the next nearest atoms on the diffusion of the active adatom were considered as multi-site interactions. Besides the simple hopping of single adatoms, the movements of dimers and trimers as the results of multiple hopping events have also been examined. Taking into account the hopping events of all adatoms, the stability of atomic configurations has been examined and the evolution of atomic configurations has also been analyzed.

Quantum-Mechanical Combinatorial Design of Solids having Target Properties

NASA Astrophysics Data System (ADS)

Zunger, Alex

2007-03-01

(1) One of the most striking aspects of solid state physics is the diversity of structural forms in which crystals appear in Nature. Not only are there many distinct crystal-types, but combinations of two or more crystalline materials (alloys) give rise to various local geometric atomic patters. The already rich repertoire of such forms has recently been significantly enhanced by the advent of artificial crystal growth techniques (MBE, STM- atom positioning, etc.) that can create desired structural forms, such as superlattices and impurity clusters even in defiance of the rules of equilibrium thermodynamics. (2) At the same time, the fields of chemistry of nanostructures and physics of structural phase-transitions have long revealed that different atomic configurations generally lead to different physical properties even without altering the chemical makeup. While the most widely - known illustration of such ``form controls function'' rule is the dramatically different color, conductivity and hardness of the allotropical forms of pure carbon (diamond,graphite, C60), the physics of semiconductor superstructures and nanostructures is full of striking examples of how optical, magnetic and transport properties depend sensitively on atomic configuration. (3) Yet, the history of material research has generally occurred via accidental discoveries of material structures having interesting physical property (semiconductivity, ferromagnetism; superconductivity etc.). This begs the question: can this discovery process be inverted, i.e. can we first articulate a desired target physical property, then search (within a class) for the configuration that has this property? (4) The number of potentially interesting atomic configurations exhibits a combinatorial explosion, so even fast synthesis or fast computations can not survey all. (5) This talk describes the recent steps made by solid state theory + computational physics to address this ``Inverse Design'' (Franceschetti & Zunger, Nature, 402, 60 (1999) problem. I will show how Genetic Algorithms, in combination with efficient (``Order N'') solutions to the Pseudopotential Schrodinger equation allow us to investigate astronomical spaces of atomic configurations in search of the structure with a target physical property. Only a small fraction of all (˜ 10**14 in our case) configurations need to be examined. Physical properties are either calculated on-the-fly (if it's easy), or first ``Cluster-Expanded'' (if the theory is difficult). I will illustrate this Inverse Band Structure approach for (a) Design of required band-gaps in semiconductor superlattices; (b) architecture of impurity --clusters with desired optical properties (PRL 97, 046401, 2006) (c) search for configuration of magnetic ions in semiconductors that maximize the ferromagnetic Curie temperature (PRL, 97, 047202, 2006).

Ab initio local-energy and local-stress analysis of tensile behaviours of tilt grain boundaries in Al and Cu

NASA Astrophysics Data System (ADS)

Wang, Hao; Kohyama, Masanori; Tanaka, Shingo; Shiihara, Yoshinori

2017-01-01

Tensile deformation and failure of Σ9 tilt grain boundaries (GBs) in Al and Cu have been examined by first-principles tensile tests (FPTTs). Local-energy and local-stress schemes were applied to clarify the variations of local energies and local hydrostatic stresses for all atoms during the deformation process. The GBs in Al and Cu exhibited quite different tensile behaviours in the FPTTs, despite their similar initial configurations. For the Al GB, there are two stages of deformation before failure. In the first stage, the back bonds of the interfacial bonds are mainly stretched, due to special high strength of the interfacial reconstructed bonds. In the second stage, the interfacial bonds begin to be significantly stretched due to high concentrated stresses, while stretching of the back bonds is suppressed. The atoms at the interfacial, back and bulk bonds have very different variations of local energies and local stresses during each stage, because the behaviour of each atom is significantly dependent on each local structural change due to the high sensitivity of sp electrons to the local environment in Al. The Cu GB has much higher tensile strength, and a natural introduction of stacking faults (SFs) occurs via the {111}< 112> shear slip in the bulk regions between the interfaces before the maximum stress is reached. This is caused by the smaller SF energy and lower ideal shear strength of Cu than Al, and is triggered by highly accumulated local energies and stress at the interface atoms. The local-energy distribution around the SF is consistent with the previous theoretical estimation. After the introduction of the SF, the local energies and stresses of all the atoms in the Cu GB supercell tend to become similar to each other during the tensile process, in contrast to the inhomogeneity in the Al GB. The origins of the different tensile behaviours observed for Al and Cu GBs are discussed with respect to the different bonding natures of Al and Cu, which are dominated by three sp valence electrons per atom for Al and by fully occupied d bands and s electrons for Cu.

Balancing Newtonian gravity and spin to create localized structures

NASA Astrophysics Data System (ADS)

Bush, Michael; Lindner, John

2015-03-01

Using geometry and Newtonian physics, we design localized structures that do not require electromagnetic or other forces to resist implosion or explosion. In two-dimensional Euclidean space, we find an equilibrium configuration of a rotating ring of massive dust whose inward gravity is the centripetal force that spins it. We find similar solutions in three-dimensional Euclidean and hyperbolic spaces, but only in the limit of vanishing mass. Finally, in three-dimensional Euclidean space, we generalize the two-dimensional result by finding an equilibrium configuration of a spherical shell of massive dust that supports itself against gravitational collapse by spinning isoclinically in four dimensions so its three-dimensional acceleration is everywhere inward. These Newtonian ``atoms'' illuminate classical physics and geometry.

Topology, edge states, and zero-energy states of ultracold atoms in one-dimensional optical superlattices with alternating on-site potentials or hopping coefficients

NASA Astrophysics Data System (ADS)

He, Yan; Wright, Kevin; Kouachi, Said; Chien, Chih-Chun

2018-02-01

One-dimensional superlattices with periodic spatial modulations of onsite potentials or tunneling coefficients can exhibit a variety of properties associated with topology or symmetry. Recent developments of ring-shaped optical lattices allow a systematic study of those properties in superlattices with or without boundaries. While superlattices with additional modulating parameters are shown to have quantized topological invariants in the augmented parameter space, we also found localized or zero-energy states associated with symmetries of the Hamiltonians. Probing those states in ultracold atoms is possible by utilizing recently proposed methods analyzing particle depletion or the local density of states. Moreover, we summarize feasible realizations of configurable optical superlattices using currently available techniques.

Rapid insights from remote sensing in the geosciences

NASA Astrophysics Data System (ADS)

Plaza, Antonio

2015-03-01

The growing availability of capacity computing for atomistic materials modeling has encouraged the use of high-accuracy computationally intensive interatomic potentials, such as SNAP. These potentials also happen to scale well on petascale computing platforms. SNAP has a very general form and uses machine-learning techniques to reproduce the energies, forces, and stress tensors of a large set of small configurations of atoms, which are obtained using high-accuracy quantum electronic structure (QM) calculations. The local environment of each atom is characterized by a set of bispectrum components of the local neighbor density projected on to a basis of hyperspherical harmonics in four dimensions. The computational cost per atom is much greater than that of simpler potentials such as Lennard-Jones or EAM, while the communication cost remains modest. We discuss a variety of strategies for implementing SNAP in the LAMMPS molecular dynamics package. We present scaling results obtained running SNAP on three different classes of machine: a conventional Intel Xeon CPU cluster; the Titan GPU-based system; and the combined Sequoia and Vulcan BlueGene/Q. The growing availability of capacity computing for atomistic materials modeling has encouraged the use of high-accuracy computationally intensive interatomic potentials, such as SNAP. These potentials also happen to scale well on petascale computing platforms. SNAP has a very general form and uses machine-learning techniques to reproduce the energies, forces, and stress tensors of a large set of small configurations of atoms, which are obtained using high-accuracy quantum electronic structure (QM) calculations. The local environment of each atom is characterized by a set of bispectrum components of the local neighbor density projected on to a basis of hyperspherical harmonics in four dimensions. The computational cost per atom is much greater than that of simpler potentials such as Lennard-Jones or EAM, while the communication cost remains modest. We discuss a variety of strategies for implementing SNAP in the LAMMPS molecular dynamics package. We present scaling results obtained running SNAP on three different classes of machine: a conventional Intel Xeon CPU cluster; the Titan GPU-based system; and the combined Sequoia and Vulcan BlueGene/Q. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corp., for the U.S. Dept. of Energy's National Nuclear Security Admin. under Contract DE-AC04-94AL85000.

Configurational forces in electronic structure calculations using Kohn-Sham density functional theory

NASA Astrophysics Data System (ADS)

Motamarri, Phani; Gavini, Vikram

2018-04-01

We derive the expressions for configurational forces in Kohn-Sham density functional theory, which correspond to the generalized variational force computed as the derivative of the Kohn-Sham energy functional with respect to the position of a material point x . These configurational forces that result from the inner variations of the Kohn-Sham energy functional provide a unified framework to compute atomic forces as well as stress tensor for geometry optimization. Importantly, owing to the variational nature of the formulation, these configurational forces inherently account for the Pulay corrections. The formulation presented in this work treats both pseudopotential and all-electron calculations in a single framework, and employs a local variational real-space formulation of Kohn-Sham density functional theory (DFT) expressed in terms of the nonorthogonal wave functions that is amenable to reduced-order scaling techniques. We demonstrate the accuracy and performance of the proposed configurational force approach on benchmark all-electron and pseudopotential calculations conducted using higher-order finite-element discretization. To this end, we examine the rates of convergence of the finite-element discretization in the computed forces and stresses for various materials systems, and, further, verify the accuracy from finite differencing the energy. Wherever applicable, we also compare the forces and stresses with those obtained from Kohn-Sham DFT calculations employing plane-wave basis (pseudopotential calculations) and Gaussian basis (all-electron calculations). Finally, we verify the accuracy of the forces on large materials systems involving a metallic aluminum nanocluster containing 666 atoms and an alkane chain containing 902 atoms, where the Kohn-Sham electronic ground state is computed using a reduced-order scaling subspace projection technique [P. Motamarri and V. Gavini, Phys. Rev. B 90, 115127 (2014), 10.1103/PhysRevB.90.115127].

Correlation between the band gap expansion and melting temperature depression of nanostructured semiconductors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, Jianwei, E-mail: jwl189@163.com; Zhao, Xinsheng; Liu, Xinjuan

The band gap and melting temperature of a semiconductor are tunable with the size and shape of the specimen at the nanometer scale, and related mechanisms remain as yet unclear. In order to understand the common origin of the size and shape effect on these two seemingly irrelevant properties, we clarify, correlate, formulate, and quantify these two properties of GaAs, GaN, InP, and InN nanocrystals from the perspectives of bond order-length-strength correlation using the core-shell configuration. The consistency in the theoretical predictions, experimental observations, and numerical calculations verify that the broken-bond-induced local bond contraction and strength gain dictates the bandmore » gap expansion, while the atomic cohesive energy loss due to bond number reduction depresses the melting point. The fraction of the under-coordinated atoms in the skin shell quantitatively determines the shape and size dependency. The atomic under-coordination in the skin down to a depth of two atomic layers inducing a change in the local chemical bond is the common physical origin.« less

Data-Driven Learning of Total and Local Energies in Elemental Boron

NASA Astrophysics Data System (ADS)

Deringer, Volker L.; Pickard, Chris J.; Csányi, Gábor

2018-04-01

The allotropes of boron continue to challenge structural elucidation and solid-state theory. Here we use machine learning combined with random structure searching (RSS) algorithms to systematically construct an interatomic potential for boron. Starting from ensembles of randomized atomic configurations, we use alternating single-point quantum-mechanical energy and force computations, Gaussian approximation potential (GAP) fitting, and GAP-driven RSS to iteratively generate a representation of the element's potential-energy surface. Beyond the total energies of the very different boron allotropes, our model readily provides atom-resolved, local energies and thus deepened insight into the frustrated β -rhombohedral boron structure. Our results open the door for the efficient and automated generation of GAPs, and other machine-learning-based interatomic potentials, and suggest their usefulness as a tool for materials discovery.

Data-Driven Learning of Total and Local Energies in Elemental Boron.

PubMed

Deringer, Volker L; Pickard, Chris J; Csányi, Gábor

2018-04-13

The allotropes of boron continue to challenge structural elucidation and solid-state theory. Here we use machine learning combined with random structure searching (RSS) algorithms to systematically construct an interatomic potential for boron. Starting from ensembles of randomized atomic configurations, we use alternating single-point quantum-mechanical energy and force computations, Gaussian approximation potential (GAP) fitting, and GAP-driven RSS to iteratively generate a representation of the element's potential-energy surface. Beyond the total energies of the very different boron allotropes, our model readily provides atom-resolved, local energies and thus deepened insight into the frustrated β-rhombohedral boron structure. Our results open the door for the efficient and automated generation of GAPs, and other machine-learning-based interatomic potentials, and suggest their usefulness as a tool for materials discovery.

Universal structural parameter to quantitatively predict metallic glass properties

DOE PAGES

Ding, Jun; Cheng, Yong-Qiang; Sheng, Howard; ...

2016-12-12

Quantitatively correlating the amorphous structure in metallic glasses (MGs) with their physical properties has been a long-sought goal. Here we introduce flexibility volume' as a universal indicator, to bridge the structural state the MG is in with its properties, on both atomic and macroscopic levels. The flexibility volume combines static atomic volume with dynamics information via atomic vibrations that probe local configurational space and interaction between neighbouring atoms. We demonstrate that flexibility volume is a physically appropriate parameter that can quantitatively predict the shear modulus, which is at the heart of many key properties of MGs. Moreover, the new parametermore » correlates strongly with atomic packing topology, and also with the activation energy for thermally activated relaxation and the propensity for stress-driven shear transformations. These correlations are expected to be robust across a very wide range of MG compositions, processing conditions and length scales.« less

Hexapole-compensated magneto-optical trap on a mesoscopic atom chip

DOE Office of Scientific and Technical Information (OSTI.GOV)

Joellenbeck, S.; Mahnke, J.; Randoll, R.

2011-04-15

Magneto-optical traps on atom chips are usually restricted to small atomic samples due to a limited capture volume caused primarily by distorted field configurations. Here we present a magneto-optical trap based on a millimeter-sized wire structure which generates a magnetic field with minimized distortions. Together with the loading from a high-flux two-dimensional magneto-optical trap, we achieve a loading rate of 8.4x10{sup 10} atoms/s and maximum number of 8.7x10{sup 9} captured atoms. The wire structure is placed outside of the vacuum to enable a further adaptation to new scientific objectives. Since all magnetic fields are applied locally without the need formore » external bias fields, the presented setup will facilitate parallel generation of Bose-Einstein condensates on a conveyor belt with a cycle rate above 1 Hz.« less

Structural features of small benzene clusters (C6H6)n (n ≤ 30) as investigated with the all-atom OPLS potential.

PubMed

Takeuchi, Hiroshi

2012-10-18

The structures of the simplest aromatic clusters, benzene clusters (C(6)H(6))(n), are not well elucidated. In the present study, benzene clusters (C(6)H(6))(n) (n ≤ 30) were investigated with the all-atom optimized parameters for liquid simulation (OPLS) potential. The global minima and low-lying minima of the benzene clusters were searched with the heuristic method combined with geometrical perturbations. The structural features and growth sequence of the clusters were examined by carrying out local structure analyses and structural similarity evaluation with rotational constants. Because of the anisotropic interaction between the benzene molecules, the local structures consisting of 13 molecules are considerably deviated from regular icosahedron, and the geometries of some of the clusters are inconsistent with the shapes constructed by the interior molecules. The distribution of the angle between the lines normal to two neighboring benzene rings is anisotropic in the clusters, whereas that in the liquid benzene is nearly isotropic. The geometries and energies of the low-lying configurations and the saddle points between them suggest that most of the configurations previously detected in supersonic expansions take different orientations for one to four neighboring molecules.

Electronic structure of metals and semiconductors: bulk, surface, and interface properties

DOE Office of Scientific and Technical Information (OSTI.GOV)

Louie, S.G.S.

1976-09-01

A theoretical study of the electronic structure of various metals and semiconductors is presented with the emphasis on understanding the properties of these materials when they are subjected to extreme conditions and in various different configurations. Among the bulk systems studied, the properties of cesium under high pressure are discussed in terms of the electronic structure calculated at various cell volumes using the pseudopotential method. Local fields or umklapp processes in semiconductors are studied within the random phase approximation (RPA). Specifically the dielectric response matrix epsilon/sub GG'/ (q = 0,omega) is evaluated numerically to determine the effects of local-field correctionsmore » in the optical spectrum of Si. Also, some comments on the excitonic mechanism of superconductivity are presented and the role of local fields is discussed. The pseudo-potential method is next extended to calculate the electronic structure of a transition metal Nb. The calculation is performed self-consistently with the use of a non-local ionic potential determined from atomic spectra. Finally the theory of the superconducting transition temperature T/sub c/ is discussed in the strong-coupling formulation of the BCS theory. The Eliashberg equations in the Matsubara representation are solved analytically and a general T/sub c/ equation is obtained. A new method is developed using pseudopotentials in a self-consistent manner to describe non-periodic systems. The method is applicable to localized configurations such as molecules, surfaces, impurities, vacancies, finite chains of atoms, adsorbates, and solid interfaces. Specific applications to surfaces, metal-semiconductor interfaces and vacancies are presented.« less

Measurement of local structural configurations associated with reversible photostructural changes in arsenic trisulfide films

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yang, C.Y.; Paesler, M.A.; Sayers, D.E.

1987-12-15

Extended x-ray-absorption fine-structure measurements have been made on three reversible and reproducible cycles of thermally annealed and light-soaked amorphous As/sub 2/S/sub 3/ films. Associated with the light-soaked material are (1) a very small increase in the population of wrong bonds in the first shell, (2) an enlarged As: S: As bond angle with an expansion of As: As distance in the second shell, (3) a larger spread in the distribution of As: S: As bond angles, and (4) an absence of any change in the third As: S shell. From these data, we present the first quantitative correlation between observedmore » local atomic structural changes and measured macroscopic properties that are associated with photodarkening. Our data demonstrate that the photoinduced structural changes mainly involve bonding alterations at S atoms as well as a change in the dihedral angle relationship between adjacent AsS/sub 3/ pyramids joined at S atoms.« less

Cooling rate dependence and local structure in aluminum monatomic metallic glass

NASA Astrophysics Data System (ADS)

Kbirou, M.; Trady, S.; Hasnaoui, A.; Mazroui, M.

2017-10-01

The local atomic structure in aluminium monatomic metallic glass is studied using molecular dynamics simulations combined with the embedded atom method (EAM). We have used a variety of analytical methods to characterise the atomic configurations of our system: the Pair Distribution Function (PDF), the Common Neighbour Analysis (CNA) and the Voronoi Tessellation Analysis. CNA was used to investigate the order change from liquid to amorphous phases, recognising that the amount of icosahedral clusters increases with the decrease of temperature. The Voronoi analysis revealed that the icosahedral-like polyhedral are the predominant ones. It has been observed that the PDF function shows a splitting in the second peak, which cannot be attributed to the only ideal icosahedral polyhedron 〈0, 0, 12, 0〉, but also to the formation of other Voronoi polyhedra 〈0, 1, 10, 2〉 . Further, the PDFs were then integrated giving the cumulative coordination number in order to compute the fractal dimension (df).

Real-space identification of intermolecular bonding with atomic force microscopy.

PubMed

Zhang, Jun; Chen, Pengcheng; Yuan, Bingkai; Ji, Wei; Cheng, Zhihai; Qiu, Xiaohui

2013-11-01

We report a real-space visualization of the formation of hydrogen bonding in 8-hydroxyquinoline (8-hq) molecular assemblies on a Cu(111) substrate, using noncontact atomic force microscopy (NC-AFM). The atomically resolved molecular structures enable a precise determination of the characteristics of hydrogen bonding networks, including the bonding sites, orientations, and lengths. The observation of bond contrast was interpreted by ab initio density functional calculations, which indicated the electron density contribution from the hybridized electronic state of the hydrogen bond. Intermolecular coordination between the dehydrogenated 8-hq and Cu adatoms was also revealed by the submolecular resolution AFM characterization. The direct identification of local bonding configurations by NC-AFM would facilitate detailed investigations of intermolecular interactions in complex molecules with multiple active sites.

Theory of carbon nanocones: mechanical chiral inversion of a micron-scale three-dimensional object.

PubMed

Jordan, Stephen P; Crespi, Vincent H

2004-12-17

Graphene cones have two degenerate configurations: their original shape and its inverse. When the apex is depressed by an external probe, the simulated mechanical response is highly nonlinear, with a broad constant-force mode appearing after a short initial Hooke's law regime. For chiral cones, the final state is an atomically exact chiral invert of the original system. If the local reflection symmetry of the graphene sheet is broken by the chemisorption of just five hydrogen atoms to the apex, then the maximal yield strength of the cone increases by approximately 40%. The high symmetry of the conical geometry can concentrate micron-scale mechanical work with atomic precision, providing a way to activate specific chemical bonds.

Predicting Atomic Decay Rates Using an Informational-Entropic Approach

NASA Astrophysics Data System (ADS)

Gleiser, Marcelo; Jiang, Nan

2018-06-01

We show that a newly proposed Shannon-like entropic measure of shape complexity applicable to spatially-localized or periodic mathematical functions known as configurational entropy (CE) can be used as a predictor of spontaneous decay rates for one-electron atoms. The CE is constructed from the Fourier transform of the atomic probability density. For the hydrogen atom with degenerate states labeled with the principal quantum number n, we obtain a scaling law relating the n-averaged decay rates to the respective CE. The scaling law allows us to predict the n-averaged decay rate without relying on the traditional computation of dipole matrix elements. We tested the predictive power of our approach up to n = 20, obtaining an accuracy better than 3.7% within our numerical precision, as compared to spontaneous decay tables listed in the literature.

Predicting Atomic Decay Rates Using an Informational-Entropic Approach

NASA Astrophysics Data System (ADS)

Gleiser, Marcelo; Jiang, Nan

2018-02-01

We show that a newly proposed Shannon-like entropic measure of shape complexity applicable to spatially-localized or periodic mathematical functions known as configurational entropy (CE) can be used as a predictor of spontaneous decay rates for one-electron atoms. The CE is constructed from the Fourier transform of the atomic probability density. For the hydrogen atom with degenerate states labeled with the principal quantum number n, we obtain a scaling law relating the n-averaged decay rates to the respective CE. The scaling law allows us to predict the n-averaged decay rate without relying on the traditional computation of dipole matrix elements. We tested the predictive power of our approach up to n = 20, obtaining an accuracy better than 3.7% within our numerical precision, as compared to spontaneous decay tables listed in the literature.

High data rate atom interferometric device

DOEpatents

Biedermann, Grant; McGuinness, Hayden James Evans; Rakholia, Akash

2015-07-21

A light-pulse atomic interferometry (LPAI) apparatus is provided. The LPAI apparatus comprises a vessel, two sets of magnetic coils configured to magnetically confine an atomic vapor in two respective magneto-optical traps (MOTs) within the vessel when activated, and an optical system configured to irradiate the atomic vapor within the vessel with laser radiation that, when suitably tuned, can launch atoms previously confined in each of the MOTs toward the other MOT. In embodiments, the magnetic coils are configured to produce a magnetic field that is non-zero at the midpoint between the traps. In embodiments, the time-of-flight of the launched atoms from one MOT to the other is 12 ms or less. In embodiments, the MOTs are situated approximately 36 mm apart. In embodiments, the apparatus is configured to activate the magnetic coils according to a particular temporal magnetic field gradient profile.

Composition Formulas of Inorganic Compounds in Terms of Cluster Plus Glue Atom Model.

PubMed

Ma, Yanping; Dong, Dandan; Wu, Aimin; Dong, Chuang

2018-01-16

The present paper attempts to identify the molecule-like structural units in inorganic compounds, by applying the so-called "cluster plus glue atom model". This model, originating from metallic glasses and quasi-crystals, describes any structure in terms of a nearest-neighbor cluster and a few outer-shell glue atoms, expressed in the cluster formula [cluster](glue atoms). Similar to the case for normal molecules where the charge transfer occurs within the molecule to meet the commonly known octet electron rule, the octet state is reached after matching the nearest-neighbor cluster with certain outer-shell glue atoms. These kinds of structural units contain information on local atomic configuration, chemical composition, and electron numbers, just as for normal molecules. It is shown that the formulas of typical inorganic compounds, such as fluorides, oxides, and nitrides, satisfy a similar octet electron rule, with the total number of valence electrons per unit formula being multiples of eight.

An assessment of memristor intrinsic fluctuations: a measurement of single atomic motion

NASA Astrophysics Data System (ADS)

Borghetti, Julien; Yang, J. Joshua; Medeiros-Ribeiro, Gilberto; Williams, R. Stanley

2010-03-01

Memristors provides electrically tunable resistance for upcoming non-volatile memory and future neuromorphic computing. One of the key benefits of such a device is its scalability, which can be demonstrated from an architectural perspective as well as from a fundamental physics limit. 4D addressing schemes utilizing cross bar structures that can be stacked several layers high above the chip embodies unlimited addressing space. On the other limit, the basic operating principles of memristive devices allow one to reach storage of information in a single atom. In this report of nanoscale (sub 50nm) devices, we detect single atom fluctuations, which would then represent the ultimate limit for noise sources thus delineating the boundary conditions for circuit design. We show that electrically induced individual atom migrations do not affect the overall device atomic configuration until a critical bias where a single local fluctuation triggers a general atomic reconfiguration. This instability illustrates the robustness of the device non-volatility upon small electrical stress.

Energy landscapes for a machine learning application to series data

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ballard, Andrew J.; Stevenson, Jacob D.; Das, Ritankar

2016-03-28

Methods developed to explore and characterise potential energy landscapes are applied to the corresponding landscapes obtained from optimisation of a cost function in machine learning. We consider neural network predictions for the outcome of local geometry optimisation in a triatomic cluster, where four distinct local minima exist. The accuracy of the predictions is compared for fits using data from single and multiple points in the series of atomic configurations resulting from local geometry optimisation and for alternative neural networks. The machine learning solution landscapes are visualised using disconnectivity graphs, and signatures in the effective heat capacity are analysed in termsmore » of distributions of local minima and their properties.« less

Inherent structures of crystalline pentacene

NASA Astrophysics Data System (ADS)

Della Valle, Raffaele Guido; Venuti, Elisabetta; Brillante, Aldo; Girlando, Alberto

2003-01-01

Using a quasi-Monte Carlo scheme, we search the potential energy surface of crystalline pentacene to sample its local minima, which represent the "inherent" structures, i.e., the possible configurations of mechanical equilibrium. The system is described in terms of rigid molecules interacting through a standard atom-atom potential model. Several hundreds of distinct minima are encountered, with a surprising variety of structural arrangements. We find that deep minima are easily accessible because they exhibit a favorable energy distribution and their attraction basins tend to be wide. Thanks to these features of the potential surface, the localization the global minimum becomes entirely feasible, allowing reliable a priori predictions of the crystallographic structures. The results for pentacene are very satisfactory. In fact, the two deepest minima correspond to the structures of the two known experimental polymorphs, which are described correctly. Further polymorphs are also likely to exist.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Levin, I.; Krayzman, V.; Woicik, J. C.

Local structures in cubic perovskite-type (Ba 0.6Bi 0.4)(Ti 0.6Sc 0.4)O 3 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-centermore » 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 kVmm -1.« less

Density effects on electronic configurations in dense plasmas

NASA Astrophysics Data System (ADS)

Faussurier, Gérald; Blancard, Christophe

2018-02-01

We present a quantum mechanical model to describe the density effects on electronic configurations inside a plasma environment. Two different approaches are given by starting from a quantum average-atom model. Illustrations are shown for an aluminum plasma in local thermodynamic equilibrium at solid density and at a temperature of 100 eV and in the thermodynamic conditions of a recent experiment designed to characterize the effects of the ionization potential depression treatment. Our approach compares well with experiment and is consistent in that case with the approach of Stewart and Pyatt to describe the ionization potential depression rather than with the method of Ecker and Kröll.

Atomic data and line intensities for the S V ion

NASA Astrophysics Data System (ADS)

Iorga, C.; Stancalie, V.

2017-05-01

The energy levels, oscillator strengths, spontaneous radiative decay rates, lifetimes and electron impact collision strengths have been obtained for the [ Ne ] 3s nl, [ Ne ] 3p nl, [ Ne ] 3d nl configurations belonging to S V ion, with n ≤ 7 and l ≤ 4, resulting in 567 fine-structure levels. The calculations have been performed within the fully relativistic Flexible Atomic Code (FAC, Gu, 2008) framework and the distorted wave approximation. To attain the desired accuracy for the levels energy, the valence-valence and valence-core correlations have been taken care of by including 96 configuration state functions (CSFs) in the model, reaching a total of 3147 fine-structure levels. Two separate calculations have been performed with the local central potential computed for two different average configurations. A third calculation is also performed without the addition of the core-excited states in the atomic model for completeness. The effects of slightly different mean configurations and valence-core correlations on the energy levels and decay rates are investigated. The collision data have been computed employing the relativistic distorted-wave method along with the atomic model containing the 96 CSFs and corresponding to the ground state mean configuration. The collision strengths corresponding to excitation from the first four fine-structure levels are given for five energy values of the scattered electron 2.65, 6.18, 11.02, 17.36, 25.43 Rydberg, plus an additional variable small energy value near the threshold. A collisional-radiative model has been employed to solve the rate equations for the populations of the 567 fine-structure levels, for a temperature of LogTE(K) = 5.2 corresponding to the maximum abundance of S V, and at densities 106-1016cm-3, assuming a Maxwellian electron energy distribution function and black body radiation of temperature 6000 K and dilution factor 0.35 for the photon distribution function. The main processes responsible for the level population variations are the electron-impact collisional excitation and the radiative decay along with their inverse processes. As a result, the level populations along with the spectral high-line intensity ratios are provided.

Giant interfacial perpendicular magnetic anisotropy in Fe/CuIn 1 -xGaxSe2 beyond Fe/MgO

NASA Astrophysics Data System (ADS)

Masuda, Keisuke; Kasai, Shinya; Miura, Yoshio; Hono, Kazuhiro

2017-11-01

We study interfacial magnetocrystalline anisotropies in various Fe/semiconductor heterostructures by means of first-principles calculations. We find that many of those systems show perpendicular magnetic anisotropy (PMA) with a positive value of the interfacial anisotropy constant Ki. In particular, the Fe/CuInSe 2 interface has a large Ki of ˜2.3 mJ /m2 , which is about 1.6 times larger than that of Fe/MgO known as a typical system with relatively large PMA. We also find that the values of Ki in almost all the systems studied in this work follow the well-known Bruno's relation, which indicates that minority-spin states around the Fermi level provide dominant contributions to the interfacial magnetocrystalline anisotropies. Detailed analyses of the local density of states and wave-vector-resolved anisotropy energy clarify that the large Ki in Fe/CuInSe 2 is attributed to the preferable 3 d -orbital configurations around the Fermi level in the minority-spin states of the interfacial Fe atoms. Moreover, we have shown that the locations of interfacial Se atoms are the key for such orbital configurations of the interfacial Fe atoms.

Experimental study of the effect of local atomic ordering on the energy band gap of melt grown InGaAsN alloys

NASA Astrophysics Data System (ADS)

Milanova, M.; Donchev, V.; Kostov, K. L.; Alonso-Álvarez, D.; Valcheva, E.; Kirilov, K.; Asenova, I.; Ivanov, I. G.; Georgiev, S.; Ekins-Daukes, N.

2017-08-01

We present a study of melt grown dilute nitride InGaAsN layers by x-ray photoelectron spectroscopy (XPS), Raman and photoluminescence (PL) spectroscopy. The purpose of the study is to determine the degree of atomic ordering in the quaternary alloy during the epitaxial growth at near thermodynamic equilibrium conditions and its influence on band gap formation. Despite the low In concentration (˜3%) the XPS data show a strong preference toward In-N bonding configuration in the InGaAsN samples. Raman spectra reveal that most of the N atoms are bonded to In instead of Ga atoms and the formation of N-centred In3Ga1 clusters. PL measurements reveal smaller optical band gap bowing as compared to the theoretical predictions for random alloy and localised tail states near the conduction band minimum.

Long range stress correlations in the inherent structures of liquids at rest

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chowdhury, Sadrul; Abraham, Sneha; Hudson, Toby

2016-03-28

Simulation studies of the atomic shear stress in the local potential energy minima (inherent structures) are reported for binary liquid mixtures in 2D and 3D. These inherent structure stresses are fundamental to slow stress relaxation and high viscosity in supercooled liquids. We find that the atomic shear stress in the inherent structures (IS’s) of both liquids at rest exhibits slowly decaying anisotropic correlations. We show that the stress correlations contribute significantly to the variance of the total shear stress of the IS configurations and consider the origins of the anisotropy and spatial extent of the stress correlations.

Local structure in BaTi O 3 - BiSc O 3 dipole glasses

DOE PAGES

Levin, I.; Krayzman, V.; Woicik, J. C.; ...

2016-03-14

Local structures in cubic perovskite-type (Ba 0.6Bi 0.4)(Ti 0.6Sc 0.4)O 3 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-centermore » 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 kVmm -1.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schneeweiss, Oldřich; Friák, Martin; Dudová, Marie

In this paper, we present experimental data showing that the equiatomic CrMnFeCoNi high-entropy alloy undergoes two magnetic transformations at temperatures below 100 K while maintaining its fcc structure down to 3 K. The first transition, paramagnetic to spin glass, was detected at 93 K and the second transition of the ferromagnetic type occurred at 38 K. Field-assisted cooling below 38 K resulted in a systematic vertical shift of the hysteresis curves. Strength and direction of the associated magnetization bias was proportional to the strength and direction of the cooling field and shows a linear dependence with a slope of 0.006more » ± 0.001 emu T. The local magnetic moments of individual atoms in the CrMnFeCoNi quinary fcc random solid solution were investigated by ab initio (electronic density functional theory) calculations. Results of the numerical analysis suggest that, irrespective of the initial configuration of local magnetic moments, the magnetic moments associated with Cr atoms align antiferromagnetically with respect to a cumulative magnetic moment of their first coordination shell. The ab initio calculations further showed that the magnetic moments of Fe and Mn atoms remain strong (between 1.5 and 2 μ B), while the local moments of Ni atoms effectively vanish. Finally, these results indicate that interactions of Mn- and/or Fe-located moments with the surrounding magnetic structure account for the observed macroscopic magnetization bias.« less

Prediction of conformationally dependent atomic multipole moments in carbohydrates

PubMed Central

Cardamone, Salvatore

2015-01-01

The conformational flexibility of carbohydrates is challenging within the field of computational chemistry. This flexibility causes the electron density to change, which leads to fluctuating atomic multipole moments. Quantum Chemical Topology (QCT) allows for the partitioning of an “atom in a molecule,” thus localizing electron density to finite atomic domains, which permits the unambiguous evaluation of atomic multipole moments. By selecting an ensemble of physically realistic conformers of a chemical system, one evaluates the various multipole moments at defined points in configuration space. The subsequent implementation of the machine learning method kriging delivers the evaluation of an analytical function, which smoothly interpolates between these points. This allows for the prediction of atomic multipole moments at new points in conformational space, not trained for but within prediction range. In this work, we demonstrate that the carbohydrates erythrose and threose are amenable to the above methodology. We investigate how kriging models respond when the training ensemble incorporating multiple energy minima and their environment in conformational space. Additionally, we evaluate the gains in predictive capacity of our models as the size of the training ensemble increases. We believe this approach to be entirely novel within the field of carbohydrates. For a modest training set size of 600, more than 90% of the external test configurations have an error in the total (predicted) electrostatic energy (relative to ab initio) of maximum 1 kJ mol−1 for open chains and just over 90% an error of maximum 4 kJ mol−1 for rings. © 2015 Wiley Periodicals, Inc. PMID:26547500

Prediction of conformationally dependent atomic multipole moments in carbohydrates.

PubMed

Cardamone, Salvatore; Popelier, Paul L A

2015-12-15

The conformational flexibility of carbohydrates is challenging within the field of computational chemistry. This flexibility causes the electron density to change, which leads to fluctuating atomic multipole moments. Quantum Chemical Topology (QCT) allows for the partitioning of an "atom in a molecule," thus localizing electron density to finite atomic domains, which permits the unambiguous evaluation of atomic multipole moments. By selecting an ensemble of physically realistic conformers of a chemical system, one evaluates the various multipole moments at defined points in configuration space. The subsequent implementation of the machine learning method kriging delivers the evaluation of an analytical function, which smoothly interpolates between these points. This allows for the prediction of atomic multipole moments at new points in conformational space, not trained for but within prediction range. In this work, we demonstrate that the carbohydrates erythrose and threose are amenable to the above methodology. We investigate how kriging models respond when the training ensemble incorporating multiple energy minima and their environment in conformational space. Additionally, we evaluate the gains in predictive capacity of our models as the size of the training ensemble increases. We believe this approach to be entirely novel within the field of carbohydrates. For a modest training set size of 600, more than 90% of the external test configurations have an error in the total (predicted) electrostatic energy (relative to ab initio) of maximum 1 kJ mol(-1) for open chains and just over 90% an error of maximum 4 kJ mol(-1) for rings. © 2015 Wiley Periodicals, Inc.

Interaction between single gold atom and the graphene edge: A study via aberration-corrected transmission electron microscopy

NASA Astrophysics Data System (ADS)

Wang, Hongtao; Li, Kun; Cheng, Yingchun; Wang, Qingxiao; Yao, Yingbang; Schwingenschlögl, Udo; Zhang, Xixiang; Yang, Wei

2012-04-01

Interaction between single noble metal atoms and graphene edges has been investigated via aberration-corrected and monochromated transmission electron microscopy. A collective motion of the Au atom and the nearby carbon atoms is observed in transition between energy-favorable configurations. Most trapping and detrapping processes are assisted by the dangling carbon atoms, which are more susceptible to knock-on displacements by electron irradiation. Thermal energy is lower than the activation barriers in transition among different energy-favorable configurations, which suggests electron-beam irradiation can be an efficient way of engineering the graphene edge with metal atoms.Interaction between single noble metal atoms and graphene edges has been investigated via aberration-corrected and monochromated transmission electron microscopy. A collective motion of the Au atom and the nearby carbon atoms is observed in transition between energy-favorable configurations. Most trapping and detrapping processes are assisted by the dangling carbon atoms, which are more susceptible to knock-on displacements by electron irradiation. Thermal energy is lower than the activation barriers in transition among different energy-favorable configurations, which suggests electron-beam irradiation can be an efficient way of engineering the graphene edge with metal atoms. Electronic supplementary information (ESI) available: Additional Figures for characterization of mono-layer CVD graphene samples with free edges and Pt atoms decorations and analysis of the effect of electron irradiation; supporting movie on edge evolution. See DOI: 10.1039/c2nr00059h

Deep-subwavelength magnetic-coupling-dominant interaction among magnetic localized surface plasmons

NASA Astrophysics Data System (ADS)

Gao, Zhen; Gao, Fei; Zhang, Youming; Zhang, Baile

2016-05-01

Magnetic coupling is generally much weaker than electric Coulomb interaction. This also applies to the well-known magnetic "meta-atoms," or split-ring resonators (SRRs) as originally proposed by Pendry et al. [IEEE Trans. Microwave Theory Tech. 47, 2075 (1999), 10.1109/22.798002], in which the associated electric dipole moments usually dictate their interaction. As a result, stereometamaterials, a stack of identical SRRs, were found with electric coupling so strong that the dispersion from merely magnetic coupling was overturned. Recently, other workers have proposed a new concept of magnetic localized surface plasmons, supported on metallic spiral structures (MSSs) at a deep-subwavelength scale. Here, we experimentally demonstrate that a stack of these magnetic "meta-atoms" can have dominant magnetic coupling in both of its two configurations. This allows magnetic-coupling-dominant energy transport along a one-dimensional stack of MSSs, as demonstrated with near-field transmission measurement. Our work not only applies this type of magnetic "meta-atom" into metamaterial construction, but also provides possibilities of magnetic metamaterial design in which the electric interaction no longer takes precedence.

Nonlocal torque operators in ab initio theory of the Gilbert damping in random ferromagnetic alloys

NASA Astrophysics Data System (ADS)

Turek, I.; Kudrnovský, J.; Drchal, V.

2015-12-01

We present an ab initio theory of the Gilbert damping in substitutionally disordered ferromagnetic alloys. The theory rests on introduced nonlocal torques which replace traditional local torque operators in the well-known torque-correlation formula and which can be formulated within the atomic-sphere approximation. The formalism is sketched in a simple tight-binding model and worked out in detail in the relativistic tight-binding linear muffin-tin orbital method and the coherent potential approximation (CPA). The resulting nonlocal torques are represented by nonrandom, non-site-diagonal, and spin-independent matrices, which simplifies the configuration averaging. The CPA-vertex corrections play a crucial role for the internal consistency of the theory and for its exact equivalence to other first-principles approaches based on the random local torques. This equivalence is also illustrated by the calculated Gilbert damping parameters for binary NiFe and FeCo random alloys, for pure iron with a model atomic-level disorder, and for stoichiometric FePt alloys with a varying degree of L 10 atomic long-range order.

Vibrational dynamics of thiocyanate and selenocyanate bound to horse heart myoglobin

DOE Office of Scientific and Technical Information (OSTI.GOV)

Maj, Michał; Oh, Younjun; Park, Kwanghee

2014-06-21

The structure and vibrational dynamics of SCN- and SeCN-bound myoglobin have been investigated using polarization-controlled IR pump-probe measurements and quantum chemistry calculations. The complexes are found to be in low and high spin states, with the dominant contribution from the latter. In addition, the Mb:SCN high spin complex exhibits a doublet feature in the thiocyanate stretch IR absorption spectra, indicating two distinct molecular conformations around the heme pocket. The binding mode of the high spin complexes was assigned to occur through the nitrogen atom, contrary to the binding through the sulfur atom that was observed in myoglobin derived from Aplysiamore » Limacina. The vibrational energy relaxation process has been found to occur substantially faster than those of free SCN{sup −} and SeCN{sup −} ions and neutral SCN- and SeCN-derivatized molecules reported previously. This supports the N-bound configurations of MbNCS and MbNCSe, because S- and Se-bound configurations are expected to have significantly long lifetimes due to the insulation effect by heavy bridge atom like S and Se in such IR probes. Nonetheless, even though their lifetimes are much shorter than those of corresponding free ions in water, the vibrational lifetimes determined for MbNCS and MbNCSe are still fairly long compared to those of azide and cyanide myoglobin systems studied before. Thus, thiocyanate and selenocyanate can be good local probes of local electrostatic environment in the heme pocket. The globin dependence on binding mode and vibrational dynamics is also discussed.« less

Conduction of molecular electronic devices: qualitative insights through atom-atom polarizabilities.

PubMed

Stuyver, T; Fias, S; De Proft, F; Fowler, P W; Geerlings, P

2015-03-07

The atom-atom polarizability and the transmission probability at the Fermi level, as obtained through the source-and-sink-potential method for every possible configuration of contacts simultaneously, are compared for polycyclic aromatic compounds. This comparison leads to the conjecture that a positive atom-atom polarizability is a necessary condition for transmission to take place in alternant hydrocarbons without non-bonding orbitals and that the relative transmission probability for different configurations of the contacts can be predicted by analyzing the corresponding atom-atom polarizability. A theoretical link between the two considered properties is derived, leading to a mathematical explanation for the observed trends for transmission based on the atom-atom polarizability.

Elementary excitations and crossover phenomenon in liquids.

PubMed

Iwashita, T; Nicholson, D M; Egami, T

2013-05-17

The elementary excitations of vibration in solids are phonons. But in liquids phonons are extremely short lived and marginalized. In this Letter through classical and ab initio molecular dynamics simulations of the liquid state of various metallic systems we show that different excitations, the local configurational excitations in the atomic connectivity network, are the elementary excitations in high temperature metallic liquids. We also demonstrate that the competition between the configurational excitations and phonons determines the so-called crossover phenomenon in liquids. These discoveries open the way to the explanation of various complex phenomena in liquids, such as fragility and the rapid increase in viscosity toward the glass transition, in terms of these excitations.

Tunneling and traversal of ultracold three-level atoms through vacuum-induced potentials

DOE Office of Scientific and Technical Information (OSTI.GOV)

Badshah, Fazal; Irfan, Muhammad; Qamar, Shahid

2011-09-15

The passage of ultracold three-level atoms through the potential induced by the vacuum cavity mode is discussed using cascade atomic configuration. We study the tunneling or traversal time of the ultracold atoms via a bimodal high-Q cavity. It is found that the phase time, which may be considered as a measure for the time required to traverse the cavity, exhibits superclassical and subclassical behaviors. Further, the dark states and interference effects in cascade atomic configuration may influence the passage time of the atom through the cavity.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stuyver, T.; Fias, S., E-mail: sfias@vub.ac.be; De Proft, F.

The atom-atom polarizability and the transmission probability at the Fermi level, as obtained through the source-and-sink-potential method for every possible configuration of contacts simultaneously, are compared for polycyclic aromatic compounds. This comparison leads to the conjecture that a positive atom-atom polarizability is a necessary condition for transmission to take place in alternant hydrocarbons without non-bonding orbitals and that the relative transmission probability for different configurations of the contacts can be predicted by analyzing the corresponding atom-atom polarizability. A theoretical link between the two considered properties is derived, leading to a mathematical explanation for the observed trends for transmission based onmore » the atom-atom polarizability.« less

Photoemission and x-ray absorption studies of the isostructural to Fe-based superconductors diluted magnetic semiconductor Ba1 -xKx(Zn1 -yMny)2As2

NASA Astrophysics Data System (ADS)

Suzuki, H.; Zhao, K.; Shibata, G.; Takahashi, Y.; Sakamoto, S.; Yoshimatsu, K.; Chen, B. J.; Kumigashira, H.; Chang, F.-H.; Lin, H.-J.; Huang, D. J.; Chen, C. T.; Gu, Bo; Maekawa, S.; Uemura, Y. J.; Jin, C. Q.; Fujimori, A.

2015-04-01

The electronic and magnetic properties of a new diluted magnetic semiconductor (DMS) Ba1 -xKx (Zn1 -yMny )2As2 , which is isostructural to so-called 122-type Fe-based superconductors, are investigated by x-ray absorption spectroscopy (XAS) and resonance photoemission spectroscopy (RPES). Mn L2 ,3-edge XAS indicates that the doped Mn atoms have a valence 2+ and strongly hybridize with the 4 p orbitals of the tetrahedrally coordinating As ligands. The Mn 3 d partial density of states obtained by RPES shows a peak around 4 eV and is relatively high between 0 and 2 eV below the Fermi level (EF) with little contribution at EF, similar to that of the archetypal DMS Ga1 -xMnxAs . This energy level creates a d5 electron configuration with S =5 /2 local magnetic moments at the Mn atoms. Hole carriers induced by K substitution for Ba atoms go into the top of the As 4 p valence band and are weakly bound to the Mn local spins. The ferromagnetic correlation between the local spins mediated by the hole carriers induces ferromagnetism in Ba1 -xKx (Zn1 -yMny )2As2 .

The Full Story of the Electron Configurations of the Transition Elements

ERIC Educational Resources Information Center

Schwarz, W. H. Eugen

2010-01-01

The dominant electronic valence configurations of atoms in chemical substances of a transition element of group "G" in period "n" is ("n" - 1)d[superscript "G"]"n"s[superscript 0]. Transition-metal chemistry is d orbital chemistry. In contrast, the ground states of free, unbound atoms derive, in most cases, from configurations ("n" -…

Magnetic properties of the CrMnFeCoNi high-entropy alloy

DOE PAGES

Schneeweiss, Oldřich; Friák, Martin; Dudová, Marie; ...

2017-07-28

In this paper, we present experimental data showing that the equiatomic CrMnFeCoNi high-entropy alloy undergoes two magnetic transformations at temperatures below 100 K while maintaining its fcc structure down to 3 K. The first transition, paramagnetic to spin glass, was detected at 93 K and the second transition of the ferromagnetic type occurred at 38 K. Field-assisted cooling below 38 K resulted in a systematic vertical shift of the hysteresis curves. Strength and direction of the associated magnetization bias was proportional to the strength and direction of the cooling field and shows a linear dependence with a slope of 0.006more » ± 0.001 emu T. The local magnetic moments of individual atoms in the CrMnFeCoNi quinary fcc random solid solution were investigated by ab initio (electronic density functional theory) calculations. Results of the numerical analysis suggest that, irrespective of the initial configuration of local magnetic moments, the magnetic moments associated with Cr atoms align antiferromagnetically with respect to a cumulative magnetic moment of their first coordination shell. The ab initio calculations further showed that the magnetic moments of Fe and Mn atoms remain strong (between 1.5 and 2 μ B), while the local moments of Ni atoms effectively vanish. Finally, these results indicate that interactions of Mn- and/or Fe-located moments with the surrounding magnetic structure account for the observed macroscopic magnetization bias.« less

Anomalous magnetic configuration of Mn{sub 2}NiAl ribbon and the role of hybridization in the martensitic transformation of Mn{sub 50}Ni{sub 50−x}Al{sub x} ribbons

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhao, R. B.; Department of Physics, Hebei Medical University, Shijiazhuang 050017; Zhao, D. W.

2014-12-08

The magnetic configuration of Mn{sub 2}NiAl ribbon has been investigated. In contrast to Ni{sub 2}MnAl, the compound Mn{sub 2}NiAl with considerable disorder does exhibit ferromagnetism and, due to exchange interaction competition, both ferromagnetic and antiferromagnetic moment orientations can coexist between nearest neighbor Mn atoms. This is unexpected in Heusler alloys. Regarding the mechanism of the martensitic transformation in Mn{sub 50}Ni{sub 50−x}Al{sub x}, it is found that increasing the Al content results in an unusual change in the lattice constant, a decrease of the transformation entropy change, and enhancement of the calculated electron localization. These results indicate that the p-d covalentmore » hybridization between Mn (or Ni) and Al atoms gradually increases at the expense of the d-d hybridization between Ni and Mn atoms. This leads to an increased stability of the austenite phase and a decrease of the martensitic transformation temperature. For 11 ≤ x ≤ 14, Mn{sub 50}Ni{sub 50−x}Al{sub x} ferromagnetic shape memory alloys are obtained.« less

Ferromagnetic properties of manganese doped iron silicide

NASA Astrophysics Data System (ADS)

Ruiz-Reyes, Angel; Fonseca, Luis F.; Sabirianov, Renat

We report the synthesis of high quality Iron silicide (FeSi) nanowires via Chemical Vapor Deposition (CVD). The materials exhibits excellent magnetic response at room temperature, especially when doped with manganese showing values of 2.0 X 10-04 emu for the FexMnySi nanowires. SEM and TEM characterization indicates that the synthesized nanowires have a diameter of approximately 80nm. MFM measurements present a clear description of the magnetic domains when the nanowires are doped with manganese. Electron Diffraction and XRD measurements confirms that the nanowires are single crystal forming a simple cubic structure with space group P213. First-principle calculations were performed on (111) FeSi surface using the Vienna ab initio simulation package (VASP). The exchange correlations were treated under the Ceperley-Alder (CA) local density approximation (LDA). The Brillouin Zone was sampled with 8x8x1 k-point grid. A total magnetic moment of about 10 μB was obtained for three different surface configuration in which the Iron atom nearest to the surface present the higher magnetization. To study the effect of Mn doping, Fe atom was replaced for a Mn. Stronger magnetization is presented when the Mn atom is close to the surface. The exchange coupling constant have been evaluated calculating the energy difference between the ferromagnetic and anti-ferromagnetic configurations.

Simulation study of 3-5 keV x-ray conversion efficiency from Ar K-shell vs. Ag L-shell targets on the National Ignition Facility laser

NASA Astrophysics Data System (ADS)

Kemp, G. E.; Colvin, J. D.; Fournier, K. B.; May, M. J.; Barrios, M. A.; Patel, M. V.; Scott, H. A.; Marinak, M. M.

2015-05-01

Tailored, high-flux, multi-keV x-ray sources are desirable for studying x-ray interactions with matter for various civilian, space and military applications. For this study, we focus on designing an efficient laser-driven non-local thermodynamic equilibrium 3-5 keV x-ray source from photon-energy-matched Ar K-shell and Ag L-shell targets at sub-critical densities (˜nc/10) to ensure supersonic, volumetric laser heating with minimal losses to kinetic energy, thermal x rays and laser-plasma instabilities. Using Hydra, a multi-dimensional, arbitrary Lagrangian-Eulerian, radiation-hydrodynamics code, we performed a parameter study by varying initial target density and laser parameters for each material using conditions readily achievable on the National Ignition Facility (NIF) laser. We employ a model, benchmarked against Kr data collected on the NIF, that uses flux-limited Lee-More thermal conductivity and multi-group implicit Monte-Carlo photonics with non-local thermodynamic equilibrium, detailed super-configuration accounting opacities from Cretin, an atomic-kinetics code. While the highest power laser configurations produced the largest x-ray yields, we report that the peak simulated laser to 3-5 keV x-ray conversion efficiencies of 17.7% and 36.4% for Ar and Ag, respectively, occurred at lower powers between ˜100-150 TW. For identical initial target densities and laser illumination, the Ag L-shell is observed to have ≳10× higher emissivity per ion per deposited laser energy than the Ar K-shell. Although such low-density Ag targets have not yet been demonstrated, simulations of targets fabricated using atomic layer deposition of Ag on silica aerogels (˜20% by atomic fraction) suggest similar performance to atomically pure metal foams and that either fabrication technique may be worth pursuing for an efficient 3-5 keV x-ray source on NIF.

On the Roles of Substrate Binding and Hinge Unfolding in Conformational Changes of Adenylate Kinase

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brokaw, Jason B.; Chu, Jhih-wei

2010-11-17

We characterized the conformational change of adenylate kinase (AK) between open and closed forms by conducting five all-atom molecular-dynamics simulations, each of 100 ns duration. Different initial structures and substrate binding configurations were used to probe the pathways of AK conformational change in explicit solvent, and no bias potential was applied. A complete closed-to-open and a partial open-to-closed transition were observed, demonstrating the direct impact of substrate-mediated interactions on shifting protein conformation. The sampled configurations suggest two possible pathways for connecting the open and closed structures of AK, affirming the prediction made based on available x-ray structures and earlier worksmore » of coarse-grained modeling. The trajectories of the all-atom molecular-dynamics simulations revealed the complexity of protein dynamics and the coupling between different domains during conformational change. Calculations of solvent density and density fluctuations surrounding AK did not show prominent variation during the transition between closed and open forms. Finally, we characterized the effects of local unfolding of an important hinge near Pro177 on the closed-to-open transition of AK and identified a novel mechanism by which hinge unfolding modulates protein conformational change. The local unfolding of Pro177 hinge induces alternative tertiary contacts that stabilize the closed structure and prevent the opening transition.« less

The stability of vacancy-like defects in amorphous silicon

NASA Astrophysics Data System (ADS)

Joly, Jean-Francois; Mousseau, Normand

2013-03-01

The contribution of vacancy-like defects to the relaxation of amorphous silicon (a-Si) has been a matter of debate for a long time. Due to their disordered nature, there is a large number local environments in which such a defect can exists. Previous numerical studies the vacancy in a-Si have been limited to small systems and very short timescales. Here we use kinectic ART (k-ART), an off-lattice kinetic Monte-Carlo simulation method with on-the-fly catalog building to study the time evolution of 1000 different single vacancy configurations in a well-relaxed a-Si model. Our results show that most of the vacancies are annihlated quickly. In fact, while 16% of the 1000 isolated vacancies survive for more than 1 ns of simulated time, 0.043% remain after 1 ms and only 6 of them survive longer than 0.1 second. Diffusion of the full vacancy is only seen in 19% of the configurations and diffusion usually leads directly to the annihilation of the defect. The actual annihilation event, in which one of the defective atoms fills the vacancy, is usually similar in all the configurations but local bonding environment heavily influence its activation barrier and relaxation energy.

Characteristics of Raman spectra for graphene oxide from ab initio simulations.

PubMed

Wang, Lu; Zhao, Jijun; Sun, Yi-Yang; Zhang, Shengbai B

2011-11-14

The Raman spectra of several locally stable structures of the graphene oxide (GO) have been simulated by ab initio calculations. Compared to graphite, the G band of GO is broadened and blueshifted due to the emergence of a series of new Raman peaks. The Raman intensities and positions of the D and G bands depend sensitively on the local atomic configurations. In addition to the normal epoxy and hydroxyl groups, other oxidation groups such as epoxy pairs are also studied. Epoxy pairs induce large blueshift of G band with respect to that of the graphite. © 2011 American Institute of Physics

Crossed Ga2O3/SnO2 multiwire architecture: a local structure study with nanometer resolution.

PubMed

Martínez-Criado, Gema; Segura-Ruiz, Jaime; Chu, Manh-Hung; Tucoulou, Remi; López, Iñaki; Nogales, Emilio; Mendez, Bianchi; Piqueras, Javier

2014-10-08

Crossed nanowire structures are the basis for high-density integration of a variety of nanodevices. Owing to the critical role of nanowires intersections in creating hybrid architectures, it has become a challenge to investigate the local structure in crossing points in metal oxide nanowires. Thus, if intentionally grown crossed nanowires are well-patterned, an ideal model to study the junction is formed. By combining electron and synchrotron beam nanoprobes, we show here experimental evidence of the role of impurities in the coupling formation, structural modifications, and atomic site configuration based on crossed Ga2O3/SnO2 nanowires. Our experiment opens new avenues for further local structure studies with both nanometer resolution and elemental sensitivity.

A Gaussian Approximation Potential for Silicon

NASA Astrophysics Data System (ADS)

Bernstein, Noam; Bartók, Albert; Kermode, James; Csányi, Gábor

We present an interatomic potential for silicon using the Gaussian Approximation Potential (GAP) approach, which uses the Gaussian process regression method to approximate the reference potential energy surface as a sum of atomic energies. Each atomic energy is approximated as a function of the local environment around the atom, which is described with the smooth overlap of atomic environments (SOAP) descriptor. The potential is fit to a database of energies, forces, and stresses calculated using density functional theory (DFT) on a wide range of configurations from zero and finite temperature simulations. These include crystalline phases, liquid, amorphous, and low coordination structures, and diamond-structure point defects, dislocations, surfaces, and cracks. We compare the results of the potential to DFT calculations, as well as to previously published models including Stillinger-Weber, Tersoff, modified embedded atom method (MEAM), and ReaxFF. We show that it is very accurate as compared to the DFT reference results for a wide range of properties, including low energy bulk phases, liquid structure, as well as point, line, and plane defects in the diamond structure.

Interacting dark resonances with plasmonic meta-molecules

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jha, Pankaj K.; Mrejen, Michael; Kim, Jeongmin

2014-09-15

Dark state physics has led to a variety of remarkable phenomena in atomic physics, quantum optics, and information theory. Here, we investigate interacting dark resonance type physics in multi-layered plasmonic meta-molecules. We theoretically demonstrate that these plasmonic meta-molecules exhibit sub-natural spectral response, analogous to conventional atomic four-level configuration, by manipulating the evanescent coupling between the bright and dark elements (plasmonic atoms). Using cascaded coupling, we show nearly 4-fold reduction in linewidth of the hybridized resonance compared to a resonantly excited single bright plasmonic atom with same absorbance. In addition, we engineered the geometry of the meta-molecules to realize efficient intramolecularmore » excitation transfer with nearly 80%, on resonant excitation, of the total absorption being localized at the second dark plasmonic atom. An analytical description of the spectral response of the structure is presented with full electrodynamics simulations to corroborate our results. Such multilayered meta-molecules can bring a new dimension to higher quality factor plasmonic resonance, efficient excitation transfer, wavelength demultiplexing, and enhanced non-linearity at nanoscale.« less

Localized overlap algorithm for unexpanded dispersion energies

NASA Astrophysics Data System (ADS)

Rob, Fazle; Misquitta, Alston J.; Podeszwa, Rafał; Szalewicz, Krzysztof

2014-03-01

First-principles-based, linearly scaling algorithm has been developed for calculations of dispersion energies from frequency-dependent density susceptibility (FDDS) functions with account of charge-overlap effects. The transition densities in FDDSs are fitted by a set of auxiliary atom-centered functions. The terms in the dispersion energy expression involving products of such functions are computed using either the unexpanded (exact) formula or from inexpensive asymptotic expansions, depending on the location of these functions relative to the dimer configuration. This approach leads to significant savings of computational resources. In particular, for a dimer consisting of two elongated monomers with 81 atoms each in a head-to-head configuration, the most favorable case for our algorithm, a 43-fold speedup has been achieved while the approximate dispersion energy differs by less than 1% from that computed using the standard unexpanded approach. In contrast, the dispersion energy computed from the distributed asymptotic expansion differs by dozens of percent in the van der Waals minimum region. A further increase of the size of each monomer would result in only small increased costs since all the additional terms would be computed from the asymptotic expansion.

Achieving DFT accuracy with a machine-learning interatomic potential: Thermomechanics and defects in bcc ferromagnetic iron

NASA Astrophysics Data System (ADS)

Dragoni, Daniele; Daff, Thomas D.; Csányi, Gábor; Marzari, Nicola

2018-01-01

We show that the Gaussian Approximation Potential (GAP) machine-learning framework can describe complex magnetic potential energy surfaces, taking ferromagnetic iron as a paradigmatic challenging case. The training database includes total energies, forces, and stresses obtained from density-functional theory in the generalized-gradient approximation, and comprises approximately 150,000 local atomic environments, ranging from pristine and defected bulk configurations to surfaces and generalized stacking faults with different crystallographic orientations. We find the structural, vibrational, and thermodynamic properties of the GAP model to be in excellent agreement with those obtained directly from first-principles electronic-structure calculations. There is good transferability to quantities, such as Peierls energy barriers, which are determined to a large extent by atomic configurations that were not part of the training set. We observe the benefit and the need of using highly converged electronic-structure calculations to sample a target potential energy surface. The end result is a systematically improvable potential that can achieve the same accuracy of density-functional theory calculations, but at a fraction of the computational cost.

Radiation-Spray Coupling for Realistic Flow Configurations

NASA Technical Reports Server (NTRS)

El-Asrag, Hossam; Iannetti, Anthony C.

2011-01-01

Three Large Eddy Simulations (LES) for a lean-direct injection (LDI) combustor are performed and compared. In addition to the cold flow simulation, the effect of radiation coupling with the multi-physics reactive flow is analyzed. The flame let progress variable approach is used as a subgrid combustion model combined with a stochastic subgrid model for spray atomization and an optically thin radiation model. For accurate chemistry modeling, a detailed Jet-A surrogate mechanism is utilized. To achieve realistic inflow, a simple recycling technique is performed at the inflow section upstream of the swirler. Good comparison is shown with the experimental data mean and root mean square profiles. The effect of combustion is found to change the shape and size of the central recirculation zone. Radiation is found to change the spray dynamics and atomization by changing the heat release distribution and the local temperature values impacting the evaporation process. The simulation with radiation modeling shows wider range of droplet size distribution by altering the evaporation rate. The current study proves the importance of radiation modeling for accurate prediction in realistic spray combustion configurations, even for low pressure systems.

Energy levels, wavelengths, and transition rates of multipole transitions (E1, E2, M1, M2) in Au{sup 67+} and Au{sup 66+} ions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hamasha, Safeia, E-mail: safeia@hu.edu.jo

2013-11-15

The fully relativistic configuration interaction method of the FAC code is used to calculate atomic data for multipole transitions in Mg-like Au (Au{sup 67+}) and Al-like Au (Au{sup 66+}) ions. Generated atomic data are important in the modeling of M-shell spectra for heavy Au ions and Au plasma diagnostics. Energy levels, oscillator strengths and transition rates are calculated for electric-dipole (E1), electric quadrupole (E2), magnetic dipole (M1), and magnetic quadrupole (M2) for transitions between excited and ground states 3l−nl{sup ′}, such that n=4,5,6,7. The local central potential is derived using the Dirac–Fock–Slater method. Correlation effects to all orders are consideredmore » by the configuration interaction expansion. All relativistic effects are included in the calculations. Calculated energy levels are compared against published values that were calculated using the multi-reference many body perturbation theory, which includes higher order QED effects. Favorable agreement was observed, with less than 0.15% difference.« less

W and X Photoluminescence Centers in Crystalline Si: Chasing Candidates at Atomic Level Through Multiscale Simulations

NASA Astrophysics Data System (ADS)

Aboy, María; Santos, Iván; López, Pedro; Marqués, Luis A.; Pelaz, Lourdes

2018-04-01

Several atomistic techniques have been combined to identify the structure of defects responsible for X and W photoluminescence lines in crystalline Si. We used kinetic Monte Carlo simulations to reproduce irradiation and annealing conditions used in photoluminescence experiments. We found that W and X radiative centers are related to small Si self-interstitial clusters but coexist with larger Si self-interstitials clusters that can act as nonradiative centers. We used molecular dynamics simulations to explore the many different configurations of small Si self-interstitial clusters, and selected those having symmetry compatible with W and X photoluminescence centers. Using ab initio simulations, we calculated their formation energy, donor levels, and energy of local vibrational modes. On the basis of photoluminescence experiments and our multiscale theoretical calculations, we discuss the possible atomic configurations responsible for W and X photoluminescence centers in Si. Our simulations also reveal that the intensity of photoluminescence lines is the result of competition between radiative centers and nonradiative competitors, which can explain the experimental quenching of W and X lines even in the presence of the photoluminescence centers.

Relativistic Thomas-Fermi treatment of compressed atoms and compressed nuclear matter cores of stellar dimensions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rotondo, M.; Rueda, Jorge A.; Xue, S.-S.

The Feynman-Metropolis-Teller treatment of compressed atoms is extended to the relativistic regimes. Each atomic configuration is confined by a Wigner-Seitz cell and is characterized by a positive electron Fermi energy. The nonrelativistic treatment assumes a pointlike nucleus and infinite values of the electron Fermi energy can be attained. In the relativistic treatment there exists a limiting configuration, reached when the Wigner-Seitz cell radius equals the radius of the nucleus, with a maximum value of the electron Fermi energy (E{sub e}{sup F}){sub max}, here expressed analytically in the ultrarelativistic approximation. The corrections given by the relativistic Thomas-Fermi-Dirac exchange term are alsomore » evaluated and shown to be generally small and negligible in the relativistic high-density regime. The dependence of the relativistic electron Fermi energies by compression for selected nuclei are compared and contrasted to the nonrelativistic ones and to the ones obtained in the uniform approximation. The relativistic Feynman-Metropolis-Teller approach here presented overcomes some difficulties in the Salpeter approximation generally adopted for compressed matter in physics and astrophysics. The treatment is then extrapolated to compressed nuclear matter cores of stellar dimensions with A{approx_equal}(m{sub Planck}/m{sub n}){sup 3}{approx}10{sup 57} or M{sub core}{approx}M{sub {circle_dot}}. A new family of equilibrium configurations exists for selected values of the electron Fermi energy varying in the range 0

Photoionization of Atoms and Molecules using a Configuration-Average Distorted-Wave Method

NASA Astrophysics Data System (ADS)

Pindzola, M. S.; Balance, C. P.; Loch, S. D.; Ludlow, J. A.

2011-05-01

A configuration-average distorted-wave method is applied to calculate the photoionization cross section for the outer subshells of the C atom and the C2 diatomic molecule. Comparisions are made with previous R-matrix and Hartree- Fock distorted-wave calculations.

Geometric Electron Models.

ERIC Educational Resources Information Center

Nika, G. Gerald; Parameswaran, R.

1997-01-01

Describes a visual approach for explaining the filling of electrons in the shells, subshells, and orbitals of the chemical elements. Enables students to apply the principles of atomic electron configuration while using manipulatives to model the building up of electron configurations as the atomic numbers of elements increase on the periodic…

Quantum transport modelling of silicon nanobeams using heterogeneous computing scheme

DOE Office of Scientific and Technical Information (OSTI.GOV)

Harb, M., E-mail: harbm@physics.mcgill.ca; Michaud-Rioux, V., E-mail: vincentm@physics.mcgill.ca; Guo, H., E-mail: guo@physics.mcgill.ca

We report the development of a powerful method for quantum transport calculations of nanowire/nanobeam structures with large cross sectional area. Our approach to quantum transport is based on Green's functions and tight-binding potentials. A linear algebraic formulation allows us to harness the massively parallel nature of Graphics Processing Units (GPUs) and our implementation is based on a heterogeneous parallel computing scheme with traditional processors and GPUs working together. Using our software tool, the electronic and quantum transport properties of silicon nanobeams with a realistic cross sectional area of ∼22.7 nm{sup 2} and a length of ∼81.5 nm—comprising 105 000 Si atoms and 24 000more » passivating H atoms in the scattering region—are investigated. The method also allows us to perform significant averaging over impurity configurations—all possible configurations were considered in the case of single impurities. Finally, the effect of the position and number of vacancy defects on the transport properties was considered. It is found that the configurations with the vacancies lying closer to the local density of states (LDOS) maxima have lower transmission functions than the configurations with the vacancies located at LDOS minima or far away from LDOS maxima, suggesting both a qualitative method to tune or estimate optimal impurity configurations as well as a physical picture that accounts for device variability. Finally, we provide performance benchmarks for structures as large as ∼42.5 nm{sup 2} cross section and ∼81.5 nm length.« less

In-situ crystallization of GeTe\\GaSb phase change memory stacked films

DOE Office of Scientific and Technical Information (OSTI.GOV)

Velea, A., E-mail: alin.velea@psi.ch; National Institute of Materials Physics, RO-077125 Magurele, Ilfov; Borca, C. N.

2014-12-21

Single and double layer phase change memory structures based on GeTe and GaSb thin films were deposited by pulsed laser deposition (PLD). Their crystallization behavior was studied using in-situ synchrotron techniques. Electrical resistance vs. temperature investigations, using the four points probe method, showed transition temperatures of 138 °C and 198 °C for GeTe and GaSb single films, respectively. It was found that after GeTe crystallization in the stacked films, Ga atoms from the GaSb layer diffused in the vacancies of the GeTe crystalline structure. Therefore, the crystallization temperature of the Sb-rich GaSb layer is decreased by more than 30 °C. Furthermore, at 210 °C,more » the antimony excess from GaSb films crystallizes as a secondary phase. At higher annealing temperatures, the crystalline Sb phase increased on the expense of GaSb crystalline phase which was reduced. Extended X-ray absorption fine structure (EXAFS) measurements at the Ga and Ge K-edges revealed changes in their local atomic environments as a function of the annealing temperature. Simulations unveil a tetrahedral configuration in the amorphous state and octahedral configuration in the crystalline state for Ge atoms, while Ga is four-fold coordinated in both as-deposited and annealed samples.« less

Local Environment Sensitivity of the Cu K-Edge XANES Features in Cu-SSZ-13: Analysis from First-Principles.

PubMed

Zhang, Renqin; McEwen, Jean-Sabin

2018-05-22

Cu K-edge X-ray absorption near-edge spectra (XANES) have been widely used to study the properties of Cu-SSZ-13. In this Letter, the sensitivity of the XANES features to the local environment for a Cu + cation with a linear configuration and a Cu 2+ cation with a square-linear configuration in Cu-SSZ-13 is reported. When a Cu + cation is bonded to H 2 O or NH 3 in a linear configuration, the XANES has a strong peak at around 8983 eV. The intensity of this peak decreases as the linear configuration is broken. As for the Cu 2+ cations in a square-planar configuration with a coordination number of 4, two peaks at around 8986 and 8993 eV are found. An intensity decrease for both peaks at around 8986 and 8993 eV is found in an NH 3 _4_Z 2 Cu model as the N-Cu-N angle changes from 180 to 100°. We correlate these features to the variation of the 4p state by PDOS analysis. In addition, the feature peaks for both the Cu + cation and Cu 2+ cation do not show a dependence on the Cu-N bond length. We further show that the feature peaks also change when the coordination number of the Cu cation is varied, while these feature peaks are independent of the zeolite topology. These findings help elucidate the experimental XANES features at an atomic and an electronic level.

Atomic force microscope with combined FTIR-Raman spectroscopy having a micro thermal analyzer

DOEpatents

Fink, Samuel D [Aiken, SC; Fondeur, Fernando F [North Augusta, SC

2011-10-18

An atomic force microscope is provided that includes a micro thermal analyzer with a tip. The micro thermal analyzer is configured for obtaining topographical data from a sample. A raman spectrometer is included and is configured for use in obtaining chemical data from the sample.

The role of configuration interaction in the LTE opacity of Fe

NASA Astrophysics Data System (ADS)

Colgan, James; Kilcrease, David; Magee, Norm; Armstrong, Gregory; Abdallah, Joe; Sherrill, Manolo; Fontes, Christopher; Zhang, Honglin; Hakel, Peter

2013-05-01

The Los Alamos National Laboratory code ATOMIC has been recently used to generate a series of local-thermodynamic-equilibrium (LTE) light element opacities for the elements H through Ne. Our calculations, which include fine-structure detail, represent a systematic improvement over previous Los Alamos opacity calculations using the LEDCOP legacy code. Recent efforts have resulted in comprehensive new calculations of the opacity of Fe. In this presentation we explore the role of configuration interaction (CI) in the Fe opacity, and show where CI influences the monochromatic opacity. We present such comparisons for conditions of astrophysical interest. The Los Alamos National Laboratory is operated by Los Alamos National Security, LLC for the National Nuclear Security Administration of the U.S. Department of Energy under Contract No. DE-AC5206NA25396.

First-principles theoretical investigation of monoatomic and dimer Mn adsorption on noble metal (111) surfaces

NASA Astrophysics Data System (ADS)

Muñoz, Francisco; Romero, Aldo H.; Mejía-López, Jose; Morán-López, J. L.

2012-03-01

A theoretical investigation of the adsorption of Mn single atoms and dimers on the (111) surface of Cu, Ag, and Au, within the framework of the density functional theory, is presented. First, the bulk and the clean (111) surface electronic structures are calculated, with results that agree well with previous reports. To understand the adatom-substrate interaction, also the electronic characteristics of the free Mn dimer are determined. Then, the electronic structure of the Mn adatom, chemisorbed on four different surface geometries, is analyzed for the three noble metals. It is found that the most stable geometry, in all three cases, Cu, Ag, and Au, occurs when the Mn atom is chemisorbed on threefold coordinated sites. For the dimer, the lowest-energy configuration corresponds to the molecule lying parallel to the surface. In the three noble metals, the geometry corresponds to both atoms chemisorbed in threefold coordinated sites, but with different local symmetry. It is also found that the magnetic configuration with the lowest energy corresponds to the antiferromagnetic arrangement of Mn atoms, with individual magnetic moments close to 5μB. The ferromagnetic and antiferromagnetic solutions, in the case of a Ag substrate, are close in energy. It is also found that in this case the Mn2 molecule is chemisorbed with very similar energy on various geometries. To study the dynamical motion of the dimer components, we calculated the potential energy barriers for the Mn motion in the various surfaces. In contrast to Cu and Au, this leads to the conclusion that on Ag the Mn dimer moves relatively freely.

Binding effects of Mn²⁺ and Zn²⁺ ions on the vibrational properties of guanine-cytosine base pairs in the Watson-Crick and Hoogsteen configurations.

PubMed

Morari, Cristian; Bogdan, Diana; Muntean, Cristina M

2012-11-01

The binding effects of Mn²⁺ and Zn²⁺ ions on the vibrational properties of guanine-cytosine base pairs have been performed using density functional theory investigations. The calculations were carried out on Watson-Crick and Hoogsteen configurations of the base pairs. We have found, that in Watson-Crick configuration, the metal is coordinated to N7 atom of guanine while, in the case of Hoogsteen configuration, the coordination is at N3 atom of guanine. We have pointed out the vibrational bands that can be used to detect the presence of metallic ions in the Watson-Crick and Hoogsteen structures. Our results show that the vibrational amplitudes of metallic atoms are strong for wavenumbers lower than 600 cm⁻¹. Also, we predict that the distinction between Watson-Crick and Hoogsteen configurations can be seen around 85, 170 and 310 cm⁻¹.

Magnetism in Pd: Magnetoconductance and transport spectroscopy of atomic contacts

NASA Astrophysics Data System (ADS)

Strigl, F.; Keller, M.; Weber, D.; Pietsch, T.; Scheer, E.

2016-10-01

Since the rapid technological progress demands for ever smaller storage units, the emergence of stable magnetic order in nanomaterials down to the single-atom regime has attracted huge scientific attention to date. Electronic transport spectroscopy has been proven to be a versatile tool for the investigation of electronic, magnetic, and mechanical properties of atomic contacts. Here we report a comprehensive experimental study of the magnetoconductance and electronic properties of Pd atomic contacts at low temperature. The analysis of electronic transport (d I /d V ) spectra and the magnetoconductance curves yields a diverse behavior of Pd single-atom contacts, which is attributed to different contact configurations. The magnetoconductance shows a nonmonotonous but mostly continuous behavior, comparable to those found in atomic contacts of band ferromagnets. In the d I /d V spectra, frequently, a pronounced zero-bias anomaly (ZBA) as well as an aperiodic and nonsymmetric fluctuation pattern are observed. While the ZBA can be interpreted as a sign of the Kondo effect, suggesting the presence of magnetic impurity, the fluctuations are evaluated in the framework of conductance fluctuations in relation to the magnetoconductance traces and to previous findings in Au atomic contacts. This thorough analysis reveals that the magnetoconductance and transport spectrum of Au atomic contacts can completely be accounted for by conductance fluctuations, while in Pd contacts the presence of local magnetic order is required.

Study of the Structural Stability in Intermetallics Using Displacive Transformation Paths

NASA Astrophysics Data System (ADS)

Sob, M.; Wang, L. G.; Vitek, V.

1997-03-01

Relative structural stability of TiAl, FeAl, NiAl and NiTi is studied by investigating displacive phase transformation paths. These include the well known tetragonal (Bain's) and trigonal deformation paths which correspond to large homogeneous straining, and also more complex paths that include the shuffling of atomic planes. The results of full-potential APW total energy calculations show that all higher-energy cubic structures studied are locally unstable with respect to some deformation modes. There may or may not be symmetry-dictated energy extrema corresponding to cubic lattices depending on the atomic ordering. However, other energy extrema that are not imposed by symmetry requirements occur along the transformation paths. Configurations corresponding to energy minima may represent metastable structures that can play an important role in interfaces and other extended defects.

Advancing differential atom interferometry for space applications

NASA Astrophysics Data System (ADS)

Chiow, Sheng-Wey; Williams, Jason; Yu, Nan

2016-05-01

Atom interferometer (AI) based sensors exhibit precision and accuracy unattainable with classical sensors, thanks to the inherent stability of atomic properties. Dual atomic sensors operating in a differential mode further extend AI applicability beyond environmental disturbances. Extraction of the phase difference between dual AIs, however, typically introduces uncertainty and systematic in excess of that warranted by each AI's intrinsic noise characteristics, especially in practical applications and real time measurements. In this presentation, we report our efforts in developing practical schemes for reducing noises and enhancing sensitivities in the differential AI measurement implementations. We will describe an active phase extraction method that eliminates the noise overhead and demonstrates a performance boost of a gravity gradiometer by a factor of 3. We will also describe a new long-baseline approach for differential AI measurements in a laser ranging assisted AI configuration. The approach uses well-developed AIs for local measurements but leverage the mature schemes of space laser interferometry for LISA and GRACE. This research was carried out at the Jet Propulsion Laboratory, California Institute of Technology, under a Contract with NASA.

Atomic Data and Spectral Line Intensities for Be-like Ions

NASA Technical Reports Server (NTRS)

Bhatia, Anand; Landi, E.

2008-01-01

Atomic data and collision rates are needed to model the spectrum of optically thin astrophysical sources. Recent observations from solar instrumentation such as SOH0 and Hinode have revealed the presence of hosts of lines emitted by high-energy configurations from ions belonging to the Be-like to the 0-like isoelectronic sequences. Data for such configurations are often unavailable in the literature. We have started a program to calculate the atomic parameters and rates for the high-energy configurations of Be-like ions of the type ls2.21.nl' where n=3,4,5. We report on the results of this project and on the diagnostic application of the predicted spectral lines.

Investigation of soot and carbon formation in small gas turbine combustors

NASA Technical Reports Server (NTRS)

Rosfjord, T. J.

1982-01-01

An investigation of hardware configurations which attempt to minimize carbon and soot-production without sacrificing performance in small gas turbine combustors was conducted. Four fuel injectors, employing either airblast atomization, pressure atomization, or fuel vaporization techniques were combined with nozzle air swirlers and injector sheaths. Eight configurations were screened at sea-level takeoff and idle test conditions. Selected configurations were focused upon in an attempt to quantify the influence of combustor pressure, inlet temperature, primary zone operation, and combustor loading on soot and carbon formation. Cycle tests were also performed. It was found that smoke emission levels depended on the combustor fluid mechanics, the atomization quality of the injector and the fuel hydrogen content.

Constructing simple yet accurate potentials for describing the solvation of HCl/water clusters in bulk helium and nanodroplets.

PubMed

Boese, A Daniel; Forbert, Harald; Masia, Marco; Tekin, Adem; Marx, Dominik; Jansen, Georg

2011-08-28

The infrared spectroscopy of molecules, complexes, and molecular aggregates dissolved in superfluid helium clusters, commonly called HElium NanoDroplet Isolation (HENDI) spectroscopy, is an established, powerful experimental technique for extracting high resolution ro-vibrational spectra at ultra-low temperatures. Realistic quantum simulations of such systems, in particular in cases where the solute is undergoing a chemical reaction, require accurate solute-helium potentials which are also simple enough to be efficiently evaluated over the vast number of steps required in typical Monte Carlo or molecular dynamics sampling. This precludes using global potential energy surfaces as often parameterized for small complexes in the realm of high-resolution spectroscopic investigations that, in view of the computational effort imposed, are focused on the intermolecular interaction of rigid molecules with helium. Simple Lennard-Jones-like pair potentials, on the other hand, fall short in providing the required flexibility and accuracy in order to account for chemical reactions of the solute molecule. Here, a general scheme of constructing sufficiently accurate site-site potentials for use in typical quantum simulations is presented. This scheme employs atom-based grids, accounts for local and global minima, and is applied to the special case of a HCl(H(2)O)(4) cluster solvated by helium. As a first step, accurate interaction energies of a helium atom with a set of representative configurations sampled from a trajectory following the dissociation of the HCl(H(2)O)(4) cluster were computed using an efficient combination of density functional theory and symmetry-adapted perturbation theory, i.e. the DFT-SAPT approach. For each of the sampled cluster configurations, a helium atom was placed at several hundred positions distributed in space, leading to an overall number of about 400,000 such quantum chemical calculations. The resulting total interaction energies, decomposed into several energetic contributions, served to fit a site-site potential, where the sites are located at the atomic positions and, additionally, pseudo-sites are distributed along the lines joining pairs of atom sites within the molecular cluster. This approach ensures that this solute-helium potential is able to describe both undissociated molecular and dissociated (zwitter-) ionic configurations, as well as the interconnecting reaction pathway without re-adjusting partial charges or other parameters depending on the particular configuration. Test calculations of the larger HCl(H(2)O)(5) cluster interacting with helium demonstrate the transferability of the derived site-site potential. This specific potential can be readily used in quantum simulations of such HCl/water clusters in bulk helium or helium nanodroplets, whereas the underlying construction procedure can be generalized to other molecular solutes in other atomic solvents such as those encountered in rare gas matrix isolation spectroscopy.

Ab initio calculations of ionic hydrocarbon compounds with heptacoordinate carbon.

PubMed

Wang, George; Rahman, A K Fazlur; Wang, Bin

2018-04-25

Ionic hydrocarbon compounds that contain hypercarbon atoms, which bond to five or more atoms, are important intermediates in chemical synthesis and may also find applications in hydrogen storage. Extensive investigations have identified hydrocarbon compounds that contain a five- or six-coordinated hypercarbon atom, such as the pentagonal-pyramidal hexamethylbenzene, C 6 (CH 3 ) 6 2+ , in which a hexacoordinate carbon atom is involved. It remains challenging to search for further higher-coordinated carbon in ionic hydrocarbon compounds, such as seven- and eight-coordinated carbon. Here, we report ab initio density functional calculations that show a stable 3D hexagonal-pyramidal configuration of tropylium trication, (C 7 H 7 ) 3+ , in which a heptacoordinate carbon atom is involved. We show that this tropylium trication is stable against deprotonation, dissociation, and structural deformation. In contrast, the pyramidal configurations of ionic C 8 H 8 compounds, which would contain an octacoordinate carbon atom, are unstable. These results provide insights for developing new molecular structures containing hypercarbon atoms, which may have potential applications in chemical synthesis and in hydrogen storage. Graphical abstract Possible structural transformations of stable configurations of (C 7 H 7 ) 3+ , which may result in the formation of the pyramidal structure that involves a heptacoordinate hypercarbon atom.

Conformational Analysis on structural perturbations of the zinc finger NEMO

NASA Astrophysics Data System (ADS)

Godwin, Ryan; Salsbury, Freddie; Salsbury Group Team

2014-03-01

The NEMO (NF-kB Essential Modulator) Zinc Finger protein (2jvx) is a functional Ubiquitin-binding domain, and plays a role in signaling pathways for immune/inflammatory responses, apoptosis, and oncogenesis [Cordier et al., 2008]. Characterized by 3 cysteines and 1 histidine residue at the active site, the biologically occurring, bound zinc configuration is a stable structural motif. Perturbations of the zinc binding residues suggest conformational changes in the 423-atom protein characterized via analysis of all-atom molecular dynamics simulations. Structural perturbations include simulations with and without a zinc ion and with and without de-protonated cysteines, resulting in four distinct configurations. Simulations of various time scales show consistent results, yet the longest, GPU driven, microsecond runs show more drastic structural and dynamic fluctuations when compared to shorter duration time-scales. The last cysteine residue (26 of 28) and the helix on which it resides exhibit a secondary, locally unfolded conformation in addition to its normal bound conformation. Combined analytics elucidate how the presence of zinc and/or protonated cysteines impact the dynamics and energetic fluctuations of NEMO. Comprehensive Cancer Center of Wake Forest University Computational Biosciences shared resource supported by NCI CCSG P30CA012197.

Invited Article: Autonomous assembly of atomically perfect nanostructures using a scanning tunneling microscope.

PubMed

Celotta, Robert J; Balakirsky, Stephen B; Fein, Aaron P; Hess, Frank M; Rutter, Gregory M; Stroscio, Joseph A

2014-12-01

A major goal of nanotechnology is to develop the capability to arrange matter at will by placing individual atoms at desired locations in a predetermined configuration to build a nanostructure with specific properties or function. The scanning tunneling microscope has demonstrated the ability to arrange the basic building blocks of matter, single atoms, in two-dimensional configurations. An array of various nanostructures has been assembled, which display the quantum mechanics of quantum confined geometries. The level of human interaction needed to physically locate the atom and bring it to the desired location limits this atom assembly technology. Here we report the use of autonomous atom assembly via path planning technology; this allows atomically perfect nanostructures to be assembled without the need for human intervention, resulting in precise constructions in shorter times. We demonstrate autonomous assembly by assembling various quantum confinement geometries using atoms and molecules and describe the benefits of this approach.

Fine- and hyperfine structure investigations of the even-parity configuration system of the atomic holmium

NASA Astrophysics Data System (ADS)

Stefanska, D.; Ruczkowski, J.; Elantkowska, M.; Furmann, B.

2018-04-01

In this work new experimental results concerning the hyperfine structure (hfs) for the even-parity level system of the holmium atom (Ho I) were obtained; additionally, hfs data obtained recently as a by-product in investigations of the odd-parity level system were summarized. In the present work the values of the magnetic dipole and the electric quadrupole hfs constants A and B were determined for 24 even-parity levels, for 14 of them for the first time. On the basis of these results, as well as on available literature data, a parametric study of the fine structure and the hyperfine structure for the even-parity configurations of atomic holmium was performed. A multi-configuration fit of 7 configurations was carried out, taking into account second-order of the perturbation theory. For unknown electronic levels predicted values of the level energies and hfs constants are given, which can facilitate further experimental investigations.

A triple point in 3-level systems

NASA Astrophysics Data System (ADS)

Nahmad-Achar, E.; Cordero, S.; López-Peña, R.; Castaños, O.

2014-11-01

The energy spectrum of a 3-level atomic system in the Ξ-configuration is studied. This configuration presents a triple point independently of the number of atoms, which remains in the thermodynamic limit. This means that in a vicinity of this point any quantum fluctuation will drastically change the composition of the ground state of the system. We study the expectation values of the atomic population of each level, the number of photons, and the probability distribution of photons at the triple point.

An accurate full-dimensional potential energy surface for H-Au(111): Importance of nonadiabatic electronic excitation in energy transfer and adsorption.

PubMed

Janke, Svenja M; Auerbach, Daniel J; Wodtke, Alec M; Kandratsenka, Alexander

2015-09-28

We have constructed a potential energy surface (PES) for H-atoms interacting with fcc Au(111) based on fitting the analytic form of the energy from Effective Medium Theory (EMT) to ab initio energy values calculated with density functional theory. The fit used input from configurations of the H-Au system with Au atoms at their lattice positions as well as configurations with the Au atoms displaced from their lattice positions. It reproduces the energy, in full dimension, not only for the configurations used as input but also for a large number of additional configurations derived from ab initio molecular dynamics (AIMD) trajectories at finite temperature. Adiabatic molecular dynamics simulations on this PES reproduce the energy loss behavior of AIMD. EMT also provides expressions for the embedding electron density, which enabled us to develop a self-consistent approach to simulate nonadiabatic electron-hole pair excitation and their effect on the motion of the incident H-atoms. For H atoms with an energy of 2.7 eV colliding with Au, electron-hole pair excitation is by far the most important energy loss pathway, giving an average energy loss ≈3 times that of the adiabatic case. This increased energy loss enhances the probability of the H-atom remaining on or in the Au slab by a factor of 2. The most likely outcome for H-atoms that are not scattered also depends prodigiously on the energy transfer mechanism; for the nonadiabatic case, more than 50% of the H-atoms which do not scatter are adsorbed on the surface, while for the adiabatic case more than 50% pass entirely through the 4 layer simulation slab.

Anomalous vibrational modes in acetanilide: a F.D.S. incoherent inelastic neutron scattering study

NASA Astrophysics Data System (ADS)

Barthes, Mariette; Eckert, Juergen; Johnson, Susanna W.; Moret, Jacques; Swanson, Basil I.; Unkefer, Clifford J.

The origin of the anomalous infra-red and Raman modes in acetanilide (C6H5NHCOCH3, or ACN)(1) , remains a subject of considerable controversy. One family of theoretical models involves Davydov-like solitons (2) nonlinear vibrational coupling (3), or "polaronic" localized modes (4)(5). An alternative interpretation of the extra-bands in terms of a Fermi resonance was proposed (6) and recently the existence of slightly non-degenerate hydrogen atom configurations (7) in the H-bond was suggested as an explanation for the anomalies.

Oxidative damage to DNA: counterion-assisted addition of water to ionized DNA.

PubMed

Barnett, Robert N; Bongiorno, Angelo; Cleveland, Charles L; Joy, Abraham; Landman, Uzi; Schuster, Gary B

2006-08-23

Oxidative damage to DNA, implicated in mutagenesis, aging, and cancer, follows electron loss that generates a radical cation that migrates to a guanine, where it may react with water to form 8-oxo-7,8-dihydroguanine (8-OxoG). Molecular dynamics and ab initio quantum simulations on a B-DNA tetradecamer reveal activated reaction pathways that depend on the local counterion arrangement. The lowest activation barrier, 0.73 eV, is found for a reaction that starts from a configuration where a Na(+) resides in the major groove near the N7 atoms of adjacent guanines, and evolves through a transition state where a bond between a water oxygen atom and a carbon atom forms concurrently with displacement of a proton toward a neighboring water molecule. Subsequently, a bonded complex of a hydronium ion and the nearest backbone phosphate group forms. This counterion-assisted proton shuttle mechanism is supported by experiments exploiting selective substitution of backbone phosphates by methylphosphonates.

Atomic and electronic properties of quasi-one-dimensional MOS2 nanowires

PubMed Central

Seivane, Lucas Fernandez; Barron, Hector; Botti, Silvana; Marques, Miguel Alexandre Lopes; Rubio, Ángel; López-Lozano, Xóchitl

2013-01-01

The structural, electronic and magnetic properties of quasi-one-dimensional MoS2 nanowires, passivated by extra sulfur, have been determined using ab initio density-functional theory. The nanostructures were simulated using several different models based on experimental electron microscopy images. It is found that independently of the geometrical details and the coverage of extra sulfur at the Mo-edge, quasi-one-dimensional metallic states are predominant in all the low-energy model structures despite their reduced dimensionality. These metallic states are localized mainly at the edges. However, the electronic and magnetic character of the NWs does not depend only on the S saturation but also on the symmetry configuration of the S edge atoms. Our results show that for the same S saturation the magnetization can be decreased by increasing the pairing of the S and Mo edge atoms. In spite of the observed pairing of S dimers at the Mo-edge, the nanowires do not experience a Peierls-like metal-insulator transition PMID:25429189

Simulation study of 3–5 keV x-ray conversion efficiency from Ar K-shell vs. Ag L-shell targets on the National Ignition Facility laser

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kemp, G. E., E-mail: kemp10@llnl.gov; Colvin, J. D.; Fournier, K. B.

2015-05-15

Tailored, high-flux, multi-keV x-ray sources are desirable for studying x-ray interactions with matter for various civilian, space and military applications. For this study, we focus on designing an efficient laser-driven non-local thermodynamic equilibrium 3–5 keV x-ray source from photon-energy-matched Ar K-shell and Ag L-shell targets at sub-critical densities (∼n{sub c}/10) to ensure supersonic, volumetric laser heating with minimal losses to kinetic energy, thermal x rays and laser-plasma instabilities. Using HYDRA, a multi-dimensional, arbitrary Lagrangian-Eulerian, radiation-hydrodynamics code, we performed a parameter study by varying initial target density and laser parameters for each material using conditions readily achievable on the National Ignition Facilitymore » (NIF) laser. We employ a model, benchmarked against Kr data collected on the NIF, that uses flux-limited Lee-More thermal conductivity and multi-group implicit Monte-Carlo photonics with non-local thermodynamic equilibrium, detailed super-configuration accounting opacities from CRETIN, an atomic-kinetics code. While the highest power laser configurations produced the largest x-ray yields, we report that the peak simulated laser to 3–5 keV x-ray conversion efficiencies of 17.7% and 36.4% for Ar and Ag, respectively, occurred at lower powers between ∼100–150 TW. For identical initial target densities and laser illumination, the Ag L-shell is observed to have ≳10× higher emissivity per ion per deposited laser energy than the Ar K-shell. Although such low-density Ag targets have not yet been demonstrated, simulations of targets fabricated using atomic layer deposition of Ag on silica aerogels (∼20% by atomic fraction) suggest similar performance to atomically pure metal foams and that either fabrication technique may be worth pursuing for an efficient 3–5 keV x-ray source on NIF.« less

Imaging domain walls between nematic quantum Hall phases on the surface of bismuth

NASA Astrophysics Data System (ADS)

Ding, Hao; Randeria, Mallika T.; Feldman, Benjamin E.; Ji, Huiwen; Cava, Robert J.; Yazdani, Ali

The sensitivity of nematic electronic phases to disorder results in short range ordering and the formation of domains. Local probes are required to investigate the character of these domains and the boundaries between them, which remain hidden in global measurements that average over microscopic configurations. In this talk, I will describe measurements performed with a scanning tunneling microscope to study local nematic order on the surface of bismuth at high magnetic field. By imaging individual anisotropic cyclotron orbit wavefunctions that are pinned to atomic-scale surface defects, we directly resolve local nematic behavior and study the evolution of nematic states across a domain wall. Through spectroscopic mapping, we explore how the broken-symmetry Landau levels disperse across the domain wall, the influence of exchange interactions at such a boundary, and the formation of one-dimensional edge states.

Sensitivity optimization of Bell-Bloom magnetometers by manipulation of atomic spin synchronization

NASA Astrophysics Data System (ADS)

Ranjbaran, M.; Tehranchi, M. M.; Hamidi, S. M.; Khalkhali, S. M. H.

2018-05-01

Many efforts have been devoted to the developments of atomic magnetometers for achieving the high sensitivity required in biomagnetic applications. To reach the high sensitivity, many types of atomic magnetometers have been introduced for optimization of the creation and relaxation rates of atomic spin polarization. In this paper, regards to sensitivity optimization techniques in the Mx configuration, we have proposed a novelty approach for synchronization of the spin precession in the Bell-Bloom magnetometers. We have utilized the phenomenological Bloch equations to simulate the spin dynamics when modulation of pumping light and radio frequency magnetic field were both used for atomic spin synchronization. Our results showed that the synchronization process, improved the magnetometer sensitivity respect to the classical configurations.

Mechanical properties of Fe rich Fe-Si alloys: ab initio local bulk-modulus viewpoint

NASA Astrophysics Data System (ADS)

Bhattacharya, Somesh Kr; Kohyama, Masanori; Tanaka, Shingo; Shiihara, Yoshinori; Saengdeejing, Arkapol; Chen, Ying; Mohri, Tetsuo

2017-11-01

Fe-rich Fe-Si alloys show peculiar bulk-modulus changes depending on the Si concentration in the range of 0-15 at.%Si. In order to clarify the origin of this phenomenon, we have performed density-functional theory calculations of supercells of Fe-Si alloy models with various Si concentrations. We have applied our recent techniques of ab initio local energy and local stress, by which we can obtain a local bulk modulus of each atom or atomic group as a local constituent of the cell-averaged bulk modulus. A2-phase alloy models are constructed by introducing Si substitution into bcc Fe as uniformly as possible so as to prevent mutual neighboring, while higher Si concentrations over 6.25 at.%Si lead to contacts between SiFe8 cubic clusters via sharing corner Fe atoms. For 12.5 at.%Si, in addition to an A2 model, we deal with partial D03 models containing local D03-like layers consisting of edge-shared SiFe8 cubic clusters. For the cell-averaged bulk modulus, we have successfully reproduced the Si-concentration dependence as a monotonic decrease until 11.11 at.%Si and a recovery at 12.5 at.%Si. The analysis of local bulk moduli of SiFe8 cubic clusters and Fe regions is effective to understand the variations of the cell-averaged bulk modulus. The local bulk moduli of Fe regions become lower for increasing Si concentration, due to the suppression of bulk-like d-d bonding states in narrow Fe regions. For higher Si concentrations till 11.11 at.%Si, corner-shared contacts or 1D chains of SiFe8 clusters lead to remarkable reduction of local bulk moduli of the clusters. At 12 at.%Si, on the other hand, two- or three-dimensional arrangements of corner- or edge-shared SiFe8 cubic clusters show greatly enhanced local bulk moduli, due to quite different bonding nature with much stronger p-d hybridization. The relation among the local bulk moduli, local electronic and magnetic structures, and local configurations such as connectivity of SiFe8 clusters and Fe-region sizes has been analyzed. The ab initio local stress has opened the way for obtaining accurate local elastic properties reflecting local valence-electron behaviors.

Charge dynamics of 57Fe probe atoms in La2Li0.5Cu0.5O4

NASA Astrophysics Data System (ADS)

Presniakov, I. A.; Sobolev, A. V.; Rusakov, V. S.; Moskvin, A. S.; Baranov, A. V.

2018-06-01

The objective of this study is to characterize the electronic state and local surrounding of 57Fe Mössbauer probe atoms within iron-doped layered perovskite La2Li0.5Cu0.5O4 containing transition metal in unusual formal oxidation states "+3". An approach based on the qualitative energy diagrams analysis and the calculations within the cluster configuration interaction method have been developed. It was shown that a large amount of charge is transferred via Cu-O bonds from the O: 2p bands to the Cu: 3d orbitals and the ground state is dominated by the d9L configuration ("Cu2+-O-" state). The dominant d9L ground state for the (CuO6) sublattice induces in the environment of the 57Fe probe cations a charge transfer Fe3+ + O-(L) → Fe4+ + O2-, which transforms "Fe3+" into "Fe4+" state. The experimental spectra in the entire temperature range 77-300 K were described with the use of the stochastic two-level model based on the assumption of dynamic equilibrium between two Fe3+↔Fe4+ valence states related to the iron atom in the [Fe(1)O4]4- center. The relaxation frequencies and activation energies of the corresponding charge fluctuations were estimated based on Mössbauer data. The results are discussed assuming a temperature-induced change in the electronic state of the [CuO4]5- clusters in the layered perovskite.

Study of alloy disorder in quantum dots through multi-million atom simulations

NASA Technical Reports Server (NTRS)

Kilmeck, Gerhard; Oyafuso, Fabiano; Boykin, T. B.; Bowen, R. C.; von Allmen, Paul A.

2003-01-01

A tight binding model which includes s, p, d, s orbitals is used to examine the electronic structures of an ensemble of dome-shaped In0.6 Ga0.4 As quantum dots. Given ensembles of identically sized quantum dots, variations in composition and configuration yield a linewidth broadening of less than 0.35 meV, much smaller than the total broadening determined from photoluminescence experiments. It is also found that the computed disorder-induced broadening is very sensitive to the applied boundary conditions, so that care must be taken to ensure proper convergence of the numerical results. Examination of local eigenenergies as functions of position shows similar convergence problems and indicates that an inaccurate resolution of the equilibrium atomic positions due to truncation of the simulation domain may be the source of the slow ground state convergence.

Calculations of long-range three-body interactions for He(n0λS )-He(n0λS )-He(n0'λL )

NASA Astrophysics Data System (ADS)

Yan, Pei-Gen; Tang, Li-Yan; Yan, Zong-Chao; Babb, James F.

2018-04-01

We theoretically investigate long-range interactions between an excited L -state He atom and two identical S -state He atoms for the cases of the three atoms all in spin-singlet states or all in spin-triplet states, denoted by He(n0λS )-He(n0λS )-He(n0'λL ), with n0 and n0' principal quantum numbers, λ =1 or 3 the spin multiplicity, and L the orbital angular momentum of a He atom. Using degenerate perturbation theory for the energies up to second-order, we evaluate the coefficients C3 of the first-order dipolar interactions and the coefficients C6 and C8 of the second-order additive and nonadditive interactions. Both the dipolar and dispersion interaction coefficients, for these three-body degenerate systems, show dependences on the geometrical configurations of the three atoms. The nonadditive interactions start to appear in second-order. To demonstrate the results and for applications, the obtained coefficients Cn are evaluated with highly accurate variationally generated nonrelativistic wave functions in Hylleraas coordinates for He(1 1S ) -He(1 1S ) -He(2 1S ) , He(1 1S ) -He(1 1S ) -He(2 1P ) , He(2 1S ) -He(2 1S ) -He(2 1P ) , and He(2 3S ) -He(2 3S ) -He(2 3P ) . The calculations are given for three like nuclei for the cases of hypothetical infinite mass He nuclei, and of real finite mass 4He or 3He nuclei. The special cases of the three atoms in equilateral triangle configurations are explored in detail, and for the cases in which one of the atoms is in a P state, we also present results for the atoms in an isosceles right triangle configuration or in an equally spaced collinear configuration. The results can be applied to construct potential energy surfaces for three helium atom systems.

Cation Distribution and Local Configuration of Fe 2+ Ions in Structurally Nonequivalent Lattice Sites of Heterometallic Fe(II)/ M(II) ( M = Mn, Co, Ni, Cu, Zn) Diaquadiformato Complexes

NASA Astrophysics Data System (ADS)

Devillers, M.; Ladrière, J.

1993-03-01

57Fe Mössbauer investigations are carried out on a wide series of heterometallic diaquadiformato Fe(II)/ M(II) complexes with M = Mn, Co, Ni, Cu, and Zn to provide a local picture of the coordination environment of the 57Fe 2+ ions as a function of (i) the nature of the host cation and (ii) the relative amounts of both metals in the matrix (between 50 and 0.25 at.% Fe). Information is obtained on the quantitative distribution of both metals between the two structurally nonequivalent lattice sites and on the local geometry around the dopant atom in each crystal site. In the mixed Fe-Cu complexes. Fe 2+ ions are preferentially incorporated in the tetrahydrated site; in Cu-rich Fe xCu 1- x(HCO 2) 2· 2H 2O, the 57Fe 2+ ions located in the hexaformato-coordinated site are surrounded by an axially compressed octahedron of formate ligands which contrasts with the elongated configuration observed in the pure iron compound and in the other mixed systems. Semiquantitative estimations of the tetragonal field splitting and of the extent of metal-ligand interactions are proposed from the temperature dependence of the quadrupole splitting values.

Enhanced laboratory sensitivity to variation of the fine-structure constant using highly charged ions.

PubMed

Berengut, J C; Dzuba, V A; Flambaum, V V

2010-09-17

We study atomic systems that are in the frequency range of optical atomic clocks and have enhanced sensitivity to potential time variation of the fine-structure constant α. The high sensitivity is due to coherent contributions from three factors: high nuclear charge Z, high ionization degree, and significant differences in the configuration composition of the states involved. Configuration crossing keeps the frequencies in the optical range despite the large ionization energies. We discuss a few promising examples that have the largest α sensitivities seen in atomic systems.

Quantum transport through disordered 1D wires: Conductance via localized and delocalized electrons

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gopar, Víctor A.

Coherent electronic transport through disordered systems, like quantum wires, is a topic of fundamental and practical interest. In particular, the exponential localization of electron wave functions-Anderson localization-due to the presence of disorder has been widely studied. In fact, Anderson localization, is not an phenomenon exclusive to electrons but it has been observed in microwave and acoustic experiments, photonic materials, cold atoms, etc. Nowadays, many properties of electronic transport of quantum wires have been successfully described within a scaling approach to Anderson localization. On the other hand, anomalous localization or delocalization is, in relation to the Anderson problem, a less studiedmore » phenomenon. Although one can find signatures of anomalous localization in very different systems in nature. In the problem of electronic transport, a source of delocalization may come from symmetries present in the system and particular disorder configurations, like the so-called Lévy-type disorder. We have developed a theoretical model to describe the statistical properties of transport when electron wave functions are delocalized. In particular, we show that only two physical parameters determine the complete conductance distribution.« less

Invited Article: Autonomous assembly of atomically perfect nanostructures using a scanning tunneling microscope

DOE Office of Scientific and Technical Information (OSTI.GOV)

Celotta, Robert J., E-mail: robert.celotta@nist.gov, E-mail: joseph.stroscio@nist.gov; Hess, Frank M.; Rutter, Gregory M.

2014-12-15

A major goal of nanotechnology is to develop the capability to arrange matter at will by placing individual atoms at desired locations in a predetermined configuration to build a nanostructure with specific properties or function. The scanning tunneling microscope has demonstrated the ability to arrange the basic building blocks of matter, single atoms, in two-dimensional configurations. An array of various nanostructures has been assembled, which display the quantum mechanics of quantum confined geometries. The level of human interaction needed to physically locate the atom and bring it to the desired location limits this atom assembly technology. Here we report themore » use of autonomous atom assembly via path planning technology; this allows atomically perfect nanostructures to be assembled without the need for human intervention, resulting in precise constructions in shorter times. We demonstrate autonomous assembly by assembling various quantum confinement geometries using atoms and molecules and describe the benefits of this approach.« less

Ground Levels and Ionization Energies for the Neutral Atoms

National Institute of Standards and Technology Data Gateway

SRD 111 Ground Levels and Ionization Energies for the Neutral Atoms (Web, free access)   Data for ground state electron configurations and ionization energies for the neutral atoms (Z = 1-104) including references.

Instantaneous Normal Modes and the Protein Glass Transition

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schulz, Roland; Krishnan, Marimuthu; Daidone, Isabella

2009-01-01

In the instantaneous normal mode method, normal mode analysis is performed at instantaneous configurations of a condensed-phase system, leading to modes with negative eigenvalues. These negative modes provide a means of characterizing local anharmonicities of the potential energy surface. Here, we apply instantaneous normal mode to analyze temperature-dependent diffusive dynamics in molecular dynamics simulations of a small protein (a scorpion toxin). Those characteristics of the negative modes are determined that correlate with the dynamical (or glass) transition behavior of the protein, as manifested as an increase in the gradient with T of the average atomic mean-square displacement at ~ 220more » K. The number of negative eigenvalues shows no transition with temperature. Further, although filtering the negative modes to retain only those with eigenvectors corresponding to double-well potentials does reveal a transition in the hydration water, again, no transition in the protein is seen. However, additional filtering of the protein double-well modes, so as to retain only those that, on energy minimization, escape to different regions of configurational space, finally leads to clear protein dynamical transition behavior. Partial minimization of instantaneous configurations is also found to remove nondiffusive imaginary modes. In summary, examination of the form of negative instantaneous normal modes is shown to furnish a physical picture of local diffusive dynamics accompanying the protein glass transition.« less

Instantaneous Normal Modes and the Protein Glass Transition

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schultz, Roland; Krishnan, Marimuthu; Daidone, Isabella

2009-01-01

In the instantaneous normal mode method, normal mode analysis is performed at instantaneous configurations of a condensed-phase system, leading to modes with negative eigenvalues. These negative modes provide a means of characterizing local anharmonicities of the potential energy surface. Here, we apply instantaneous normal mode to analyze temperature-dependent diffusive dynamics in molecular dynamics simulations of a small protein (a scorpion toxin). Those characteristics of the negative modes are determined that correlate with the dynamical (or glass) transition behavior of the protein, as manifested as an increase in the gradient with T of the average atomic mean-square displacement at 220 K.more » The number of negative eigenvalues shows no transition with temperature. Further, although filtering the negative modes to retain only those with eigenvectors corresponding to double-well potentials does reveal a transition in the hydration water, again, no transition in the protein is seen. However, additional filtering of the protein double-well modes, so as to retain only those that, on energy minimization, escape to different regions of configurational space, finally leads to clear protein dynamical transition behavior. Partial minimization of instantaneous configurations is also found to remove nondiffusive imaginary modes. In summary, examination of the form of negative instantaneous normal modes is shown to furnish a physical picture of local diffusive dynamics accompanying the protein glass transition.« less

The displacement effect of a fluorine atom in CaF2 on the band structure

NASA Astrophysics Data System (ADS)

Mir, A.; Zaoui, A.; Bensaid, D.

2018-05-01

We obtained the results for each configuration [100], [110] and [111] and each configuration contains two atoms of calcium and four fluorine atoms with lattice type B. This study was made by a code that is based on the DFT called wien2k. The results obtained are in good agreement with the experiment. For CaF2, an important variation of the fluoride ions concentration in CaF2 after displacement has been observed on the map of e-Density. The interpretation of the results is based on the existence of an important number of defects which are created by changing the atomic positions inside of sub lattice.

N incorporation and associated localized vibrational modes in GaSb

NASA Astrophysics Data System (ADS)

Buckeridge, J.; Scanlon, D. O.; Veal, T. D.; Ashwin, M. J.; Walsh, A.; Catlow, C. R. A.

2014-01-01

We present results of electronic structure calculations on the N-related localized vibrational modes in the dilute nitride alloy GaSb1-xNx. By calculating the formation energies of various possible N incorporation modes in the alloy, we determine the most favorable N configurations, and we calculate their vibrational mode frequencies using density functional theory under the generalized gradient approximation to electron exchange and correlation, including the effects of the relativistic spin-orbit interactions. For a single N impurity, we find substitution on an Sb site, NSb, to be most favorable, and for a two-N-atom complex, we find the N-N split interstitial on an Sb site to be most favorable. For these defects, as well as, for comparison, defects comprising two N atoms on neighboring Sb sites and a N-Sb split interstitial on an Sb site, we find well-localized vibration modes (LVMs), which should be experimentally observable. The frequency of the triply degenerate LVM associated with NSb is determined to be 427.6 cm-1. Our results serve as a guide to future experimental studies to elucidate the incorporation of small concentrations of N in GaSb, which is known to lead to a reduction of the band gap and opens the possibility of using the material for long-wavelength applications.

Atomic alignment effect in the dissociative energy transfer reaction of metal carbonyls (Fe(CO)5, Ni(CO)4) with oriented Ar (3P2, M(J) = 2).

PubMed

Ohoyama, H; Matsuura, Y

2011-10-13

The atomic alignment effect has been studied for the dissociative energy transfer reaction of metal carbonyls (Fe(CO)(5), Ni(CO)(4)) with the oriented Ar ((3)P(2), M(J) = 2). The emission intensity from the excited metal products (Fe*, Ni*) has been measured as a function of the atomic alignment in the collision frame. The selectivity of the atomic orbital alignment of Ar ((3)P(2), M(J) = 2) (rank 2 moment, a(2)) is found to be opposite for the two reaction systems; the Fe(CO)(5) reaction is favorable at the Π configuration (positive a(2)), while the Ni(CO)(4) reaction is favorable at the Σ configuration (negative a(2)). Moreover, a significant spin alignment effect (rank 4 moment, a(4)) is recognized only in the Ni(CO)(4) reaction. The atomic alignment effect turns out to be essentially different between the two reaction systems; the Fe(CO)(5) reaction is controlled by the configuration of the half-filled 3p atomic orbital of Ar ((3)P(2)) in the collision frame (L dependence), whereas the Ni(CO)(4) reaction is controlled by the configuration of the total angular moment J (including spin) of Ar ((3)P(2)) in the collision frame (J dependence). As the origin of J dependence observed only in the Ni(CO)(4) reaction, the correlation (and/or the interference) between two electron exchange processes via the electron rearrangements is proposed.

An atomic gravitational wave interferometric sensor in low earth orbit (AGIS-LEO)

NASA Astrophysics Data System (ADS)

Hogan, Jason M.; Johnson, David M. S.; Dickerson, Susannah; Kovachy, Tim; Sugarbaker, Alex; Chiow, Sheng-Wey; Graham, Peter W.; Kasevich, Mark A.; Saif, Babak; Rajendran, Surjeet; Bouyer, Philippe; Seery, Bernard D.; Feinberg, Lee; Keski-Kuha, Ritva

2011-07-01

We propose an atom interferometer gravitational wave detector in low Earth orbit (AGIS-LEO). Gravitational waves can be observed by comparing a pair of atom interferometers separated by a 30 km baseline. In the proposed configuration, one or three of these interferometer pairs are simultaneously operated through the use of two or three satellites in formation flight. The three satellite configuration allows for the increased suppression of multiple noise sources and for the detection of stochastic gravitational wave signals. The mission will offer a strain sensitivity of {<10^{-18}/sqrt{Hz}} in the 50mHz-10Hz frequency range, providing access to a rich scientific region with substantial discovery potential. This band is not currently addressed with the LIGO, VIRGO, or LISA instruments. We analyze systematic backgrounds that are relevant to the mission and discuss how they can be mitigated at the required levels. Some of these effects do not appear to have been considered previously in the context of atom interferometry, and we therefore expect that our analysis will be broadly relevant to atom interferometric precision measurements. Finally, we present a brief conceptual overview of shorter-baseline ({lesssim100 m}) atom interferometer configurations that could be deployed as proof-of-principle instruments on the International Space Station (AGIS-ISS) or an independent satellite.

Infiltrated Zinc Oxide in Poly(methyl methacrylate): An Atomic Cycle Growth Study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ocola, Leonidas E.; Connolly, Aine; Gosztola, David J.

We have investigated the growth of zinc oxide in a polymer matrix by sequential infiltration synthesis (SiS). The atomic cycle-by-cycle self-terminating reaction growth investigation was done using photoluminescence (PL), Raman, and X-ray photoemission spectroscopy (XPS). Results show clear differences between Zn atom configurations at the initial stages of growth. Mono Zn atoms (O-Zn and O-Zn-O) exhibit pure UV emission with little evidence of deep level oxygen vacancy states (VO). Dimer Zn atoms (O-Zn-O-Zn and O-Zn-O-Zn-O) show strong UV and visible PL emission from VO states 20 times greater than that from the mono Zn atom configuration. After three precursor cycles,more » the PL emission intensity drops significantly exhibiting first evidence of crystal formation as observed with Raman spectroscopy via the presence of longitudinal optical phonons. We also report a first confirmation of energy transfer between polymer and ZnO where the polymer absorbs light at 241 nm and emits at 360 nm, which coincides with the ZnO UV emission peak. Our work shows that ZnO dimers are unique ZnO configurations with high PL intensity, unique O1s oxidation states, and sub-10 ps absorption and decay, which are interesting properties for novel quantum material applications.« less

Mechanochemical formation of heterogeneous diamond structures during rapid uniaxial compression in graphite

NASA Astrophysics Data System (ADS)

Kroonblawd, Matthew P.; Goldman, Nir

2018-05-01

We predict mechanochemical formation of heterogeneous diamond structures from rapid uniaxial compression in graphite using quantum molecular dynamics simulations. Ensembles of simulations reveal the formation of different diamondlike products starting from thermal graphite crystal configurations. We identify distinct classes of final products with characteristic probabilities of formation, stress states, and electrical properties and show through simulations of rapid quenching that these products are nominally stable and can be recovered at room temperature and pressure. Some of the diamond products exhibit significant disorder and partial closure of the energy gap between the highest-occupied and lowest-unoccupied molecular orbitals (i.e., the HOMO-LUMO gap). Seeding atomic vacancies in graphite significantly biases toward forming products with small HOMO-LUMO gap. We show that a strong correlation between the HOMO-LUMO gap and disorder in tetrahedral bonding configurations informs which kinds of structural defects are associated with gap closure. The rapid diffusionless transformation of graphite is found to lock vacancy defects into the final diamond structure, resulting in configurations that prevent s p3 bonding and lead to localized HOMO and LUMO states with a small gap.

Role of thermal history in atomic dynamics of chalcogenide glass: A case study on Ge{sub 20}Te{sub 80} glass

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sharma, Yashika; Kalra, Geetanjali; Murugavel, Sevi, E-mail: murug@physics.du.ac.in

The non-existence of thermodynamic equilibrium in glasses, their thermal history plays a very crucial role in explaining the relaxation behavior in various time scales and its configurational states. More importantly, the associated relaxation behavior is related mainly to the structural phenomenon of the glasses. Here, we report the dependence of quenching rate on the variation of structural units. The local structures of these glasses are monitored by recording the Raman spectroscopy and related to the different configurational states. The observed variations in structural differences are reflected in the measured density of the corresponding glasses. The quenching rate dependent of themore » relative fractions of edge-shared and corner-shared GeTe{sub 4} tetrahedral units are shown to be consistent with the corresponding variations in the measured density values.« less

X-alpha calculation of transition energies in multiply ionized atoms

NASA Technical Reports Server (NTRS)

Ringers, D. A.; Chen, M. H.

1974-01-01

It is shown that the accuracy of calculations can be improved if appropriate (different) values of alpha are used for each configuration. Alternatively, the Slater Transition state can be used, wherein a total energy difference is related to a difference in single electron eigenvalues. By a series expansion, the value of alpha for an excited configuration can be related to its value for the ground state configuration. The terms Delta alpha (delta Epsilon/delta alpha) exhibit a similar dependence on atomic number as the ground state values of alpha. Results of sample calculations are reported and compared with experiment.

Single photon at a configurable quantum-memory-based beam splitter

NASA Astrophysics Data System (ADS)

Guo, Xianxin; Mei, Yefeng; Du, Shengwang

2018-06-01

We report the demonstration of a configurable coherent quantum-memory-based beam splitter (BS) for a single-photon wave packet making use of laser-cooled 85Rb atoms and electromagnetically induced transparency. The single-photon wave packet is converted (stored) into a collective atomic spin state and later retrieved (split) into two nearly opposing directions. The storage time, beam-splitting ratio, and relative phase are configurable and can be dynamically controlled. We experimentally confirm that such a BS preserves the quantum particle nature of the single photon and the coherence between the two split wave packets of the single photon.

Multiscale approach to the determination of the photoactive yellow protein signaling state ensemble.

PubMed

A Rohrdanz, Mary; Zheng, Wenwei; Lambeth, Bradley; Vreede, Jocelyne; Clementi, Cecilia

2014-10-01

The nature of the optical cycle of photoactive yellow protein (PYP) makes its elucidation challenging for both experiment and theory. The long transition times render conventional simulation methods ineffective, and yet the short signaling-state lifetime makes experimental data difficult to obtain and interpret. Here, through an innovative combination of computational methods, a prediction and analysis of the biological signaling state of PYP is presented. Coarse-grained modeling and locally scaled diffusion map are first used to obtain a rough bird's-eye view of the free energy landscape of photo-activated PYP. Then all-atom reconstruction, followed by an enhanced sampling scheme; diffusion map-directed-molecular dynamics are used to focus in on the signaling-state region of configuration space and obtain an ensemble of signaling state structures. To the best of our knowledge, this is the first time an all-atom reconstruction from a coarse grained model has been performed in a relatively unexplored region of molecular configuration space. We compare our signaling state prediction with previous computational and more recent experimental results, and the comparison is favorable, which validates the method presented. This approach provides additional insight to understand the PYP photo cycle, and can be applied to other systems for which more direct methods are impractical.

Morphology dependent near-field response in atomistic plasmonic nanocavities.

PubMed

Chen, Xing; Jensen, Lasse

2018-06-21

In this work we examine how the atomistic morphologies of plasmonic dimers control the near-field response by using an atomistic electrodynamics model. At large separations, the field enhancement in the junction follows a simple inverse power law as a function of the gap separation, which agrees with classical antenna theory. However, when the separations are smaller than 0.8 nm, the so-called quantum size regime, the field enhancement is screened and thus deviates from the simple power law. Our results show that the threshold distance for the deviation depends on the specific morphology of the junction. The near field in the junction can be localized to an area of less than 1 nm2 in the presence of an atomically sharp tip, but the separation distances leading to a large confinement of near field depend strongly on the specific atomistic configuration. More importantly, the highly confined fields lead to large field gradients particularly in a tip-to-surface junction, which indicates that such a plasmonic structure favors observing strong field gradient effects in near-field spectroscopy. We find that for atomically sharp tips the field gradient becomes significant and depends strongly on the local morphology of a tip. We expect our findings to be crucial for understanding the origin of high-resolution near-field spectroscopy and for manipulating optical cavities through atomic structures in the strongly coupled plasmonic systems.

Alternative types of molecule-decorated atomic chains in Au–CO–Au single-molecule junctions

PubMed Central

Balogh, Zoltán; Makk, Péter

2015-01-01

Summary We investigate the formation and evolution of Au–CO single-molecule break junctions. The conductance histogram exhibits two distinct molecular configurations, which are further investigated by a combined statistical analysis. According to conditional histogram and correlation analysis these molecular configurations show strong anticorrelations with each other and with pure Au monoatomic junctions and atomic chains. We identify molecular precursor configurations with somewhat higher conductance, which are formed prior to single-molecule junctions. According to detailed length analysis two distinct types of molecule-affected chain-formation processes are observed, and we compare these results to former theoretical calculations considering bridge- and atop-type molecular configurations where the latter has reduced conductance due to destructive Fano interference. PMID:26199840

Alternative types of molecule-decorated atomic chains in Au-CO-Au single-molecule junctions.

PubMed

Balogh, Zoltán; Makk, Péter; Halbritter, András

2015-01-01

We investigate the formation and evolution of Au-CO single-molecule break junctions. The conductance histogram exhibits two distinct molecular configurations, which are further investigated by a combined statistical analysis. According to conditional histogram and correlation analysis these molecular configurations show strong anticorrelations with each other and with pure Au monoatomic junctions and atomic chains. We identify molecular precursor configurations with somewhat higher conductance, which are formed prior to single-molecule junctions. According to detailed length analysis two distinct types of molecule-affected chain-formation processes are observed, and we compare these results to former theoretical calculations considering bridge- and atop-type molecular configurations where the latter has reduced conductance due to destructive Fano interference.

Local light-induced magnetization using nanodots and chiral molecules.

PubMed

Dor, Oren Ben; Morali, Noam; Yochelis, Shira; Baczewski, Lech Tomasz; Paltiel, Yossi

2014-11-12

With the increasing demand for miniaturization, nanostructures are likely to become the primary components of future integrated circuits. Different approaches are being pursued toward achieving efficient electronics, among which are spin electronics devices (spintronics). In principle, the application of spintronics should result in reducing the power consumption of electronic devices. Recently a new, promising, effective approach for spintronics has emerged, using spin selectivity in electron transport through chiral molecules. In this work, using chiral molecules and nanocrystals, we achieve local spin-based magnetization generated optically at ambient temperatures. Through the chiral layer, a spin torque can be transferred without permanent charge transfer from the nanocrystals to a thin ferromagnetic layer, creating local perpendicular magnetization. We used Hall sensor configuration and atomic force microscopy (AFM) to measure the induced local magnetization. At low temperatures, anomalous spin Hall effects were measured using a thin Ni layer. The results may lead to optically controlled spintronics logic devices that will enable low power consumption, high density, and cheap fabrication.

Electrochemically assisted localized etching of ZnO single crystals in water using a catalytically active Pt-coated atomic force microscopy probe

NASA Astrophysics Data System (ADS)

Shibata, Takayuki; Yamamoto, Kota; Sasano, Junji; Nagai, Moeto

2017-09-01

This paper presents a nanofabrication technique based on the electrochemically assisted chemical dissolution of zinc oxide (ZnO) single crystals in water at room temperature using a catalytically active Pt-coated atomic force microscopy (AFM) probe. Fabricated grooves featured depths and widths of several tens and several hundreds of nanometers, respectively. The material removal rate of ZnO was dramatically improved by controlling the formation of hydrogen ions (H+) on the surface of the catalytic Pt-coated probe via oxidation of H2O molecules; this reaction can be enhanced by applying a cathodic potential to an additional Pt-wire working electrode in a three-electrode configuration. Consequently, ZnO can be dissolved chemically in water as a soluble Zn2+ species via a reaction with H+ species present in high concentrations in the immediate vicinity of the AFM tip apex.

Modeling the structural, dynamical, and magnetic properties of liquid Al1-xMnx ( x=0.14 , 0.2, and 0.4): A first-principles investigation

NASA Astrophysics Data System (ADS)

Jakse, N.; Pasturel, A.

2007-07-01

We report the results of first-principles molecular dynamics simulations of liquid Al1-xMnx alloys at three different compositions. The local structure as defined by the Bhatia-Thornton partial structure factors is found to display significant changes at x=0.4 . In addition, a structural analysis using three-dimensional pair-analysis techniques evidences a fivefold symmetry around x=0.14 , in agreement with the experimental quasicrystal-forming range, and an increasing complexity of the Frank-Kasper polytetrahedral symmetry around Mn atoms at x=0.4 . We also examine the time evolution of the configurations at the three compositions in terms of the mean-square displacements and self-diffusion coefficients. Finally, we show a strong interplay between the structural changes and the evolution of the magnetic properties of the Mn atoms as a function of composition.

Single-ion microwave near-field quantum sensor

NASA Astrophysics Data System (ADS)

Wahnschaffe, M.; Hahn, H.; Zarantonello, G.; Dubielzig, T.; Grondkowski, S.; Bautista-Salvador, A.; Kohnen, M.; Ospelkaus, C.

2017-01-01

We develop an intuitive model of 2D microwave near-fields in the unusual regime of centimeter waves localized to tens of microns. Close to an intensity minimum, a simple effective description emerges with five parameters that characterize the strength and spatial orientation of the zero and first order terms of the near-field, as well as the field polarization. Such a field configuration is realized in a microfabricated planar structure with an integrated microwave conductor operating near 1 GHz. We use a single 9 Be+ ion as a high-resolution quantum sensor to measure the field distribution through energy shifts in its hyperfine structure. We find agreement with simulations at the sub-micron and few-degree level. Our findings give a clear and general picture of the basic properties of oscillatory 2D near-fields with applications in quantum information processing, neutral atom trapping and manipulation, chip-scale atomic clocks, and integrated microwave circuits.

Coherent Population Trapping in a Superconducting Phase Qubit

NASA Astrophysics Data System (ADS)

Kelly, William R.; Dutton, Zachary; Ohki, Thomas A.; Schlafer, John; Mookerji, Bhaskar; Kline, Jeffery S.; Pappas, David P.

2010-03-01

The phenomenon of Coherent Population Trapping (CPT) of an atom (or solid state ``artificial atom''), and the associated effect of Electromagnetically Induced Transparency (EIT), are clear demonstrations of quantum interference due to coherence in multi-level quantum systems. We report observation of CPT in a superconducting phase qubit by simultaneously driving two coherent transitions in a λ-type configuration, utilizing the three lowest lying levels of a local minimum of the phase qubit. We observe ˜60% suppression of excited state population under conditions of two-photon resonance, where EIT and CPT are expected to occur. We present data and matching theoretical simulations showing the development of CPT in time. We also used the observed time dependence of the excited state population to characterize quantum dephasing times of the system, as predicted in [1]. [1] K.V. Murali, Z. Dutton, W.D. Oliver, D.S. Crankshaw, and T.P.Orlando, Phys. Rev. Lett. 93, 087003 (2004).

Dielectric function for doped graphene layer with barium titanate

NASA Astrophysics Data System (ADS)

Martinez Ramos, Manuel; Garces Garcia, Eric; Magana, Fernado; Vazquez Fonseca, Gerardo Jorge

2015-03-01

The aim of our study is to calculate the dielectric function for a system formed with a graphene layer doped with barium titanate. Density functional theory, within the local density approximation, plane-waves and pseudopotentials scheme as implemented in Quantum Espresso suite of programs was used. We considered 128 carbon atoms with a barium titanate cluster of 11 molecules as unit cell with periodic conditions. The geometry optimization is achieved. Optimization of structural configuration is performed by relaxation of all atomic positions to minimize their total energies. Band structure, density of states and linear optical response (the imaginary part of dielectric tensor) were calculated. We thank Dirección General de Asuntos del Personal Académico de la Universidad Nacional Autónoma de México, partial financial support by Grant IN-106514 and we also thank Miztli Super-Computing center the technical assistance.

The evolving quality of frictional contact with graphene.

PubMed

Li, Suzhi; Li, Qunyang; Carpick, Robert W; Gumbsch, Peter; Liu, Xin Z; Ding, Xiangdong; Sun, Jun; Li, Ju

2016-11-24

Graphite and other lamellar materials are used as dry lubricants for macroscale metallic sliding components and high-pressure contacts. It has been shown experimentally that monolayer graphene exhibits higher friction than multilayer graphene and graphite, and that this friction increases with continued sliding, but the mechanism behind this remains subject to debate. It has long been conjectured that the true contact area between two rough bodies controls interfacial friction. The true contact area, defined for example by the number of atoms within the range of interatomic forces, is difficult to visualize directly but characterizes the quantity of contact. However, there is emerging evidence that, for a given pair of materials, the quality of the contact can change, and that this can also strongly affect interfacial friction. Recently, it has been found that the frictional behaviour of two-dimensional materials exhibits traits unlike those of conventional bulk materials. This includes the abovementioned finding that for few-layer two-dimensional materials the static friction force gradually strengthens for a few initial atomic periods before reaching a constant value. Such transient behaviour, and the associated enhancement of steady-state friction, diminishes as the number of two-dimensional layers increases, and was observed only when the two-dimensional material was loosely adhering to a substrate. This layer-dependent transient phenomenon has not been captured by any simulations. Here, using atomistic simulations, we reproduce the experimental observations of layer-dependent friction and transient frictional strengthening on graphene. Atomic force analysis reveals that the evolution of static friction is a manifestation of the natural tendency for thinner and less-constrained graphene to re-adjust its configuration as a direct consequence of its greater flexibility. That is, the tip atoms become more strongly pinned, and show greater synchrony in their stick-slip behaviour. While the quantity of atomic-scale contacts (true contact area) evolves, the quality (in this case, the local pinning state of individual atoms and the overall commensurability) also evolves in frictional sliding on graphene. Moreover, the effects can be tuned by pre-wrinkling. The evolving contact quality is critical for explaining the time-dependent friction of configurationally flexible interfaces.

Sulfur Adsorption on the Goethite (110) Surface

NASA Astrophysics Data System (ADS)

Simonetti, S.; Damiani, D.; Brizuela, G.; Juan, A.

The electronic structure of S adsorption on goethite (110) surface has been studied by ASED-MO cluster calculations. For S location, the most exposed surface atoms of goethite surface were selected. The calculations show that the surface offers several places for S adsorption. The most energetically stable system corresponds to S location above H atom. We studied in detail the configurations that correspond to the higher OP values. For these configurations, the H-S and Fe-S computed distances are 2.1 and 3.7 Å, respectively. The H-S and Fe-S are mainly bonding interaction with OP values of 0.156 and 0.034, respectively. The Fe-S interaction mainly involves Fe 3dx2-y2 atomic orbitals with lesser participation of Fe 4py and Fe 3dyz atomic orbitals. The O-S interaction shows the same bonding and antibonding contributions giving a small OP value. The O-S interaction involves O 2p orbitals. There is an electron transfer to the Fe atom from the S atom. On the other hand, there is an electron transfer to S atom from the H and O atoms, respectively.

A project based on multi-configuration Dirac-Fock calculations for plasma spectroscopy

NASA Astrophysics Data System (ADS)

Comet, M.; Pain, J.-C.; Gilleron, F.; Piron, R.

2017-09-01

We present a project dedicated to hot plasma spectroscopy based on a Multi-Configuration Dirac-Fock (MCDF) code, initially developed by J. Bruneau. The code is briefly described and the use of the transition state method for plasma spectroscopy is detailed. Then an opacity code for local-thermodynamic-equilibrium plasmas using MCDF data, named OPAMCDF, is presented. Transition arrays for which the number of lines is too large to be handled in a Detailed Line Accounting (DLA) calculation can be modeled within the Partially Resolved Transition Array method or using the Unresolved Transition Arrays formalism in jj-coupling. An improvement of the original Partially Resolved Transition Array method is presented which gives a better agreement with DLA computations. Comparisons with some absorption and emission experimental spectra are shown. Finally, the capability of the MCDF code to compute atomic data required for collisional-radiative modeling of plasma at non local thermodynamic equilibrium is illustrated. In addition to photoexcitation, this code can be used to calculate photoionization, electron impact excitation and ionization cross-sections as well as autoionization rates in the Distorted-Wave or Close Coupling approximations. Comparisons with cross-sections and rates available in the literature are discussed.

Measurement of the first ionization potential of lawrencium, element 103.

PubMed

Sato, T K; Asai, M; Borschevsky, A; Stora, T; Sato, N; Kaneya, Y; Tsukada, K; Düllmann, Ch E; Eberhardt, K; Eliav, E; Ichikawa, S; Kaldor, U; Kratz, J V; Miyashita, S; Nagame, Y; Ooe, K; Osa, A; Renisch, D; Runke, J; Schädel, M; Thörle-Pospiech, P; Toyoshima, A; Trautmann, N

2015-04-09

The chemical properties of an element are primarily governed by the configuration of electrons in the valence shell. Relativistic effects influence the electronic structure of heavy elements in the sixth row of the periodic table, and these effects increase dramatically in the seventh row--including the actinides--even affecting ground-state configurations. Atomic s and p1/2 orbitals are stabilized by relativistic effects, whereas p3/2, d and f orbitals are destabilized, so that ground-state configurations of heavy elements may differ from those of lighter elements in the same group. The first ionization potential (IP1) is a measure of the energy required to remove one valence electron from a neutral atom, and is an atomic property that reflects the outermost electronic configuration. Precise and accurate experimental determination of IP1 gives information on the binding energy of valence electrons, and also, therefore, on the degree of relativistic stabilization. However, such measurements are hampered by the difficulty in obtaining the heaviest elements on scales of more than one atom at a time. Here we report that the experimentally obtained IP1 of the heaviest actinide, lawrencium (Lr, atomic number 103), is 4.96(+0.08)(-0.07) electronvolts. The IP1 of Lr was measured with (256)Lr (half-life 27 seconds) using an efficient surface ion-source and a radioisotope detection system coupled to a mass separator. The measured IP1 is in excellent agreement with the value of 4.963(15) electronvolts predicted here by state-of-the-art relativistic calculations. The present work provides a reliable benchmark for theoretical calculations and also opens the way for IP1 measurements of superheavy elements (that is, transactinides) on an atom-at-a-time scale.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Katoch, Neha, E-mail: nehakatoch2@gmail.com; Kapoor, Pooja; Sharma, Munish

We report stability and electronic properties of benzene molecule adsorbed on the Au atomic layer within the framework of density function theory (DFT). Horizontal configuration of benzene on the top site of Au monolayer prefers energetically over other studied configurations. On the adsorption of benzene, the ballistic conductance of Au monolayer is found to decrease from 4G{sub 0} to 2G{sub 0} suggesting its applications for the fabrications of organic sensor devices based on the Au atomic layers.

Evaluation of atomic constants for optical radiation, volume 2

NASA Technical Reports Server (NTRS)

Kylstra, C. D.; Schneider, R. J.

1974-01-01

Various atomic constant for 23 elements from helium to mercury were computed and are presented in tables. The data given for each element start with the element name, its atomic number, its ionic state, and the designation and series limit for each parent configuration. This is followed by information on the energy level, parent configuration, and designation for each term available to the program. The matrix elements subtables are ordered by the sequence numbers, which represent the initial and final levels of the transitions. Each subtable gives the following: configuration of the core or parent, designation and energy level for the reference state, effective principal quantum number, energy of the series limit, value of the matrix element for the reference state interacting with itself, and sum of all of the dipole matrix elements listed in the subtable. Dipole and quadrupole interaction data are also given.

DFT investigation of the vibrational properties of GC Watson-Crick and Hoogsteen base pairs in the presence of Mg²⁺, Ca²⁺, and Cu²⁺ ions.

PubMed

Morari, Cristian; Muntean, Cristina M; Tripon, Carmen; Buimaga-Iarinca, Luiza; Calborean, Adrian

2014-04-01

The binding effects of Mg²⁺, Ca²⁺, and Cu²⁺ ions on the vibrational properties of guanine-cytosine base pairs have been performed using density functional theory investigations. Both Watson-Crick and Hoogsteen configurations of the base pairs were investigated. In Watson-Crick configuration, the metal was coordinated at N7 atom of guanine, while in the case of Hoogsteen configuration, the coordination is at N3 atom of guanine. We have pointed out the geometric properties of the metal-GC base pairs structure, as well as the vibrational bands that can be used to detect the presence of metallic ions in the Watson-Crick and Hoogsteen GC structures. For the geometric models used by us, the vibrational amplitudes of metallic atoms were stronger for wavenumbers lower than 500 cm⁻¹. This suggests that in the experimental studies on DNA the presence of the three metallic atoms (Mg, Ca, and Cu) can be explicitly detected at low frequencies.

Characterization of Structural and Configurational Properties of DNA by Atomic Force Microscopy.

PubMed

Meroni, Alice; Lazzaro, Federico; Muzi-Falconi, Marco; Podestà, Alessandro

2018-01-01

We describe a method to extract quantitative information on DNA structural and configurational properties from high-resolution topographic maps recorded by atomic force microscopy (AFM). DNA molecules are deposited on mica surfaces from an aqueous solution, carefully dehydrated, and imaged in air in Tapping Mode. Upon extraction of the spatial coordinates of the DNA backbones from AFM images, several parameters characterizing DNA structure and configuration can be calculated. Here, we explain how to obtain the distribution of contour lengths, end-to-end distances, and gyration radii. This modular protocol can be also used to characterize other statistical parameters from AFM topographies.

Potentialities of a new sigma(+)-sigma(-)laser configuration for radiative cooling and trapping

NASA Astrophysics Data System (ADS)

Dalibard, J.; Reynaud, S.; Cohen-Tannoudji, C.

1984-11-01

In the process of cooling and trapping neutral atoms, a new laser configuration is investigated which consists of two counterpropagating laser beams with orthogonal sigma(+) and sigma(-)polarizations. It is shown that such a configuration looks more promising than an ordinary standing wave (where the two counterpropagating waves have the same polarization), and this result is explained as being due to angular momentum conservation which prevents any coherent redistribution of photons between the two waves. The present conclusions are based on a quantitative calculation of the various parameters (potential depth, friction coefficient, diffusion coefficient) describing the mean value and the fluctuations of the radiative forces experienced, in such a laser configuration, by an atom with a J = 0 ground state and a J = 1 excited state.

Structural and electronic properties of double-walled boron nitride nanocones

NASA Astrophysics Data System (ADS)

Brito, E.; Silva, T. S.; Guerra, T.; Leite, L.; Azevedo, S.; Freitas, A.; Kaschny, J. R.

2018-01-01

First principles calculations were applied to study the structural and electronic properties of different configurations of double-walled boron nitride nanocones with a disclination angle of 60°. The analysis includes different rotation angles, distance between apexes, as well as distinct types of antiphase boundaries. The calculations indicate that the non-rotated configuration of double-walled nanocone with a defective line composed by C and N atoms, forming C-N bonds, is the most stable configuration. It was found that the yam angle, apexes distance and defective line composition present significant influence on the electronic properties of such structures. Moreover, analyzing the spin charge density, for the electronic states near the Fermi level, it was also found that the configuration with a defective line containing C atoms presents a net magnetic moment.

Probing local bias-induced transitions using photothermal excitation contact resonance atomic force microscopy and voltage spectroscopy

DOE PAGES

Li, Qian; Jesse, Stephen; Tselev, Alexander; ...

2015-01-05

In this paper, nanomechanical properties are closely related to the states of matter, including chemical composition, crystal structure, mesoscopic domain configuration, etc. Investigation of these properties at the nanoscale requires not only static imaging methods, e.g., contact resonance atomic force microscopy (CR-AFM), but also spectroscopic methods capable of revealing their dependence on various external stimuli. Here we demonstrate the voltage spectroscopy of CR-AFM, which was realized by combining photothermal excitation (as opposed to the conventional piezoacoustic excitation method) with the band excitation technique. We applied this spectroscopy to explore local bias-induced phenomena ranging from purely physical to surface electromechanical andmore » electrochemical processes. Our measurements show that the changes in the surface properties associated with these bias-induced transitions can be accurately assessed in a fast and dynamic manner, using resonance frequency as a signature. Finally, with many of the advantages offered by photothermal excitation, contact resonance voltage spectroscopy not only is expected to find applications in a broader field of nanoscience but also will provide a basis for future development of other nanoscale elastic spectroscopies.« less

Direct Depth- and Lateral- Imaging of Nanoscale Magnets Generated by Ion Impact

PubMed Central

Röder, Falk; Hlawacek, Gregor; Wintz, Sebastian; Hübner, René; Bischoff, Lothar; Lichte, Hannes; Potzger, Kay; Lindner, Jürgen; Fassbender, Jürgen; Bali, Rantej

2015-01-01

Nanomagnets form the building blocks for a variety of spin-transport, spin-wave and data storage devices. In this work we generated nanoscale magnets by exploiting the phenomenon of disorder-induced ferromagnetism; disorder was induced locally on a chemically ordered, initially non-ferromagnetic, Fe60Al40 precursor film using  nm diameter beam of Ne+ ions at 25 keV energy. The beam of energetic ions randomized the atomic arrangement locally, leading to the formation of ferromagnetism in the ion-affected regime. The interaction of a penetrating ion with host atoms is known to be spatially inhomogeneous, raising questions on the magnetic homogeneity of nanostructures caused by ion-induced collision cascades. Direct holographic observations of the flux-lines emergent from the disorder-induced magnetic nanostructures were made in order to measure the depth- and lateral- magnetization variation at ferromagnetic/non-ferromagnetic interfaces. Our results suggest that high-resolution nanomagnets of practically any desired 2-dimensional geometry can be directly written onto selected alloy thin films using a nano-focussed ion-beam stylus, thus enabling the rapid prototyping and testing of novel magnetization configurations for their magneto-coupling and spin-wave properties. PMID:26584789

Heat Transfer to Surfaces of Finite Catalytic Activity in Frozen Dissociated Hypersonic Flow

NASA Technical Reports Server (NTRS)

Chung, Paul M.; Anderson, Aemer D.

1961-01-01

The heat transfer due to catalytic recombination of a partially dissociated diatomic gas along the surfaces of two-dimensional and axisymmetric bodies with finite catalytic efficiencies is studied analytically. An integral method is employed resulting in simple yet relatively complete solutions for the particular configurations considered. A closed form solution is derived which enables one to calculate atom mass-fraction distribution, therefore catalytic heat transfer distribution, along the surface of a flat plate in frozen compressible flow with and without transpiration. Numerical calculations are made to determine the atom mass-fraction distribution along an axisymmetric conical body with spherical nose in frozen hypersonic compressible flow. A simple solution based on a local similarity concept is found to be in good agreement with these numerical calculations. The conditions are given for which the local similarity solution is expected to be satisfactory. The limitations on the practical application of the analysis to the flight of the blunt bodies in the atmosphere are discussed. The use of boundary-layer theory and the assumption of frozen flow restrict application of the analysis to altitudes between about 150,000 and 250,000 feet.

Are strategies in physics discrete? A remote controlled investigation

NASA Astrophysics Data System (ADS)

Heck, Robert; Sherson, Jacob F.; www. scienceathome. org Team; players Team

2017-04-01

In science, strategies are formulated based on observations, calculations, or physical insight. For any given physical process, often several distinct strategies are identified. Are these truly distinct or simply low dimensional representations of a high dimensional continuum of solutions? Our online citizen science platform www.scienceathome.org used by more than 150,000 people recently enabled finding solutions to fast, 1D single atom transport [Nature2016]. Surprisingly, player trajectories bunched into discrete solution strategies (clans) yielding clear, distinct physical insight. Introducing the multi-dimensional vector in the direction of other local maxima we locate narrow, high-yield ``bridges'' connecting the clans. This demonstrates for this problem that a continuum of solutions with no clear physical interpretation does in fact exist. Next, four distinct strategies for creating Bose-Einstein condensates were investigated experimentally: hybrid and crossed dipole trap configurations in combination with either large volume or dimple loading from a magnetic trap. We find that although each conventional strategy appears locally optimal, ``bridges'' can be identified. In a novel approach, the problem was gamified allowing 750 citizen scientists to contribute to the experimental optimization yielding nearly a factor two improvement in atom number.

Chains of benzenes with lithium-atom adsorption: Vibrations and spontaneous symmetry breaking

NASA Astrophysics Data System (ADS)

Ortiz, Yenni P.; Stegmann, Thomas; Klein, Douglas J.; Seligman, Thomas H.

2017-09-01

We study effects of different configurations of adsorbates on the vibrational modes as well as symmetries of polyacenes and poly-p-phenylenes focusing on lithium atom adsorption. We found that the spectra of the vibrational modes distinguish the different configurations. For more regular adsorption schemes the lowest states are bending and torsion modes of the skeleton, which are essentially followed by the adsorbate. On poly-p-phenylenes we found that lithium adsorption reduces and often eliminates the torsion between rings thus increasing symmetry. There is spontaneous symmetry breaking in poly-p-phenylenes due to double adsorption of lithium atoms on alternating rings.

High-dimensional atom localization via spontaneously generated coherence in a microwave-driven atomic system.

PubMed

Wang, Zhiping; Chen, Jinyu; Yu, Benli

2017-02-20

We investigate the two-dimensional (2D) and three-dimensional (3D) atom localization behaviors via spontaneously generated coherence in a microwave-driven four-level atomic system. Owing to the space-dependent atom-field interaction, it is found that the detecting probability and precision of 2D and 3D atom localization behaviors can be significantly improved via adjusting the system parameters, the phase, amplitude, and initial population distribution. Interestingly, the atom can be localized in volumes that are substantially smaller than a cubic optical wavelength. Our scheme opens a promising way to achieve high-precision and high-efficiency atom localization, which provides some potential applications in high-dimensional atom nanolithography.

First principles calculation of the structural, electronic, and magnetic properties of Au-Pd atomic chains

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dave, Mudra R., E-mail: mdave-phy@yahoo.co.in; Sharma, A. C.

2015-06-24

The structural, electronic and magnetic properties of free standing Au-Pd bimetallic atomic chain is studied using ab-initio method. It is found that electronic and magnetic properties of chains depend on position of atoms and number of atoms. Spin polarization factor for different atomic configuration of atomic chain is calculated predicting a half metallic behavior. It suggests a total spin polarised transport in these chains.

New Theoretical Developments in Exploring Electronically Excited States: Including Localized Configuration Interaction Singles and Application to Large Helium Clusters

NASA Astrophysics Data System (ADS)

Closser, Kristina Danielle

This thesis presents new developments in excited state electronic structure theory. Contrasted with the ground state, the electronically excited states of atoms and molecules often are unstable and have short lifetimes, exhibit a greater diversity of character and are generally less well understood. The very unusual excited states of helium clusters motivated much of this work. These clusters consist of large numbers of atoms (experimentally 103--109 atoms) and bands of nearly degenerate excited states. For an isolated atom the lowest energy excitation energies are from 1s → 2s and 1s → 2 p transitions, and in clusters describing the lowest energy band minimally requires four states per atom. In the ground state the clusters are weakly bound by van der Waals interactions, however in the excited state they can form well-defined covalent bonds. The computational cost of quantum chemical calculations rapidly becomes prohibitive as the size of the systems increase. Standard excited-state methods such as configuration interaction singles (CIS) and time-dependent density functional theory (TD-DFT) can be used with ≈100 atoms, and are optimized to treat only a few states. Thus, one of our primary aims is to develop a method which can treat these large systems with large numbers of nearly degenerate excited states. Additionally, excited states are generally formed far from their equilibrium structures. Vertical excitations from the ground state induce dynamics in the excited states. Thus, another focus of this work is to explore the results of these forces and the fate of the excited states. Very little was known about helium cluster excited states when this work began, thus we first investigated the excitations in small helium clusters consisting of 7 or 25 atoms using CIS. The character of these excited states was determined using attachment/detachment density analysis and we found that in the n = 2 manifold the excitations could generally be interpreted as superpositions of atomic states with surface states appearing close to the atomic excitation energies and interior states being blue shifted by up to ≈2 eV. The dynamics resulting from excitation of He_7 were subsequently explored using ab initio molecular dynamics (AIMD). These simulations were performed with classical adiabatic dynamics coupled to a new state-following algorithm on CIS potential energy surfaces. Most clusters were found to completely dissociate and resulted in a single excited atomic state (90%), however, some trajectories formed bound, He*2 (3%), and a few yielded excited trimers (<0.5%). Comparisons were made with available experimental information on much larger clusters. Various applications of this state following algorithm are also presented. In addition to AIMD, these include excited-state geometry optimization and minimal energy path finding via the growing string method. When using state following we demonstrate that more physical results can be obtained with AIMD calculations. Also, the optimized geometries of three excited states of cytosine, two of which were not found without state following, and the minimal energy path between the lowest two singlet excited states of protonated formaldimine are offered as example applications. Finally, to address large clusters, a local variation of CIS was developed. This method exploits the properties of absolutely localized molecular orbitals (ALMOs) to limit the total number of excitations to scaling only linearly with cluster size, which results in formal scaling with the third power of the system size. The derivation of the equations and design of the algorithm are discussed in detail, and computational timings as well as a pilot application to the size dependence of the helium cluster spectrum are presented.

Surface Passivation in Empirical Tight Binding

NASA Astrophysics Data System (ADS)

He, Yu; Tan, Yaohua; Jiang, Zhengping; Povolotskyi, Michael; Klimeck, Gerhard; Kubis, Tillmann

2016-03-01

Empirical Tight Binding (TB) methods are widely used in atomistic device simulations. Existing TB methods to passivate dangling bonds fall into two categories: 1) Method that explicitly includes passivation atoms is limited to passivation with atoms and small molecules only. 2) Method that implicitly incorporates passivation does not distinguish passivation atom types. This work introduces an implicit passivation method that is applicable to any passivation scenario with appropriate parameters. This method is applied to a Si quantum well and a Si ultra-thin body transistor oxidized with SiO2 in several oxidation configurations. Comparison with ab-initio results and experiments verifies the presented method. Oxidation configurations that severely hamper the transistor performance are identified. It is also shown that the commonly used implicit H atom passivation overestimates the transistor performance.

Geometrical eigen-subspace framework based molecular conformation representation for efficient structure recognition and comparison

NASA Astrophysics Data System (ADS)

Li, Xiao-Tian; Yang, Xiao-Bao; Zhao, Yu-Jun

2017-04-01

We have developed an extended distance matrix approach to study the molecular geometric configuration through spectral decomposition. It is shown that the positions of all atoms in the eigen-space can be specified precisely by their eigen-coordinates, while the refined atomic eigen-subspace projection array adopted in our approach is demonstrated to be a competent invariant in structure comparison. Furthermore, a visual eigen-subspace projection function (EPF) is derived to characterize the surrounding configuration of an atom naturally. A complete set of atomic EPFs constitute an intrinsic representation of molecular conformation, based on which the interatomic EPF distance and intermolecular EPF distance can be reasonably defined. Exemplified with a few cases, the intermolecular EPF distance shows exceptional rationality and efficiency in structure recognition and comparison.

Atomic scale simulations of pyrochlore oxides with a tight-binding variable-charge model: implications for radiation tolerance.

PubMed

Sattonnay, G; Tétot, R

2014-02-05

Atomistic simulations with new interatomic potentials derived from a tight-binding variable-charge model were performed in order to investigate the lattice properties and the defect formation energies in Gd2Ti2O7 and Gd2Zr2O7 pyrochlores. The main objective was to determine the role played by the defect stability on the radiation tolerance of these compounds. Calculations show that the titanate has a more covalent character than the zirconate. Moreover, the properties of oxygen Frenkel pairs, cation antisite defects and cation Frenkel pairs were studied. In Gd2Ti2O7 the cation antisite defect and the Ti-Frenkel pair are not stable: they evolve towards more stable defect configurations during the atomic relaxation process. This phenomenon is driven by a decrease of the Ti coordination number down to five which leads to a local atomic reorganization and strong structural distortions around the defects. These kinds of atomic rearrangements are not observed around defects in Gd2Zr2O7. Therefore, the defect stability in A2B2O7 depends on the ability of B atoms to accommodate high coordination number (higher than six seems impossible for Ti). The accumulation of structural distortions around Ti-defects due to this phenomenon could drive the Gd2Ti2O7 amorphization induced by irradiation.

Electronic and Spatial Structures of Water-Soluble Dinitrosyl Iron Complexes with Thiol-Containing Ligands Underlying Their Ability to Act as Nitric Oxide and Nitrosonium Ion Donors

PubMed Central

Vanin, Anatoly F.; Burbaev, Dosymzhan Sh.

2011-01-01

The ability of mononuclear dinitrosyl iron commplexes (M-DNICs) with thiolate ligands to act as NO donors and to trigger S-nitrosation of thiols can be explain only in the paradigm of the model of the [Fe+(NO+)2] core ({Fe(NO)2}7 according to the Enemark-Feltham classification). Similarly, the {(RS−)2Fe+(NO+)2}+ structure describing the distribution of unpaired electron density in M-DNIC corresponds to the low-spin (S = 1/2) state with a d7 electron configuration of the iron atom and predominant localization of the unpaired electron on MO(dz2) and the square planar structure of M-DNIC. On the other side, the formation of molecular orbitals of M-DNIC including orbitals of the iron atom, thiolate and nitrosyl ligands results in a transfer of electron density from sulfur atoms to the iron atom and nitrosyl ligands. Under these conditions, the positive charge on the nitrosyl ligands diminishes appreciably, the interaction of the ligands with hydroxyl ions or with thiols slows down and the hydrolysis of nitrosyl ligands and the S-nitrosating effect of the latter are not manifested. Most probably, the S-nitrosating effect of nitrosyl ligands is a result of weak binding of thiolate ligands to the iron atom under conditions favoring destabilization of M-DNIC. PMID:22505886

Electronic and spatial structures of water-soluble dinitrosyl iron complexes with thiol-containing ligands underlying their ability to act as nitric oxide and nitrosonium ion donors.

PubMed

Vanin, Anatoly F; Burbaev, Dosymzhan Sh

2011-01-01

The ability of mononuclear dinitrosyl iron commplexes (M-DNICs) with thiolate ligands to act as NO donors and to trigger S-nitrosation of thiols can be explain only in the paradigm of the model of the [Fe(+)(NO(+))(2)] core ({Fe(NO)(2)}(7) according to the Enemark-Feltham classification). Similarly, the {(RS(-))(2)Fe(+)(NO(+))(2)}(+) structure describing the distribution of unpaired electron density in M-DNIC corresponds to the low-spin (S = 1/2) state with a d(7) electron configuration of the iron atom and predominant localization of the unpaired electron on MO(d(z2)) and the square planar structure of M-DNIC. On the other side, the formation of molecular orbitals of M-DNIC including orbitals of the iron atom, thiolate and nitrosyl ligands results in a transfer of electron density from sulfur atoms to the iron atom and nitrosyl ligands. Under these conditions, the positive charge on the nitrosyl ligands diminishes appreciably, the interaction of the ligands with hydroxyl ions or with thiols slows down and the hydrolysis of nitrosyl ligands and the S-nitrosating effect of the latter are not manifested. Most probably, the S-nitrosating effect of nitrosyl ligands is a result of weak binding of thiolate ligands to the iron atom under conditions favoring destabilization of M-DNIC.

Deep Learning of Atomically Resolved Scanning Transmission Electron Microscopy Images: Chemical Identification and Tracking Local Transformations

DOE PAGES

Ziatdinov, Maxim; Dyck, Ondrej; Maksov, Artem; ...

2017-12-07

Recent advances in scanning transmission electron and scanning probe microscopies have opened unprecedented opportunities in probing the materials structural parameters and various functional properties in real space with an angstrom-level precision. This progress has been accompanied by exponential increase in the size and quality of datasets produced by microscopic and spectroscopic experimental techniques. These developments necessitate adequate methods for extracting relevant physical and chemical information from the large datasets, for which a priori information on the structures of various atomic configurations and lattice defects is limited or absent. Here we demonstrate an application of deep neural networks to extracting informationmore » from atomically resolved images including location of the atomic species and type of defects. We develop a “weakly-supervised” approach that uses information on the coordinates of all atomic species in the image, extracted via a deep neural network, to identify a rich variety of defects that are not part of an initial training set. We further apply our approach to interpret complex atomic and defect transformation, including switching between different coordination of silicon dopants in graphene as a function of time, formation of peculiar silicon dimer with mixed 3-fold and 4-fold coordination, and the motion of molecular “rotor”. In conclusion, this deep learning based approach resembles logic of a human operator, but can be scaled leading to significant shift in the way of extracting and analyzing information from raw experimental data.« less

Collision of impurities with Bose–Einstein condensates

NASA Astrophysics Data System (ADS)

Lingua, F.; Lepori, L.; Minardi, F.; Penna, V.; Salasnich, L.

2018-04-01

Quantum dynamics of impurities in a bath of bosons is a long-standing problem in solid-state, plasma, and atomic physics. Recent experimental and theoretical investigations with ultracold atoms have focused on this problem, studying atomic impurities immersed in an atomic Bose–Einstein condensate (BEC) and for various relative coupling strengths tuned by the Fano‑Feshbach resonance technique. Here, we report extensive numerical simulations on a closely related problem: the collision between a bosonic impurity consisting of a few 41K atoms and a BEC of 87Rb atoms in a quasi one-dimensional configuration and under a weak harmonic axial confinement. For small values of the inter-species interaction strength (regardless of its sign), we find that the impurity, which starts from outside the BEC, simply causes the BEC cloud to oscillate back and forth, but the frequency of oscillation depends on the interaction strength. For intermediate couplings, after a few cycles of oscillation the impurity is captured by the BEC, and strongly changes its amplitude of oscillation. In the strong interaction regime, if the inter-species interaction is attractive, a local maximum (bright soliton) in the BEC density occurs where the impurity is trapped; if, instead, the inter-species interaction is repulsive, the impurity is not able to enter the BEC cloud and the reflection coefficient is close to one. However, if the initial displacement of the impurity is increased, the impurity is able to penetrate the cloud, leading to the appearance of a moving hole (dark soliton) in the BEC.

Deep Learning of Atomically Resolved Scanning Transmission Electron Microscopy Images: Chemical Identification and Tracking Local Transformations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ziatdinov, Maxim; Dyck, Ondrej; Maksov, Artem

Recent advances in scanning transmission electron and scanning probe microscopies have opened unprecedented opportunities in probing the materials structural parameters and various functional properties in real space with an angstrom-level precision. This progress has been accompanied by exponential increase in the size and quality of datasets produced by microscopic and spectroscopic experimental techniques. These developments necessitate adequate methods for extracting relevant physical and chemical information from the large datasets, for which a priori information on the structures of various atomic configurations and lattice defects is limited or absent. Here we demonstrate an application of deep neural networks to extracting informationmore » from atomically resolved images including location of the atomic species and type of defects. We develop a “weakly-supervised” approach that uses information on the coordinates of all atomic species in the image, extracted via a deep neural network, to identify a rich variety of defects that are not part of an initial training set. We further apply our approach to interpret complex atomic and defect transformation, including switching between different coordination of silicon dopants in graphene as a function of time, formation of peculiar silicon dimer with mixed 3-fold and 4-fold coordination, and the motion of molecular “rotor”. In conclusion, this deep learning based approach resembles logic of a human operator, but can be scaled leading to significant shift in the way of extracting and analyzing information from raw experimental data.« less

Deep Learning of Atomically Resolved Scanning Transmission Electron Microscopy Images: Chemical Identification and Tracking Local Transformations.

PubMed

Ziatdinov, Maxim; Dyck, Ondrej; Maksov, Artem; Li, Xufan; Sang, Xiahan; Xiao, Kai; Unocic, Raymond R; Vasudevan, Rama; Jesse, Stephen; Kalinin, Sergei V

2017-12-26

Recent advances in scanning transmission electron and scanning probe microscopies have opened exciting opportunities in probing the materials structural parameters and various functional properties in real space with angstrom-level precision. This progress has been accompanied by an exponential increase in the size and quality of data sets produced by microscopic and spectroscopic experimental techniques. These developments necessitate adequate methods for extracting relevant physical and chemical information from the large data sets, for which a priori information on the structures of various atomic configurations and lattice defects is limited or absent. Here we demonstrate an application of deep neural networks to extract information from atomically resolved images including location of the atomic species and type of defects. We develop a "weakly supervised" approach that uses information on the coordinates of all atomic species in the image, extracted via a deep neural network, to identify a rich variety of defects that are not part of an initial training set. We further apply our approach to interpret complex atomic and defect transformation, including switching between different coordination of silicon dopants in graphene as a function of time, formation of peculiar silicon dimer with mixed 3-fold and 4-fold coordination, and the motion of molecular "rotor". This deep learning-based approach resembles logic of a human operator, but can be scaled leading to significant shift in the way of extracting and analyzing information from raw experimental data.

Al atom on MoO3(010) surface: adsorption and penetration using density functional theory.

PubMed

Wu, Hong-Zhang; Bandaru, Sateesh; Wang, Da; Liu, Jin; Lau, Woon Ming; Wang, Zhenling; Li, Li-Li

2016-03-14

Interfacial issues, such as the interfacial structure and the interdiffusion of atoms at the interface, are fundamental to the understanding of the ignition and reaction mechanisms of nanothermites. This study employs first-principle density functional theory to model Al/MoO3 by placing an Al adatom onto a unit cell of a MoO3(010) slab, and to probe the initiation of interfacial interactions of Al/MoO3 nanothermite by tracking the adsorption and subsurface-penetration of the Al adatom. The calculations show that the Al adatom can spontaneously go through the topmost atomic plane (TAP) of MoO3(010) and reach the 4-fold hollow adsorption-site located below the TAP, with this subsurface adsorption configuration being the most preferred one among all plausible adsorption configurations. Two other plausible configurations place the Al adatom at two bridge sites located above the TAP of MoO3(010) but the Al adatom can easily penetrate below this TAP to a relatively more stable adsorption configuration, with a small energy barrier of merely 0.2 eV. The evidence of subsurface penetration of Al implies that Al/MoO3 likely has an interface with intermixing of Al, Mo and O atoms. These results provide new insights on the interfacial interactions of Al/MoO3 and the ignition/combustion mechanisms of Al/MoO3 nanothermites.

Effects of configurational disorder on the elastic properties of icosahedral boron-rich alloys based on B6O, B13C2, and B4C, and their mixing thermodynamics

NASA Astrophysics Data System (ADS)

Ektarawong, A.; Simak, S. I.; Hultman, L.; Birch, J.; Tasnádi, F.; Wang, F.; Alling, B.

2016-04-01

The elastic properties of alloys between boron suboxide (B6O) and boron carbide (B13C2), denoted by (B6O)1-x(B13C2)x, as well as boron carbide with variable carbon content, ranging from B13C2 to B4C are calculated from first-principles. Furthermore, the mixing thermodynamics of (B6O)1-x(B13C2)x is studied. A superatom-special quasirandom structure approach is used for modeling different atomic configurations, in which effects of configurational disorder between the carbide and suboxide structural units, as well as between boron and carbon atoms within the units, are taken into account. Elastic properties calculations demonstrate that configurational disorder in B13C2, where a part of the C atoms in the CBC chains substitute for B atoms in the B12 icosahedra, drastically increase the Young's and shear modulus, as compared to an atomically ordered state, B12(CBC). These calculated elastic moduli of the disordered state are in excellent agreement with experiments. Configurational disorder between boron and carbon can also explain the experimentally observed almost constant elastic moduli of boron carbide as the carbon content is changed from B4C to B13C2. The elastic moduli of the (B6O)1-x(B13C2)x system are also practically unchanged with composition if boron-carbon disorder is taken into account. By investigating the mixing thermodynamics of the alloys, in which the Gibbs free energy is determined within the mean-field approximation for the configurational entropy, we outline the pseudo-binary phase diagram of (B6O)1-x(B13C2)x. The phase diagram reveals the existence of a miscibility gap at all temperatures up to the melting point. Also, the coexistence of B6O-rich as well as ordered or disordered B13C2-rich domains in the material prepared through equilibrium routes is predicted.

The fate of H atom adducts to 3'-uridine monophosphate.

PubMed

Wang, Ran; Zhang, Ru Bo; Eriksson, Leif A

2010-07-29

The stabilities of the adducts deriving from H free radical addition to the O2, O4, and C5 positions of 3'-uridine monophosphate (3'UMP) are studied by the hybrid density functional B3LYP approach. Upon H atom addition at the O2 position, a concerted low-barrier proton-transfer process will initially occur, followed by the potential ruptures of the N-glycosidic or beta-phosphate bonds. The rupture barriers are strongly influenced by the rotational configuration of the phosphate group at the 3' terminal, and are influenced by bulk solvation effects. The O4-H adduct has the highest thermal stability, as the localization of the unpaired electron does not enable cleavage of either the C1'-N1 or the C3'-O(P) bonds. For the most stable adduct, with H atom added to the C5 position, the rate-controlled step is the H2'a abstraction by the C6 radical site, after which the subsequent strand rupture reactions proceed with low barriers. The main unpaired electron densities are presented for the transient species. Combined with previous results, it is concluded that the H atom adducts are more facile to drive the strand scission rather than N-glycosidic bond ruptures within the nucleic acid bases.

Adsorbate-induced reconstruction in the phase 1 × 2-3H/Rh(110)

NASA Astrophysics Data System (ADS)

Michl, M.; Nichtl-Pecher, W.; Oed, W.; Landskron, H.; Heinz, K.; Müller, K.

1989-10-01

The 1 × 2-3H superstructure of hydrogen on Rh(110) at coverage θ = {3}/{2} is analysed by low energy electron diffraction at 90 K. The spectra of eight beams are recorded with a computer-controlled TV measurement technique which yields low noise data even for weak superstructure spots by multiple averaging. Comparison to full dynamical calculations shows that a kinematic treatment of the hydrogen layer diffraction coupled to the full dynamical diffraction of the substrate is a very good approximation. Spectra computed in this way are compared with experimental data by R-factor evaluation. The three non-equivalent hydrogen atoms are found to adsorb in quasi-three-fold coordinated adsorption sites with slightly different local configurations and with H-Rh bond lengths between 1.87 and 1.93 Å to the first-layer rhodium atoms. Interaction between the adatoms seems to weaken the bonding to the adjacent atom in the second layer, so that H-Rh bond lengths larger than 2.17 Å result. A slight reconstruction of the substrate is necessary to bring superstructure spot intensities near the experimentally observed level. Rhodium atoms bonded to two hydrogen atoms are moved out of the surface by 0.03 ± 0.02 Å relative to Rh atoms bonded to only a single H atom. The relaxation of the first Rh layer spacing is determined to be {d 12}/{d 0} = -3.8 ± 1% and {d 22}/{d 0} = 0 ± 1% . The best fit Pendry R-factor is 0.33.

Sensitivity function analysis of gravitational wave detection with single-laser and large-momentum-transfer atomic sensors

NASA Astrophysics Data System (ADS)

Tang, Biao; Zhang, Bao-Cheng; Zhou, Lin; Wang, Jin; Zhan, Ming-Sheng

2015-03-01

Recently, a configuration using atomic interferometers (AIs) had been suggested for the detection of gravitational waves. A new AI with some additional laser pulses for implementing large momentum transfer was also put forward, in order to reduce the effect of shot noise and laser frequency noise. We use a sensitivity function to analyze all possible configurations of the new AI and to distinguish how many momenta are transferred in a specific configuration. By analyzing the new configuration, we further explore a detection scheme for gravitational waves, in particular, that ameliorates laser frequency noise. We find that the amelioration occurs in such a scheme, but novelly, in some cases, the frequency noise can be canceled completely by using a proper data processing method. Supported by the National Natural Science Foundation of China.

Three-dimensional atom localization via electromagnetically induced transparency in a three-level atomic system.

PubMed

Wang, Zhiping; Cao, Dewei; Yu, Benli

2016-05-01

We present a new scheme for three-dimensional (3D) atom localization in a three-level atomic system via measuring the absorption of a weak probe field. Owing to the space-dependent atom-field interaction, the position probability distribution of the atom can be directly determined by measuring the probe absorption. It is found that, by properly varying the parameters of the system, the probability of finding the atom in 3D space can be almost 100%. Our scheme opens a promising way to achieve high-precision and high-efficiency 3D atom localization, which provides some potential applications in laser cooling or atom nano-lithography via atom localization.

Spectral neighbor analysis method for automated generation of quantum-accurate interatomic potentials

NASA Astrophysics Data System (ADS)

Thompson, A. P.; Swiler, L. P.; Trott, C. R.; Foiles, S. M.; Tucker, G. J.

2015-03-01

We present a new interatomic potential for solids and liquids called Spectral Neighbor Analysis Potential (SNAP). The SNAP potential has a very general form and uses machine-learning techniques to reproduce the energies, forces, and stress tensors of a large set of small configurations of atoms, which are obtained using high-accuracy quantum electronic structure (QM) calculations. The local environment of each atom is characterized by a set of bispectrum components of the local neighbor density projected onto a basis of hyperspherical harmonics in four dimensions. The bispectrum components are the same bond-orientational order parameters employed by the GAP potential [1]. The SNAP potential, unlike GAP, assumes a linear relationship between atom energy and bispectrum components. The linear SNAP coefficients are determined using weighted least-squares linear regression against the full QM training set. This allows the SNAP potential to be fit in a robust, automated manner to large QM data sets using many bispectrum components. The calculation of the bispectrum components and the SNAP potential are implemented in the LAMMPS parallel molecular dynamics code. We demonstrate that a previously unnoticed symmetry property can be exploited to reduce the computational cost of the force calculations by more than one order of magnitude. We present results for a SNAP potential for tantalum, showing that it accurately reproduces a range of commonly calculated properties of both the crystalline solid and the liquid phases. In addition, unlike simpler existing potentials, SNAP correctly predicts the energy barrier for screw dislocation migration in BCC tantalum.

Structural stability and electronic properties of β-tetragonal boron: A first-principles study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hayami, Wataru, E-mail: hayami.wataru@nims.go.jp

2015-01-15

It is known that elemental boron has five polymorphs: α- and β-rhombohedral, α- and β-tetragonal, and the high-pressure γ phase. β-tetragonal (β-t) boron was first discovered in 1960, but there have been only a few studies since then. We have thoroughly investigated, using first-principles calculations, the atomic and electronic structures of β-t boron, the details of which were not known previously. The difficulty of calculation arises from the fact that β-t boron has a large unit cell that contains between 184 and 196 atoms, with 12 partially-occupied interstitial sites. This makes the number of configurations of interstitial atoms too greatmore » to calculate them all. By introducing assumptions based on symmetry and preliminary calculations, the number of configurations to calculate can be greatly reduced. It was eventually found that β-t boron has the lowest total energy, with 192 atoms (8 interstitial atoms) in an orthorhombic lattice. The total energy per atom was between those of α- and β-rhombohedral boron. Another tetragonal structure with 192 atoms was found to have a very close energy. The valence bands were fully filled and the gaps were about 1.16 to 1.54 eV, making it comparable to that of β-rhombohedral boron. - Graphical abstract: Electronic density distribution for the lowest-energy configuration (N=192) viewed from the 〈1 0 0〉 direction. Left: isosurface (yellow) at d=0.09 electrons/a.u.{sup 3} Right: isosurface (orange) at d=0.12 electrons/a.u.{sup 3}. - Highlights: • β-tetragonal boron was thoroughly investigated using first-principles calculations. • The lowest energy structure contains 192 atoms in an orthorhombic lattice. • Another tetragonal structure with 192 atoms has a very close energy. • The total energy per atom is between those of α- and β-rhombohedral boron. • The band gap of the lowest energy structure is about 1.16 to 1.54 eV.« less

Bloch equation and atom-field entanglement scenario in three-level systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sen, Surajit; Nath, Mihir Ranjan; Dey, Tushar Kanti

2011-09-23

We study the exact solution of the lambda, vee and cascade type of three-level system with distinct Hamiltonian for each configuration expressed in the SU(3) basis. The semiclassical models are solved by solving respective Bloch equation and the existence of distinct non-linear constants are discussed which are different for different configuration. Apart from proposing a qutrit wave function, the atom-field entanglement is studied for the quantized three-level systems using the Phoenix-Knight formalism and corresponding population inversion are compared.

Configuration interaction in charge exchange spectra of tin and xenon

NASA Astrophysics Data System (ADS)

D'Arcy, R.; Morris, O.; Ohashi, H.; Suda, S.; Tanuma, H.; Fujioka, S.; Nishimura, H.; Nishihara, K.; Suzuki, C.; Kato, T.; Koike, F.; O'Sullivan, G.

2011-06-01

Charge-state-specific extreme ultraviolet spectra from both tin ions and xenon ions have been recorded at Tokyo Metropolitan University. The electron cyclotron resonance source spectra were produced from charge exchange collisions between the ions and rare gas target atoms. To identify unknown spectral lines of tin and xenon, atomic structure calculations were performed for Sn14+-Sn17+ and Xe16+-Xe20+ using the Hartree-Fock configuration interaction code of Cowan (1981 The Theory of Atomic Structure and Spectra (Berkeley, CA: University of California Press)). The energies of the capture states involved in the single-electron process that occurs in these slow collisions were estimated using the classical over-barrier model.

The interaction of mercury with halogenated graphene

NASA Astrophysics Data System (ADS)

Kirchofer, Abigail; Sasmaz, Erdem; Wilcox, Jennifer

2011-03-01

The interaction of mercury with halogenated graphene was studied using plane-wave density functional theory. Various configurations of H, Hg, O and Br or Cl on the zigzag edge sites of graphene were investigated. Although Hg-Br (or -Cl) complexes were found to be stable on the surface, the most stable configurations found were those with Hg adjacent to O. The surface atoms Hg, O, and Br tend to repel each other during geometric optimization, moving towards an H atom nearest-neighbor where possible. The strength of the Hg-graphene interaction is very sensitive to the local environment. The Hg-graphene binding energy is strongest when the Hg is located next to a surface O but not immediately next to a bound Br. DOS analysis revealed that Hg adsorption involves a gain in Hg 6 p-states and a loss in Hg 5 s electron density, resulting in an oxidized surface-bound Hg complex. DOS analysis suggests that Br strengthens the Hg-graphene interaction by modifying the surface carbon electron density; however, when Br is adjacent to Hg, a direct Hg-Br interaction weakens the Hg-C bond. These investigations provide insight into the mechanism associated with enhanced Hg adsorption on Br-functionalized carbon materials for Hg emissions reductions from coal-fired power plant applications. The authors acknowledge the financial support by Electric Power Research Institute (EPRI).

Resonance fluorescence based two- and three-dimensional atom localization

NASA Astrophysics Data System (ADS)

Wahab, Abdul; Rahmatullah; Qamar, Sajid

2016-06-01

Two- and three-dimensional atom localization in a two-level atom-field system via resonance fluorescence is suggested. For the two-dimensional localization, the atom interacts with two orthogonal standing-wave fields, whereas for the three-dimensional atom localization, the atom interacts with three orthogonal standing-wave fields. The effect of the detuning and phase shifts associated with the corresponding standing-wave fields is investigated. A precision enhancement in position measurement of the single atom can be noticed via the control of the detuning and phase shifts.

Electron spin relaxation governed by Raman processes both for Cu2+ ions and carbonate radicals in KHCO3 crystals: EPR and electron spin echo studies

NASA Astrophysics Data System (ADS)

Hoffmann, Stanislaw K.; Goslar, Janina; Lijewski, Stefan

2012-08-01

EPR studies of Cu2+ and two free radicals formed by γ-radiation were performed for KHCO3 single crystal at room temperature. From the rotational EPR results we concluded that Cu2+ is chelated by two carbonate molecules in a square planar configuration with spin-Hamiltonian parameters g|| = 2.2349 and A|| = 18.2 mT. Free radicals were identified as neutral HOCOrad with unpaired electron localized on the carbon atom and a radical anion CO3·- with unpaired electron localized on two oxygen atoms. The hyperfine splitting of the EPR lines by an interaction with a single hydrogen atom of HOCOrad was observed with isotropic coupling constants ao = 0.31 mT. Two differently oriented radical sites were identified in the crystal unit cell. Electron spin-lattice relaxation measured by electron spin echo methods shows that both Cu2+ and free radicals relax via two-phonon Raman processes with almost the same relaxation rate. The temperature dependence of the relaxation rate 1/T1 is well described with the effective Debye temperature ΘD = 175 K obtained from a fit to the Debye-type phonon spectrum. We calculated a more realistic Debye temperature value from available elastic constant values of the crystal as ΘD = 246 K. This ΘD-value and the Debye phonon spectrum approximation give a much worse fit to the experimental results. Possible contributions from a local mode or an optical mode are considered and it is suggested that the real phonon spectrum should be used for the relaxation data interpretation. It is unusual that free radicals in KHCO3 relax similarly to the well localized Cu2+ ions, which suggests a small destruction of the host crystal lattice by the ionizing irradiation allowing well coupling between radical and lattice dynamics.

Thermal nanostructure: An order parameter multiscale ensemble approach

NASA Astrophysics Data System (ADS)

Cheluvaraja, S.; Ortoleva, P.

2010-02-01

Deductive all-atom multiscale techniques imply that many nanosystems can be understood in terms of the slow dynamics of order parameters that coevolve with the quasiequilibrium probability density for rapidly fluctuating atomic configurations. The result of this multiscale analysis is a set of stochastic equations for the order parameters whose dynamics is driven by thermal-average forces. We present an efficient algorithm for sampling atomistic configurations in viruses and other supramillion atom nanosystems. This algorithm allows for sampling of a wide range of configurations without creating an excess of high-energy, improbable ones. It is implemented and used to calculate thermal-average forces. These forces are then used to search the free-energy landscape of a nanosystem for deep minima. The methodology is applied to thermal structures of Cowpea chlorotic mottle virus capsid. The method has wide applicability to other nanosystems whose properties are described by the CHARMM or other interatomic force field. Our implementation, denoted SIMNANOWORLD™, achieves calibration-free nanosystem modeling. Essential atomic-scale detail is preserved via a quasiequilibrium probability density while overall character is provided via predicted values of order parameters. Applications from virology to the computer-aided design of nanocapsules for delivery of therapeutic agents and of vaccines for nonenveloped viruses are envisioned.

Coherent population trapping with polarization modulation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yun, Peter, E-mail: enxue.yun@obspm.fr; Guérandel, Stéphane; Clercq, Emeric de

Coherent population trapping (CPT) is extensively studied for future vapor cell clocks of high frequency stability. In the constructive polarization modulation CPT scheme, a bichromatic laser field with polarization and phase synchronously modulated is applied on an atomic medium. A high contrast CPT signal is observed in this so-called double-modulation configuration, due to the fact that the atomic population does not leak to the extreme Zeeman states, and that the two CPT dark states, which are produced successively by the alternate polarizations, add constructively. Here, we experimentally investigate CPT signal dynamics first in the usual configuration, a single circular polarization.more » The double-modulation scheme is then addressed in both cases: one pulse Rabi interaction and two pulses Ramsey interaction. The impact and the optimization of the experimental parameters involved in the time sequence are reviewed. We show that a simple seven-level model explains the experimental observations. The double-modulation scheme yields a high contrast similar to the one of other high contrast configurations like push-pull optical pumping or crossed linear polarization scheme, with a setup allowing a higher compactness. The constructive polarization modulation is attractive for atomic clock, atomic magnetometer, and high precision spectroscopy applications.« less

Polarization effects in the interaction between multi-level atoms and two optical fields

NASA Astrophysics Data System (ADS)

Colín-Rodríguez, R.; Flores-Mijangos, J.; Hernández-Gómez, S.; Jáuregui, R.; López-Hernández, O.; Mojica-Casique, C.; Ponciano-Ojeda, F.; Ramírez-Martínez, F.; Sahagún, D.; Volke-Sepúlveda, K.; Jiménez-Mier, J.

2015-06-01

Polarized velocity selective spectra for rubidium atoms in a room temperature cell are presented. The experiments were performed in the lambda configuration (D2 manifold) and in the 5s\\to 5{{p}3/2}\\to 5{{d}j} ladder configuration. For the lambda configuration the effect of the probe beam intensity in the absorption and polarization spectra are compared with results of a rate equation approximation. Good overall agreement between experiment and theory is found. The results indicate different saturation rates for each of the atomic transitions. Distinctive polarization signals with hyperfine-resolved components are found for the ladder 5{{d}3/2} and 5{{d}5/2} upper states. Fluorescence detection of the 420 nm that results from the second step in the cascade decay 5{{d}j}\\to 6{{p}{{j\\prime }}}\\to 5s was used in the ladder experiments. This fluorescence was also used for the detection of the 5{{p}3/2}\\to 6{{p}3/2} electric dipole forbidden transition in atomic rubidium that occurs at 911 nm. The 6{{p}3/2} hyperfine structure was resolved in this continuous wave, non-dipole excitation.

Primary radiation damage of Zr-0.5%Nb binary alloy: atomistic simulation by molecular dynamics method

NASA Astrophysics Data System (ADS)

Tikhonchev, M.; Svetukhin, V.; Kapustin, P.

2017-09-01

Ab initio calculations predict high positive binding energy (˜1 eV) between niobium atoms and self-interstitial configurations in hcp zirconium. It allows the expectation of increased niobium fraction in self-interstitials formed under neutron irradiation in atomic displacement cascades. In this paper, we report the results of molecular dynamics simulation of atomic displacement cascades in Zr-0.5%Nb binary alloy and pure Zr at the temperature of 300 K. Two sets of n-body interatomic potentials have been used for the Zr-Nb system. We consider a cascade energy range of 2-20 keV. Calculations show close estimations of the average number of produced Frenkel pairs in the alloy and pure Zr. A high fraction of Nb is observed in the self-interstitial configurations. Nb is mainly detected in single self-interstitial configurations, where its fraction reaches tens of percent, i.e. more than its tenfold concentration in the matrix. The basic mechanism of this phenomenon is the trapping of mobile self-interstitial configurations by niobium. The diffusion of pure zirconium and mixed zirconium-niobium self-interstitial configurations in the zirconium matrix at 300 K has been simulated. We observe a strong dependence of the estimated diffusion coefficients and fractions of Nb in self-interstitials produced in displacement cascades on the potential.

Synthesis and evaluation of the inhibitory activity of the four stereoisomers of the potent and selective human γ-glutamyl transpeptidase inhibitor GGsTop.

PubMed

Watanabe, Bunta; Tabuchi, Yukiko; Wada, Kei; Hiratake, Jun

2017-11-01

2-Amino-4-{[3-(carboxymethyl)phenoxy](methoxy)phosphoryl}butanoic acid (GGsTop) is a potent, highly selective, nontoxic, and irreversible inhibitor of γ-glutamyl transpeptidase (GGT). GGsTop has been widely used in academic and medicinal research, and also as an active ingredient (Nahlsgen) in commercial anti-aging cosmetics. GGsTop consists of four stereoisomers due to the presence of two stereogenic centers, i.e., the α-carbon atom of the glutamate mimic (l/d) and the phosphorus atom (R P /S P ). In this study, each stereoisomer of GGsTop was synthesized stereoselectively and their inhibitory activity against human GGT was evaluated. The l- and d-configurations of each stereoisomer were determined by a combination of a chiral pool synthesis and chiral HPLC analysis. The synthesis of the four stereoisomers of GGsTop used chiral synthetic precursors that were separated by chiral HPLC on a preparative scale. With respect to the configuration of the α-carbon atom of the glutamate mimic, the l-isomer (k on =174M -1 s -1 ) was ca. 8-fold more potent than the d-isomer (k on =21.5M -1 s -1 ). In contrast, the configuration of the phosphorus atom is critical for GGT inhibitory activity. Based on a molecular modeling approach, the absolute configuration of the phosphorus atom of the active GGsTop isomers was postulated to be S P . The S P -isomers inhibited human GGT (k on =21.5-174M -1 s -1 ), while the R P -isomers were inactive even at concentrations of 0.1mM. Copyright © 2017 Elsevier Ltd. All rights reserved.

Effects of correlated hybridization in the single-impurity Anderson model

NASA Astrophysics Data System (ADS)

Líbero, Valter; Veiga, Rodrigo

2013-03-01

The development of new materials often dependents on the theoretical foundations which study the microscopic matter, i.e., the way atoms interact and create distinct configurations. Among the interesting materials, those with partially filled d or f orbitals immersed in nonmagnetic metals have been described by the Anderson model, which takes into account Coulomb correlation (U) when a local level (energy Ed) is doubled occupied, and an electronic hybridization between local levels and conduction band states. In addition, here we include a correlated hybridization term, which depends on the local-level occupation number involved. This term breaks particle-hole symmetry (even when U + 2Ed = 0), enhances charge fluctuations on local levels and as a consequence strongly modifies the crossover between the Hamiltonian fixed-points, even suppressing one or other. We exemplify these behaviors showing data obtained from the Numerical Renormalization Group (NRG) computation for the impurity temperature-dependent specific heat, entropy and magnetic susceptibility. The interleaving procedure is used to recover the continuum spectrum after the NRG-logarithmic discretization of the conduction band. Fundação de Amparo à Pesquisa do Estado de São Paulo - FAPESP.

A strategy to find minimal energy nanocluster structures.

PubMed

Rogan, José; Varas, Alejandro; Valdivia, Juan Alejandro; Kiwi, Miguel

2013-11-05

An unbiased strategy to search for the global and local minimal energy structures of free standing nanoclusters is presented. Our objectives are twofold: to find a diverse set of low lying local minima, as well as the global minimum. To do so, we use massively the fast inertial relaxation engine algorithm as an efficient local minimizer. This procedure turns out to be quite efficient to reach the global minimum, and also most of the local minima. We test the method with the Lennard-Jones (LJ) potential, for which an abundant literature does exist, and obtain novel results, which include a new local minimum for LJ13 , 10 new local minima for LJ14 , and thousands of new local minima for 15≤N≤65. Insights on how to choose the initial configurations, analyzing the effectiveness of the method in reaching low-energy structures, including the global minimum, are developed as a function of the number of atoms of the cluster. Also, a novel characterization of the potential energy surface, analyzing properties of the local minima basins, is provided. The procedure constitutes a promising tool to generate a diverse set of cluster conformations, both two- and three-dimensional, that can be used as an input for refinement by means of ab initio methods. Copyright © 2013 Wiley Periodicals, Inc.

The behavior of small helium clusters near free surfaces in tungsten

NASA Astrophysics Data System (ADS)

Barashev, A. V.; Xu, H.; Stoller, R. E.

2014-11-01

The results of a computational study of helium-vacancy clusters in tungsten are reported. A recently developed atomistic kinetic Monte Carlo method employing empirical interatomic potentials was used to investigate the behavior of clusters composed of three interstitial-helium atoms near {1 1 1}, {1 1 0} and {1 0 0} free surfaces. Multiple configurations were examined and the local energy landscape was characterized to determine cluster mobility and the potential for interactions with the surface. The clusters were found to be highly mobile if far from the surface, but were attracted and bound to the surface when within a distance of a few lattice parameters. When near the surface, the clusters were transformed into an immobile configuration due to the creation of a Frenkel pair; the vacancy was incorporated into what became a He3-vacancy complex. The corresponding interstitial migrated to and became an adatom on the free surface. This process can contribute to He retention, and may be responsible for the observed deterioration of the plasma-exposed tungsten surfaces.

New Advancements in the Study of the Uniform Electron Gas with Full Configuration Interaction Quantum Monte Carlo

NASA Astrophysics Data System (ADS)

Ruggeri, Michele; Luo, Hongjun; Alavi, Ali

Full Configuration Interaction Quantum Monte Carlo (FCIQMC) is able to give remarkably accurate results in the study of atoms and molecules. The study of the uniform electron gas (UEG) on the other hand has proven to be much harder, particularly in the low density regime. The source of this difficulty comes from the strong interparticle correlations that arise at low density, and essentially forbid the study of the electron gas in proximity of Wigner crystallization. We extend a previous study on the three dimensional electron gas computing the energy of a fully polarized gas for N=27 electrons at high and medium density (rS = 0 . 5 to 5 . 0). We show that even when dealing with a polarized UEG the computational cost of the study of systems with rS > 5 . 0 is prohibitive; in order to deal with correlations and to extend the density range that to be studied we introduce a basis of localized states and an effective transcorrelated Hamiltonian.

Can nonadditive dispersion forces explain chain formation of nanoparticles?

NASA Astrophysics Data System (ADS)

Kwaadgras, Bas W.; Verdult, Maarten W. J.; Dijkstra, Marjolein; van Roij, René

2013-03-01

We study to what extent dielectric nanoparticles prefer to self-assemble into linear chains or into more compact structures. To calculate the Van der Waals (VdW) attraction between the clusters we use the Coupled Dipole Method (CDM), which treats each atom in the nanoparticle as an inducible oscillating point dipole. The VdW attraction then results from the full many-body interactions between the dipoles. For non-capped nanoparticles, we calculate in which configuration the VdW attraction is maximal. We find that in virtually all cases we studied, many-body effects only result in local potential minima at the linear configuration, as opposed to global ones, and that these metastable minima are in most cases rather shallow compared to the thermal energy. In this work, we also compare the CDM results with those from Hamaker-de Boer and Axilrod-Teller theory to investigate the influence of the many-body effects and the accuracy of these two approximate methods.

Pt Single Atoms Embedded in the Surface of Ni Nanocrystals as Highly Active Catalysts for Selective Hydrogenation of Nitro Compounds.

PubMed

Peng, Yuhan; Geng, Zhigang; Zhao, Songtao; Wang, Liangbing; Li, Hongliang; Wang, Xu; Zheng, Xusheng; Zhu, Junfa; Li, Zhenyu; Si, Rui; Zeng, Jie

2018-06-13

Single-atom catalysts exhibit high selectivity in hydrogenation due to their isolated active sites, which ensure uniform adsorption configurations of substrate molecules. Compared with the achievement in catalytic selectivity, there is still a long way to go in exploiting the catalytic activity of single-atom catalysts. Herein, we developed highly active and selective catalysts in selective hydrogenation by embedding Pt single atoms in the surface of Ni nanocrystals (denoted as Pt 1 /Ni nanocrystals). During the hydrogenation of 3-nitrostyrene, the TOF numbers based on surface Pt atoms of Pt 1 /Ni nanocrystals reached ∼1800 h -1 under 3 atm of H 2 at 40 °C, much higher than that of Pt single atoms supported on active carbon, TiO 2 , SiO 2 , and ZSM-5. Mechanistic studies reveal that the remarkable activity of Pt 1 /Ni nanocrystals derived from sufficient hydrogen supply because of spontaneous dissociation of H 2 on both Pt and Ni atoms as well as facile diffusion of H atoms on Pt 1 /Ni nanocrystals. Moreover, the ensemble composed of the Pt single atom and nearby Ni atoms in Pt 1 /Ni nanocrystals leads to the adsorption configuration of 3-nitrostyrene favorable for the activation of nitro groups, accounting for the high selectivity for 3-vinylaniline.

Hydrogen atom kinetics in capacitively coupled plasmas

NASA Astrophysics Data System (ADS)

Nunomura, Shota; Katayama, Hirotaka; Yoshida, Isao

2017-05-01

Hydrogen (H) atom kinetics has been investigated in capacitively coupled very high frequency (VHF) discharges at powers of 16-780 mW cm-2 and H2 gas pressures of 0.1-2 Torr. The H atom density has been measured using vacuum ultra violet absorption spectroscopy (VUVAS) with a micro-discharge hollow cathode lamp as a VUV light source. The measurements have been performed in two different electrode configurations of discharges: conventional parallel-plate diode and triode with an intermediate mesh electrode. We find that in the triode configuration, the H atom density is strongly reduced across the mesh electrode. The H atom density varies from ˜1012 cm-3 to ˜1010 cm-3 by crossing the mesh with 0.2 mm in thickness and 36% in aperture ratio. The fluid model simulations for VHF discharge plasmas have been performed to study the H atom generation, diffusion and recombination kinetics. The simulations suggest that H atoms are generated in the bulk plasma, by the electron impact dissociation (e + H2 \\to e + 2H) and the ion-molecule reaction (H2 + + H2 \\to {{{H}}}3+ + H). The diffusion of H atoms is strongly limited by a mesh electrode, and thus the mesh geometry influences the spatial distribution of the H atoms. The loss of H atoms is dominated by the surface recombination.

An atomistic fingerprint algorithm for learning ab initio molecular force fields

NASA Astrophysics Data System (ADS)

Tang, Yu-Hang; Zhang, Dongkun; Karniadakis, George Em

2018-01-01

Molecular fingerprints, i.e., feature vectors describing atomistic neighborhood configurations, is an important abstraction and a key ingredient for data-driven modeling of potential energy surface and interatomic force. In this paper, we present the density-encoded canonically aligned fingerprint algorithm, which is robust and efficient, for fitting per-atom scalar and vector quantities. The fingerprint is essentially a continuous density field formed through the superimposition of smoothing kernels centered on the atoms. Rotational invariance of the fingerprint is achieved by aligning, for each fingerprint instance, the neighboring atoms onto a local canonical coordinate frame computed from a kernel minisum optimization procedure. We show that this approach is superior over principal components analysis-based methods especially when the atomistic neighborhood is sparse and/or contains symmetry. We propose that the "distance" between the density fields be measured using a volume integral of their pointwise difference. This can be efficiently computed using optimal quadrature rules, which only require discrete sampling at a small number of grid points. We also experiment on the choice of weight functions for constructing the density fields and characterize their performance for fitting interatomic potentials. The applicability of the fingerprint is demonstrated through a set of benchmark problems.

A canonical stability-elasticity relationship verified for one million face-centred-cubic structures.

PubMed

Maisel, Sascha B; Höfler, Michaela; Müller, Stefan

2012-11-29

Any thermodynamically stable or metastable phase corresponds to a local minimum of a potentially very complicated energy landscape. But however complex the crystal might be, this energy landscape is of parabolic shape near its minima. Roughly speaking, the depth of this energy well with respect to some reference level determines the thermodynamic stability of the system, and the steepness of the parabola near its minimum determines the system's elastic properties. Although changing alloying elements and their concentrations in a given material to enhance certain properties dates back to the Bronze Age, the systematic search for desirable properties in metastable atomic configurations at a fixed stoichiometry is a very recent tool in materials design. Here we demonstrate, using first-principles studies of four binary alloy systems, that the elastic properties of face-centred-cubic intermetallic compounds obey certain rules. We reach two conclusions based on calculations on a huge subset of the face-centred-cubic configuration space. First, the stiffness and the heat of formation are negatively correlated with a nearly constant Spearman correlation for all concentrations. Second, the averaged stiffness of metastable configurations at a fixed concentration decays linearly with their distance to the ground-state line (the phase diagram of an alloy at zero Kelvin). We hope that our methods will help to simplify the quest for new materials with optimal properties from the vast configuration space available.

High performance current and spin diode of atomic carbon chain between transversely symmetric ribbon electrodes.

PubMed

Dong, Yao-Jun; Wang, Xue-Feng; Yang, Shuo-Wang; Wu, Xue-Mei

2014-08-21

We demonstrate that giant current and high spin rectification ratios can be achieved in atomic carbon chain devices connected between two symmetric ferromagnetic zigzag-graphene-nanoribbon electrodes. The spin dependent transport simulation is carried out by density functional theory combined with the non-equilibrium Green's function method. It is found that the transverse symmetries of the electronic wave functions in the nanoribbons and the carbon chain are critical to the spin transport modes. In the parallel magnetization configuration of two electrodes, pure spin current is observed in both linear and nonlinear regions. However, in the antiparallel configuration, the spin-up (down) current is prohibited under the positive (negative) voltage bias, which results in a spin rectification ratio of order 10(4). When edge carbon atoms are substituted with boron atoms to suppress the edge magnetization in one of the electrodes, we obtain a diode with current rectification ratio over 10(6).

High performance current and spin diode of atomic carbon chain between transversely symmetric ribbon electrodes

PubMed Central

Dong, Yao-Jun; Wang, Xue-Feng; Yang, Shuo-Wang; Wu, Xue-Mei

2014-01-01

We demonstrate that giant current and high spin rectification ratios can be achieved in atomic carbon chain devices connected between two symmetric ferromagnetic zigzag-graphene-nanoribbon electrodes. The spin dependent transport simulation is carried out by density functional theory combined with the non-equilibrium Green's function method. It is found that the transverse symmetries of the electronic wave functions in the nanoribbons and the carbon chain are critical to the spin transport modes. In the parallel magnetization configuration of two electrodes, pure spin current is observed in both linear and nonlinear regions. However, in the antiparallel configuration, the spin-up (down) current is prohibited under the positive (negative) voltage bias, which results in a spin rectification ratio of order 104. When edge carbon atoms are substituted with boron atoms to suppress the edge magnetization in one of the electrodes, we obtain a diode with current rectification ratio over 106. PMID:25142376

Atomic oxygen degradation of Intelsat 4-type solar array interconnects: Laboratory investigations

NASA Technical Reports Server (NTRS)

Koontz, S. L.; Cross, J. B.; Hoffbauer, M. A.; Kirkendahl, T. D.

1991-01-01

A Hughes 506 type communication satellite belonging to the Intelsat organization was marooned in low Earth orbit on March 14, 1990, following failure of the Titan third stage to separate properly. The satellite, Intelsat VI, was designed for service in geosynchronous orbit and contains several material configurations which are susceptible to attack by atomic oxygen. Analysis showed the silver foil interconnects in the satellite photovoltaic array to be the key materials issue because the silver is exposed directly to the atomic oxygen ram flux. The results are reported of atomic oxygen degradation testing of Intelsat VI type silver foil interconnects both as virgin material and in a configured solar cell element. Test results indicate that more than 80 pct. of the original thickness of silver in the Intelsat VI solar array interconnects should remain after completion of the proposed Space Shuttle rescue and/or reboost mission.

MgCu metallic glass

NASA Astrophysics Data System (ADS)

Durandurdu, Murat

2018-03-01

We generate an amorphous MgCu model using the rapid solidification of the melt through a first-principles molecular dynamics approach within a generalised gradient approximation and reveal, for the first time, its structural features and mechanical properties in details. The liquid and glassy MgCu are found to acquire slightly distinct local structures. Yet in both forms of MgCu, most Cu atoms have a tendency to form the ideal and defective icosahedrons while Mg atoms are arranged in complex configurations. The mean coordination number of Cu and Mg at 300 K is 11.31 and 13.73, respectively. The short-range order of MgCu glass is projected to be different than the known crystalline MgCu and Mg2Cu phases. The mechanical properties of MgCu glass and the CsCl-type MgCu crystal are computed and compared. On the basis of the enthalpy analyses, a possible pressure-induced crystallisation of the MgCu glass into a CsCl-type structure is proposed to occur at around 11 GPa.

Absorption and folding of melittin onto lipid bilayer membranes via unbiased atomic detail microsecond molecular dynamics simulation.

PubMed

Chen, Charles H; Wiedman, Gregory; Khan, Ayesha; Ulmschneider, Martin B

2014-09-01

Unbiased molecular simulation is a powerful tool to study the atomic details driving functional structural changes or folding pathways of highly fluid systems, which present great challenges experimentally. Here we apply unbiased long-timescale molecular dynamics simulation to study the ab initio folding and partitioning of melittin, a template amphiphilic membrane active peptide. The simulations reveal that the peptide binds strongly to the lipid bilayer in an unstructured configuration. Interfacial folding results in a localized bilayer deformation. Akin to purely hydrophobic transmembrane segments the surface bound native helical conformer is highly resistant against thermal denaturation. Circular dichroism spectroscopy experiments confirm the strong binding and thermostability of the peptide. The study highlights the utility of molecular dynamics simulations for studying transient mechanisms in fluid lipid bilayer systems. This article is part of a Special Issue entitled: Interfacially Active Peptides and Proteins. Guest Editors: William C. Wimley and Kalina Hristova. Copyright © 2014. Published by Elsevier B.V.

Intralayer magnetic ordering in Ge/Mn digital alloys

NASA Astrophysics Data System (ADS)

Otrokov, M. M.; Ernst, A.; Ostanin, S.; Fischer, G.; Buczek, P.; Sandratskii, L. M.; Hergert, W.; Mertig, I.; Kuznetsov, V. M.; Chulkov, E. V.

2011-04-01

We present a first-principles investigation of the electronic properties of Ge/Mn digital alloys obtained by the insertion of Mn monolayers in the Ge host. The main attention is devoted to the study of the magnetic properties of the Mn layers for various types of ordering of the Mn atoms. Depending on the type of Mn position three different structures are considered: substitutional, interstitial, and combined substitutional-interstitial. In all three cases numerical structural relaxation of the atomic positions has been performed. We find that the intralayer exchange parameters depend strongly on the crystal structure. For the substitutional and interstitial types of structure the stable magnetic order was found to be ferromagnetic. For the mixed substitutional-interstitial structure the ferromagnetic configuration appears unstable and a complex ferrimagnetic structure forms. The spin-wave excitations are calculated within the Heisenberg model. The critical temperatures of the magnetic phase transitions are determined using Monte Carlo simulations with interatomic exchange parameters obtained for two different magnetic reference states: a ferromagnetic and a disordered local moment state.

Identifying Atomic Scale Structure in Undoped/Doped Semicrystalline P3HT Using Inelastic Neutron Scattering

DOE PAGES

Harrelson, Thomas F.; Cheng, Yongqiang Q.; Li, Jun; ...

2017-03-07

The greatest advantage of organic materials is the ability to synthetically tune desired properties. However, structural heterogeneity often obfuscates the relationship between chemical structure and functional properties. Inelastic neutron scattering (INS) is sensitive to both local structure and chemical environment and provides atomic level details that cannot be obtained through other spectroscopic or diffraction methods. INS data are composed of a density of vibrational states with no selection rules, which means that every structural configuration is equally weighted in the spectrum. This allows the INS spectrum to be quantitatively decomposed into different structural motifs. Here in this paper we presentmore » INS measurements of the semiconducting polymer P3HT doped with F4TCNQ supported by density functional theory calculations to identify two dominant families of undoped crystalline structures and one dominant doped structural motif, in spite of considerable heterogeneity. The differences between the undoped and doped structures indicate that P3HT side chains flatten upon doping.« less

Adsorption and Dissociation of Molecular Oxygen on the (0001) Surface of Double Hexagonal Close Packed Americium

NASA Astrophysics Data System (ADS)

Dholabhai, Pratik; Atta-Fynn, Raymond; Ray, Asok

2008-03-01

Oxygen molecule adsorption on (0001) surface of double hexagonal packed americium has been studied in detail within the framework of density functional theory using a full-potential all-electron linearized augmented plane wave plus local orbitals method. The most stable configuration corresponded to molecular dissociation with the oxygen atoms occupying neighboring three-fold hollow h3 sites. Chemisorption energies and adsorption geometries for the adsorbed species, and change in work functions, magnetic moments, partial charges inside muffin-tins, difference charge density distributions and density of states for the bare Am slab and the Am slab after adsorption of the oxygen molecule will be discussed. The effects of chemisorption on Am 5f electron localization-delocalization in the vicinity of the Fermi level and the reaction barrier calculation for the dissociation of oxygen molecule to the most stable h3 sites will be discussed.

A stable compound of helium and sodium at high pressure

DOE PAGES

Dong, Xiao; Oganov, Artem R.; Goncharov, Alexander F.; ...

2017-02-06

Helium is generally understood to be chemically inert and this is due to its extremely stable closed-shell electronic configuration, zero electron affinity and an unsurpassed ionization potential. It is not known to form thermodynamically stable compounds, except a few inclusion compounds. Here, using the ab initio evolutionary algorithm USPEX and subsequent high-pressure synthesis in a diamond anvil cell, we report the discovery of a thermodynamically stable compound of helium and sodium, Na 2He, which has a fluorite-type structure and is stable at pressures >113 GPa. We show that the presence of He atoms causes strong electron localization and makes thismore » material insulating. This phase is an electride, with electron pairs localized in interstices, forming eight-centre two-electron bonds within empty Na 8 cubes. As a result, we also predict the existence of Na 2HeO with a similar structure at pressures above 15 GPa.« less

Polyanion Driven Antiferromagnetic and Insulating Ground State of Olivine Phosphates: LiMPO4

NASA Astrophysics Data System (ADS)

Jena, Ajit Kumar; Nanda, B. R. K.; Condensed Matter Theory; Computation Team

Through density functional calculations we have investigated the electronic and magnetic properties of LiMPO4, where M is a 3d transition metal element. We find that contrary to many transition metal oxides, in these Olivine phosphates the band gap is originated due to crystal field anisotropy as well as weak O-p - M-d covalent interaction. Both of them are attributed to the presence of PO43- polyanion. The anisotropic crystal field, in the absence of covalent interactions, creates atomically localized non-degenerate M-d states and therefore the gap is a natural outcome. Onsite repulsion, due to strong correlation effect, further enhances the gap. These localized d states favor high-spin configuration which leads to antiferromagnetic ordering due to Hund's coupling. Experimentally observed low Neel temperature of this family of compounds is explained from the DFT obtained spin exchange interaction parameters. Work supported by Nissan Research Program.

A stable compound of helium and sodium at high pressure

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dong, Xiao; Oganov, Artem R.; Goncharov, Alexander F.

Helium is generally understood to be chemically inert and this is due to its extremely stable closed-shell electronic configuration, zero electron affinity and an unsurpassed ionization potential. It is not known to form thermodynamically stable compounds, except a few inclusion compounds. Here, using the ab initio evolutionary algorithm USPEX and subsequent high-pressure synthesis in a diamond anvil cell, we report the discovery of a thermodynamically stable compound of helium and sodium, Na 2He, which has a fluorite-type structure and is stable at pressures >113 GPa. We show that the presence of He atoms causes strong electron localization and makes thismore » material insulating. This phase is an electride, with electron pairs localized in interstices, forming eight-centre two-electron bonds within empty Na 8 cubes. We also predict the existence of Na 2HeO with a similar structure at pressures above 15 GPa.« less

A stable compound of helium and sodium at high pressure

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dong, Xiao; Oganov, Artem R.; Goncharov, Alexander F.

Helium is generally understood to be chemically inert and this is due to its extremely stable closed-shell electronic configuration, zero electron affinity and an unsurpassed ionization potential. It is not known to form thermodynamically stable compounds, except a few inclusion compounds. Here, using the ab initio evolutionary algorithm USPEX and subsequent high-pressure synthesis in a diamond anvil cell, we report the discovery of a thermodynamically stable compound of helium and sodium, Na 2He, which has a fluorite-type structure and is stable at pressures >113 GPa. We show that the presence of He atoms causes strong electron localization and makes thismore » material insulating. This phase is an electride, with electron pairs localized in interstices, forming eight-centre two-electron bonds within empty Na 8 cubes. As a result, we also predict the existence of Na 2HeO with a similar structure at pressures above 15 GPa.« less

Kinetic-energy matrix elements for atomic Hylleraas-CI wave functions.

PubMed

Harris, Frank E

2016-05-28

Hylleraas-CI is a superposition-of-configurations method in which each configuration is constructed from a Slater-type orbital (STO) product to which is appended (linearly) at most one interelectron distance rij. Computations of the kinetic energy for atoms by this method have been difficult due to the lack of formulas expressing these matrix elements for general angular momentum in terms of overlap and potential-energy integrals. It is shown here that a strategic application of angular-momentum theory, including the use of vector spherical harmonics, enables the reduction of all atomic kinetic-energy integrals to overlap and potential-energy matrix elements. The new formulas are validated by showing that they yield correct results for a large number of integrals published by other investigators.

Atom chips with free-standing two-dimensional electron gases: advantages and challenges

NASA Astrophysics Data System (ADS)

Sinuco-León, G. A.; Krüger, P.; Fromhold, T. M.

2018-03-01

In this work, we consider the advantages and challenges of using free-standing two-dimensional electron gases (2DEG) as active components in atom chips for manipulating ultracold ensembles of alkali atoms. We calculate trapping parameters achievable with typical high-mobility 2DEGs in an atom chip configuration and identify advantages of this system for trapping atoms at sub-micron distances from the atom chip. We show how the sensitivity of atomic gases to magnetic field inhomogeneity can be exploited for controlling the atoms with quantum electronic devices and, conversely, using the atoms to probe the structural and transport properties of semiconductor devices.

Delaminated graphene at silicon carbide facets: atomic scale imaging and spectroscopy.

PubMed

Nicotra, Giuseppe; Ramasse, Quentin M; Deretzis, Ioannis; La Magna, Antonino; Spinella, Corrado; Giannazzo, Filippo

2013-04-23

Atomic-resolution structural and spectroscopic characterization techniques (scanning transmission electron microscopy and electron energy loss spectroscopy) are combined with nanoscale electrical measurements (conductive atomic force microscopy) to study at the atomic scale the properties of graphene grown epitaxially through the controlled graphitization of a hexagonal SiC(0001) substrate by high temperature annealing. This growth technique is known to result in a pronounced electron-doping (∼10(13) cm(-2)) of graphene, which is thought to originate from an interface carbon buffer layer strongly bound to the substrate. The scanning transmission electron microscopy analysis, carried out at an energy below the knock-on threshold for carbon to ensure no damage is imparted to the film by the electron beam, demonstrates that the buffer layer present on the planar SiC(0001) face delaminates from it on the (112n) facets of SiC surface steps. In addition, electron energy loss spectroscopy reveals that the delaminated layer has a similar electronic configuration to purely sp2-hybridized graphene. These observations are used to explain the local increase of the graphene sheet resistance measured around the surface steps by conductive atomic force microscopy, which we suggest is due to significantly lower substrate-induced doping and a resonant scattering mechanism at the step regions. A first-principles-calibrated theoretical model is proposed to explain the structural instability of the buffer layer on the SiC facets and the resulting delamination.

Single and double carbon vacancies in pyrene as first models for graphene defects: A survey of the chemical reactivity toward hydrogen

NASA Astrophysics Data System (ADS)

Nieman, Reed; Das, Anita; Aquino, Adélia J. A.; Amorim, Rodrigo G.; Machado, Francisco B. C.; Lischka, Hans

2017-01-01

Graphene is regarded as one of the most promising materials for nanoelectronics applications. Defects play an important role in modulating its electronic properties and also enhance its chemical reactivity. In this work the reactivity of single vacancies (SV) and double vacancies (DV) in reaction with a hydrogen atom Hr is studied. Because of the complicated open shell electronic structures of these defects due to dangling bonds, multireference configuration interaction (MRCI) methods are being used in combination with a previously developed defect model based on pyrene. Comparison of the stability of products derived from Csbnd Hr bond formation with different carbon atoms of the different polyaromatic hydrocarbons is made. In the single vacancy case the most stable structure is the one where the incoming hydrogen is bound to the carbon atom carrying the dangling bond. However, stable Csbnd Hr bonded structures are also observed in the five-membered ring of the single vacancy. In the double vacancy, most stable bonding of the reactant Hr atom is found in the five-membered rings. In total, Csbnd Hr bonds, corresponding to local energy minimum structures, are formed with all carbon atoms in the different defect systems and the pyrene itself. Reaction profiles for the four lowest electronic states show in the case of a single vacancy a complex picture of curve crossings and avoided crossings which will give rise to a complex nonadiabatic reaction dynamics involving several electronic states.

Cretin Memory Flow on Sierra

DOE Office of Scientific and Technical Information (OSTI.GOV)

Langer, S. H.; Scott, H. A.

2016-08-05

The Cretin iCOE project has a goal of enabling the efficient generation of Non-LTE opacities for use in radiation-hydrodynamic simulation codes using the Nvidia boards on LLNL’s upcoming Sierra system. Achieving the desired level of accuracy for some simulations require the use of a vary large number of atomic configurations (a configuration includes the atomic level for all electrons and how they are coupled together). The NLTE rate matrix needs to be solved separately in each zone. Calculating NLTE opacities can consume more time than all other physics packages used in a simulation.

On the Use of a Mixed Gaussian/Finite-Element Basis Set for the Calculation of Rydberg States

NASA Technical Reports Server (NTRS)

Thuemmel, Helmar T.; Langhoff, Stephen (Technical Monitor)

1996-01-01

Configuration-interaction studies are reported for the Rydberg states of the helium atom using mixed Gaussian/finite-element (GTO/FE) one particle basis sets. Standard Gaussian valence basis sets are employed, like those, used extensively in quantum chemistry calculations. It is shown that the term values for high-lying Rydberg states of the helium atom can be obtained accurately (within 1 cm -1), even for a small GTO set, by augmenting the n-particle space with configurations, where orthonormalized interpolation polynomials are singly occupied.

Atom Interferometry in a Warm Vapor

DOE PAGES

Biedermann, G. W.; McGuinness, H. J.; Rakholia, A. V.; ...

2017-04-17

Here, we demonstrate matter-wave interference in a warm vapor of rubidium atoms. Established approaches to light-pulse atom interferometry rely on laser cooling to concentrate a large ensemble of atoms into a velocity class resonant with the atom optical light pulse. In our experiment, we show that clear interference signals may be obtained without laser cooling. This effect relies on the Doppler selectivity of the atom interferometer resonance. Lastly, this interferometer may be configured to measure accelerations, and we demonstrate that multiple interferometers may be operated simultaneously by addressing multiple velocity classes.

Atom optics in the time domain

NASA Astrophysics Data System (ADS)

Arndt, M.; Szriftgiser, P.; Dalibard, J.; Steane, A. M.

1996-05-01

Atom-optics experiments are presented using a time-modulated evanescent light wave as an atomic mirror in the trampoline configuration, i.e., perpendicular to the direction of the atomic free fall. This modulated mirror is used to accelerate cesium atoms, to focus their trajectories, and to apply a ``multiple lens'' to separately focus different velocity classes of atoms originating from a point source. We form images of a simple two-slit object to show the resolution of the device. The experiments are modelled by a general treatment analogous to classical ray optics.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Biedermann, G. W.; McGuinness, H. J.; Rakholia, A. V.

Here, we demonstrate matter-wave interference in a warm vapor of rubidium atoms. Established approaches to light-pulse atom interferometry rely on laser cooling to concentrate a large ensemble of atoms into a velocity class resonant with the atom optical light pulse. In our experiment, we show that clear interference signals may be obtained without laser cooling. This effect relies on the Doppler selectivity of the atom interferometer resonance. Lastly, this interferometer may be configured to measure accelerations, and we demonstrate that multiple interferometers may be operated simultaneously by addressing multiple velocity classes.

Overview of Three-Dimensional Atomic-Resolution Holography and Imaging Techniques: Recent Advances in Local-Structure Science

NASA Astrophysics Data System (ADS)

Daimon, Hiroshi

2018-06-01

Local three-dimensional (3D) atomic arrangements without periodicity have not been able to be studied until recently. Recently, several holographies and related techniques have been developed to reveal the 3D atomic arrangement around specific atoms with no translational symmetry. This review gives an overview of these new local 3D atomic imaging techniques.

High-Resolution Coarse-Grained Modeling Using Oriented Coarse-Grained Sites.

PubMed

Haxton, Thomas K

2015-03-10

We introduce a method to bring nearly atomistic resolution to coarse-grained models, and we apply the method to proteins. Using a small number of coarse-grained sites (about one per eight atoms) but assigning an independent three-dimensional orientation to each site, we preferentially integrate out stiff degrees of freedom (bond lengths and angles, as well as dihedral angles in rings) that are accurately approximated by their average values, while retaining soft degrees of freedom (unconstrained dihedral angles) mostly responsible for conformational variability. We demonstrate that our scheme retains nearly atomistic resolution by mapping all experimental protein configurations in the Protein Data Bank onto coarse-grained configurations and then analytically backmapping those configurations back to all-atom configurations. This roundtrip mapping throws away all information associated with the eliminated (stiff) degrees of freedom except for their average values, which we use to construct optimal backmapping functions. Despite the 4:1 reduction in the number of degrees of freedom, we find that heavy atoms move only 0.051 Å on average during the roundtrip mapping, while hydrogens move 0.179 Å on average, an unprecedented combination of efficiency and accuracy among coarse-grained protein models. We discuss the advantages of such a high-resolution model for parametrizing effective interactions and accurately calculating observables through direct or multiscale simulations.

Intrinsic two-dimensional states on the pristine surface of tellurium

NASA Astrophysics Data System (ADS)

Li, Pengke; Appelbaum, Ian

2018-05-01

Atomic chains configured in a helical geometry have fascinating properties, including phases hosting localized bound states in their electronic structure. We show how the zero-dimensional state—bound to the edge of a single one-dimensional helical chain of tellurium atoms—evolves into two-dimensional bands on the c -axis surface of the three-dimensional trigonal bulk. We give an effective Hamiltonian description of its dispersion in k space by exploiting confinement to a virtual bilayer, and elaborate on the diminished role of spin-orbit coupling. These intrinsic gap-penetrating surface bands were neglected in the interpretation of seminal experiments, where two-dimensional transport was otherwise attributed to extrinsic accumulation layers.

Anomalous vibrational modes in acetanilide: A F. D. S. incoherent inelastic neutron scattering study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Barthes, M.; Moret, J.; Eckert, J.

1991-01-01

The origin of the anomalous infra-red and Raman modes in acetanilide (C{sub 6}H{sub 5}NHCOCH{sub 3}, or ACN), remains a subject of considerable controversy. One family of theoretical models involves Davydov-like solitons nonlinear vibrational coupling, or polaronic'' localized modes. An alternative interpretation of the extra-bands in terms of a Fermi resonance was proposed and recently the existence of slightly non-degenerate hydrogen atom configurations in the H-bond was suggested as an explanation for the anomalies. In this paper we report some new results on the anomalous vibrational modes in ACN that were obtained by inelastic incoherent neutron scattering (INS).

Holographic Reconstruction of Photoelectron Diffraction and Its Circular Dichroism for Local Structure Probing

NASA Astrophysics Data System (ADS)

Matsui, Fumihiko; Matsushita, Tomohiro; Daimon, Hiroshi

2018-06-01

The local atomic structure around a specific element atom can be recorded as a photoelectron diffraction pattern. Forward focusing peaks and diffraction rings around them indicate the directions and distances from the photoelectron emitting atom to the surrounding atoms. The state-of-the-art holography reconstruction algorithm enables us to image the local atomic arrangement around the excited atom in a real space. By using circularly polarized light as an excitation source, the angular momentum transfer from the light to the photoelectron induces parallax shifts in these diffraction patterns. As a result, stereographic images of atomic arrangements are obtained. These diffraction patterns can be used as atomic-site-resolved probes for local electronic structure investigation in combination with spectroscopy techniques. Direct three-dimensional atomic structure visualization and site-specific electronic property analysis methods are reviewed. Furthermore, circular dichroism was also found in valence photoelectron and Auger electron diffraction patterns. The investigation of these new phenomena provides hints for the development of new techniques for local structure probing.

Hierarchical structures of amorphous solids characterized by persistent homology

PubMed Central

Hiraoka, Yasuaki; Nakamura, Takenobu; Hirata, Akihiko; Escolar, Emerson G.; Matsue, Kaname; Nishiura, Yasumasa

2016-01-01

This article proposes a topological method that extracts hierarchical structures of various amorphous solids. The method is based on the persistence diagram (PD), a mathematical tool for capturing shapes of multiscale data. The input to the PDs is given by an atomic configuration and the output is expressed as 2D histograms. Then, specific distributions such as curves and islands in the PDs identify meaningful shape characteristics of the atomic configuration. Although the method can be applied to a wide variety of disordered systems, it is applied here to silica glass, the Lennard-Jones system, and Cu-Zr metallic glass as standard examples of continuous random network and random packing structures. In silica glass, the method classified the atomic rings as short-range and medium-range orders and unveiled hierarchical ring structures among them. These detailed geometric characterizations clarified a real space origin of the first sharp diffraction peak and also indicated that PDs contain information on elastic response. Even in the Lennard-Jones system and Cu-Zr metallic glass, the hierarchical structures in the atomic configurations were derived in a similar way using PDs, although the glass structures and properties substantially differ from silica glass. These results suggest that the PDs provide a unified method that extracts greater depth of geometric information in amorphous solids than conventional methods. PMID:27298351

Multiscale Macromolecular Simulation: Role of Evolving Ensembles

PubMed Central

Singharoy, A.; Joshi, H.; Ortoleva, P.J.

2013-01-01

Multiscale analysis provides an algorithm for the efficient simulation of macromolecular assemblies. This algorithm involves the coevolution of a quasiequilibrium probability density of atomic configurations and the Langevin dynamics of spatial coarse-grained variables denoted order parameters (OPs) characterizing nanoscale system features. In practice, implementation of the probability density involves the generation of constant OP ensembles of atomic configurations. Such ensembles are used to construct thermal forces and diffusion factors that mediate the stochastic OP dynamics. Generation of all-atom ensembles at every Langevin timestep is computationally expensive. Here, multiscale computation for macromolecular systems is made more efficient by a method that self-consistently folds in ensembles of all-atom configurations constructed in an earlier step, history, of the Langevin evolution. This procedure accounts for the temporal evolution of these ensembles, accurately providing thermal forces and diffusions. It is shown that efficiency and accuracy of the OP-based simulations is increased via the integration of this historical information. Accuracy improves with the square root of the number of historical timesteps included in the calculation. As a result, CPU usage can be decreased by a factor of 3-8 without loss of accuracy. The algorithm is implemented into our existing force-field based multiscale simulation platform and demonstrated via the structural dynamics of viral capsomers. PMID:22978601

Interacting Dark Resonances with Plasmonic Meta-Molecules

DTIC Science & Technology

2014-09-17

different K-subsystems, as seen in Fig. 1(b). Within the transparency window, of the K-configuration atomic electromagnetic induced transparency ( EIT ...exhibits EIT -type phenomena as seen by a reduction in absorbance at x 264 THz. The basic physical mechanism behind this EIT -type phenomena can be...radiative plasmonic atom.5 However, in the presence of a second dark plasmonic atom, the EIT -type transparency at FIG. 1. (a) Atomic four-level system

Energy Landscape of All-Atom Protein-Protein Interactions Revealed by Multiscale Enhanced Sampling

PubMed Central

Moritsugu, Kei; Terada, Tohru; Kidera, Akinori

2014-01-01

Protein-protein interactions are regulated by a subtle balance of complicated atomic interactions and solvation at the interface. To understand such an elusive phenomenon, it is necessary to thoroughly survey the large configurational space from the stable complex structure to the dissociated states using the all-atom model in explicit solvent and to delineate the energy landscape of protein-protein interactions. In this study, we carried out a multiscale enhanced sampling (MSES) simulation of the formation of a barnase-barstar complex, which is a protein complex characterized by an extraordinary tight and fast binding, to determine the energy landscape of atomistic protein-protein interactions. The MSES adopts a multicopy and multiscale scheme to enable for the enhanced sampling of the all-atom model of large proteins including explicit solvent. During the 100-ns MSES simulation of the barnase-barstar system, we observed the association-dissociation processes of the atomistic protein complex in solution several times, which contained not only the native complex structure but also fully non-native configurations. The sampled distributions suggest that a large variety of non-native states went downhill to the stable complex structure, like a fast folding on a funnel-like potential. This funnel landscape is attributed to dominant configurations in the early stage of the association process characterized by near-native orientations, which will accelerate the native inter-molecular interactions. These configurations are guided mostly by the shape complementarity between barnase and barstar, and lead to the fast formation of the final complex structure along the downhill energy landscape. PMID:25340714

Spectral neighbor analysis method for automated generation of quantum-accurate interatomic potentials

DOE Office of Scientific and Technical Information (OSTI.GOV)

Thompson, Aidan P.; Swiler, Laura P.; Trott, Christian R.

2015-03-15

Here, we present a new interatomic potential for solids and liquids called Spectral Neighbor Analysis Potential (SNAP). The SNAP potential has a very general form and uses machine-learning techniques to reproduce the energies, forces, and stress tensors of a large set of small configurations of atoms, which are obtained using high-accuracy quantum electronic structure (QM) calculations. The local environment of each atom is characterized by a set of bispectrum components of the local neighbor density projected onto a basis of hyperspherical harmonics in four dimensions. The bispectrum components are the same bond-orientational order parameters employed by the GAP potential [1].more » The SNAP potential, unlike GAP, assumes a linear relationship between atom energy and bispectrum components. The linear SNAP coefficients are determined using weighted least-squares linear regression against the full QM training set. This allows the SNAP potential to be fit in a robust, automated manner to large QM data sets using many bispectrum components. The calculation of the bispectrum components and the SNAP potential are implemented in the LAMMPS parallel molecular dynamics code. We demonstrate that a previously unnoticed symmetry property can be exploited to reduce the computational cost of the force calculations by more than one order of magnitude. We present results for a SNAP potential for tantalum, showing that it accurately reproduces a range of commonly calculated properties of both the crystalline solid and the liquid phases. In addition, unlike simpler existing potentials, SNAP correctly predicts the energy barrier for screw dislocation migration in BCC tantalum.« less

Spectral neighbor analysis method for automated generation of quantum-accurate interatomic potentials

DOE Office of Scientific and Technical Information (OSTI.GOV)

Thompson, A.P., E-mail: athomps@sandia.gov; Swiler, L.P., E-mail: lpswile@sandia.gov; Trott, C.R., E-mail: crtrott@sandia.gov

2015-03-15

We present a new interatomic potential for solids and liquids called Spectral Neighbor Analysis Potential (SNAP). The SNAP potential has a very general form and uses machine-learning techniques to reproduce the energies, forces, and stress tensors of a large set of small configurations of atoms, which are obtained using high-accuracy quantum electronic structure (QM) calculations. The local environment of each atom is characterized by a set of bispectrum components of the local neighbor density projected onto a basis of hyperspherical harmonics in four dimensions. The bispectrum components are the same bond-orientational order parameters employed by the GAP potential [1]. Themore » SNAP potential, unlike GAP, assumes a linear relationship between atom energy and bispectrum components. The linear SNAP coefficients are determined using weighted least-squares linear regression against the full QM training set. This allows the SNAP potential to be fit in a robust, automated manner to large QM data sets using many bispectrum components. The calculation of the bispectrum components and the SNAP potential are implemented in the LAMMPS parallel molecular dynamics code. We demonstrate that a previously unnoticed symmetry property can be exploited to reduce the computational cost of the force calculations by more than one order of magnitude. We present results for a SNAP potential for tantalum, showing that it accurately reproduces a range of commonly calculated properties of both the crystalline solid and the liquid phases. In addition, unlike simpler existing potentials, SNAP correctly predicts the energy barrier for screw dislocation migration in BCC tantalum.« less

Support effects on adsorption and catalytic activation of O2 in single atom iron catalysts with graphene-based substrates.

PubMed

Gao, Zheng-Yang; Yang, Wei-Jie; Ding, Xun-Lei; Lv, Gang; Yan, Wei-Ping

2018-03-07

The adsorption and catalytic activation of O 2 on single atom iron catalysts with graphene-based substrates were investigated systematically by density functional theory calculation. It is found that the support effects of graphene-based substrates have a significant influence on the stability of the single atom catalysts, the adsorption configuration, the electron transfer mechanism, the adsorption energy and the energy barrier. The differences in the stable adsorption configuration of O 2 on single atom iron catalysts with different graphene-based substrates can be well understood by the symmetrical matching principle based on frontier molecular orbital analysis. There are two different mechanisms of electron transfer, in which the Fe atom acts as the electron donor in single vacancy graphene-based substrates while the Fe atom mainly acts as the bridge for electron transfer in double vacancy graphene-based substrates. The Fermi softness and work function are good descriptors of the adsorption energy and they can well reveal the relationship between electronic structure and adsorption energy. This single atom iron catalyst with single vacancy graphene modified by three nitrogen atoms is a promising non-noble metal single atom catalyst in the adsorption and catalytic oxidation of O 2 . Furthermore, the findings can lay the foundation for the further study of graphene-based support effects and provide a guideline for the development and design of new non-noble-metal single atom catalysts.

Teleporting entanglements of cavity-field states

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pires, Geisa; Baseia, B.; Almeida, N.G. de

2004-08-01

We present a scheme to teleport an entanglement of zero- and one-photon states from one cavity to another. The scheme, which has 100% success probability, relies on two perfect and identical bimodal cavities, a collection of two kinds of two-level atoms, a three-level atom in a ladder configuration driven by a classical field, Ramsey zones, and selective atomic-state detectors.

Evaluation of fuel injection configurations to control carbon and soot formation in small GT combustors

NASA Technical Reports Server (NTRS)

Rosfjord, T. J.; Briehl, D.

1982-01-01

An experimental program to investigate hardware configurations which attempt to minimize carbon formation and soot production without sacrificing performance in small gas turbine combustors has been conducted at the United Technologies Research Center. Four fuel injectors, embodying either airblast atomization, pressure atomization, or fuel vaporization techniques, were combined with nozzle air swirlers and injector sheaths, and evaluated at test conditions which included and extended beyond standard small gas turbine combustor operation. Extensive testing was accomplished with configurations embodying either a spill return or a T-vaporizer injector. Minimal carbon deposits were observed on the spill return nozzle for tests using either Jet A or ERBS test fuel. A more extensive film of soft carbon was observed on the vaporizer after operation at standard engine conditions, with large carbonaceous growths forming on the device during off-design operation at low combustor inlet temperature. Test results indicated that smoke emission levels depended on the combustor fluid mechanics (especially the mixing rates near the injector), the atomization quality of the injector and the fuel hydrogen content.

Core excitation effects on oscillator strengths for transitions in four electron atomic systems

NASA Astrophysics Data System (ADS)

Chang, T. N.; Luo, Yuxiang

2007-06-01

By including explicitly the electronic configurations with two and three simultaneously excited electronic orbital, we have extended the BSCI (B-spline based configuration interaction) method [1] to estimate directly the effect of inner shell core excitation to oscillator strengths for transitions in four-electron atomic systems. We will present explicitly the change in oscillator strengths due to core excitations, especially for transitions involving doubly excited states and those with very small oscillator strengths. The length and velocity results are typically in agreement better than 1% or less. [1] Tu-nan Chang, in Many-body Theory of Atomic Structure and Photoionization, edited by T. N. Chang (World Scientific, Singapore, 1993), p. 213-47; and T. N. Chang and T. K. Fang, Elsevier Radiation Physics and Chemistry 70, 173-190 (2004).

Kinetic-energy matrix elements for atomic Hylleraas-CI wave functions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Harris, Frank E., E-mail: harris@qtp.ufl.edu

Hylleraas-CI is a superposition-of-configurations method in which each configuration is constructed from a Slater-type orbital (STO) product to which is appended (linearly) at most one interelectron distance r{sub ij}. Computations of the kinetic energy for atoms by this method have been difficult due to the lack of formulas expressing these matrix elements for general angular momentum in terms of overlap and potential-energy integrals. It is shown here that a strategic application of angular-momentum theory, including the use of vector spherical harmonics, enables the reduction of all atomic kinetic-energy integrals to overlap and potential-energy matrix elements. The new formulas are validatedmore » by showing that they yield correct results for a large number of integrals published by other investigators.« less

A relativistic density functional study of the role of 5f electrons in atomic and molecular adsorptions on actinide surfaces

NASA Astrophysics Data System (ADS)

Huda, Muhammad Nurul

Atomic and molecular adsorptions of oxygen and hydrogen on actinide surfaces have been studied within the generalized gradient approximations to density functional theory (GGA-DFT). The primary goal of this work is to understand the details of the adsorption processes, such as chemisorption sites, energies, adsorption configurations and activation energies for dissociation of molecules; and the signature role of the plutonium 5f electrons. The localization of the 5f electrons remains one of central questions in actinides and one objective here is to understand the extent to which localizations plays a role in adsorption on actinide surfaces. We also investigated the magnetism of the plutonium surfaces, given the fact that magnetism in bulk plutonium is a highly controversial issue, and the surface magnetism of it is not a well explored territory. Both the non-spin-polarized and spin-polarized calculations have been performed to arrive at our conclusions. We have studied both the atomic and molecular hydrogen and oxygen adsorptions on plutonium (100) and (111) surfaces. We have also investigated the oxygen molecule adsorptions on uranium (100) surface. Comparing the adsorption on uranium and plutonium (100) surfaces, we have seen that O2 chemisorption energy for the most favorable adsorption site on uranium surface has higher chemisorption energy, 9.492 eV, than the corresponding plutonium site, 8.787 eV. Also degree of localization of 5f electrons is less for uranium surface. In almost all of the cases, the most favorable adsorption sites are found where the coordination numbers are higher. For example, we found center sites are the most favorable sites for atomic adsorptions. In general oxygen reacts more strongly with plutonium surface than hydrogen. We found that atomic oxygen adsorption energy on (100) surface is 3.613 eV more than that of the hydrogen adsorptions, considering only the most favorable site. This is also true for molecular adsorptions, as the oxygen molecules on both (100) and (111) plutonium surfaces dissociate almost spontaneously, whereas hydrogen needs some activation energy to dissociate. From spin-polarized calculations we found both (100) and (111) surfaces have the layer by layer alternating spin-magnetic behavior. In general adsorption of H2 and O2 do not change this behavior.

Atomic scale behavior of oxygen-based radicals in water

NASA Astrophysics Data System (ADS)

Verlackt, C. C. W.; Neyts, E. C.; Bogaerts, A.

2017-03-01

Cold atmospheric pressure plasmas in and in contact with liquids represent a growing field of research for various applications. Understanding the interactions between the plasma generated species and the liquid is crucial. In this work we perform molecular dynamics (MD) simulations based on a quantum mechanical method, i.e. density-functional based tight-binding (DFTB), to examine the interactions of OH radicals and O atoms in bulk water. Our calculations reveal that the transport of OH radicals through water is not only governed by diffusion, but also by an equilibrium reaction of H-abstraction with water molecules. Furthermore, when two OH radicals encounter each other, they either form a stable cluster, or react, resulting in the formation of a new water molecule and an O atom. In addition, the O atoms form either oxywater (when in singlet configuration) or they remain stable in solution (when in triplet configuration), stressing the important role that O atoms can play in aqueous solution, and in contact with biomolecules. Our observations are in line with both experimental and ab initio results from the literature.

Ab-initio calculations of the proton location in topaz-OH, Al2SiO4(OH)2

NASA Astrophysics Data System (ADS)

Churakov, S. V.; Wunder, B.

The position of hydrogen in the structure of topaz-OH was determined by means of ab-initio quantum-mechanic calculations. Static lattice energy calculations predict the existence of four non-equivalent positions of protons, which are characterized by O4-H1... O1, O4-H2... O2, O4-H3... O3 and O4-H4... O4 hydrogen bonds. The distribution of the protons between positions of local equilibrium is controlled by the proton-proton avoidance rule and the strength of the hydrogen bonds. The most favourable configuration of hydrogen atoms is achieved for adjacent protons, which form O4-H3... O3 and O4-H4... O4 hydrogen bonds, respectively. The thermal excitation of atoms at a temperature of 55 K is large enough for the hydrogen atoms occasionally to change their positions to form O4-H1... O1 and O4-H2... O2 bonds. At ambient pressures and higher temperatures the protons are in a dynamic exchange between the allowed positions of local minima. As a consequence, for nearly room-temperature conditions, the dynamic change between different structural configurations leads to the violation of all possible symmetry elements and with that to space group #E5/E5#1. The flipping of the protons between different sites is achieved by simple rotation of the OH-dipole and does not produce any significant distortion of the framework of topaz, whose symmetry remains that of the space group Pbnm. Therefore, no reduction of symmetry has been observed in former X-ray studies on topaz-OH. Calculated IR absorption spectra of topaz-OH were found to be in good agreement with measured spectra. According to the calculations, the two favourable configurations of protons might correspond to the measured peak splitting within the OH-stretching range. An experimentally observed low-frequency band at 3520 cm-1 was assigned to the OH-stretching of the O4-H3... O3 bond, while the band at 3600 cm-1 was attributed to OH-stretching of the O4-H4... O4 hydrogen bond. The broad peak in FAR-IR frequency range at 100-150 cm-1 is attributed to the stretching of H3... O3 and H4... O4 contacts. The rate of proton exchange at 670 K among different sites was estimated by ab-inito molecular dynamic simulations. The calculations predict that flipping of adjacent protons between O4-H3... O3 and O4-H4... O4 bonds at 670 K occur at a rate of about 1.96 THz.

Cooperative use of VCD and XRD for the determination of tetrahydrobenzoisoquinolines absolute configuration: a reliable proof of memory of chirality and retention of configuration in enediyne rearrangements.

PubMed

Mondal, Shovan; Naubron, Jean-Valère; Campolo, Damien; Giorgi, Michel; Bertrand, Michéle P; Nechab, Malek

2013-12-01

The absolute configurations (AC) of azaheterocylic compounds resulting from the cascade rearrangement of enediynes involving only light atoms were unambiguously assigned by the joint use of vibrational circular dichroism (VCD) and copper radiation single crystal X-ray diffraction (XRD). These AC determinations proved that the rearrangements of enediynes proceeded with memory of chirality and retention of configuration. © 2013 Wiley Periodicals, Inc.

Ab initio studies of isolated boron substitutional defects in graphane

NASA Astrophysics Data System (ADS)

Mapasha, R. E.; Chetty, N.

2017-10-01

We have systematically studied energetics, structural and electronic properties of different configurations of the B atoms substituting C-H pairs located on a single hexagonal ring in a graphane system using the first-principles density functional theory (DFT). A total number of 12 distinct B dopants configurations were identified and characterized. Based on the formation energy analysis, we found that relative stability of B dopants depends greatly on the defect configurations. Our results suggest that the B substitutions prefer to be distributed randomly but avoiding the formation of homo-elemental B-B bonds in a graphane system, at any concentration. Generally, the values of band gap decrease as the number of B dopants increases, but the low energy configurations have large band gaps compared to those that have homo-elemental bonds. As a result, the band gap of graphane can be fine tuned through the change in the structural arrangement of B atoms. The adequate control of the electronic structure of graphane through doping should be essential for technological device applications.

Theory of vibrationally assisted tunneling for hydroxyl monomer flipping on Cu(110)

NASA Astrophysics Data System (ADS)

Gustafsson, Alexander; Ueba, Hiromu; Paulsson, Magnus

2014-10-01

To describe vibrationally mediated configuration changes of adsorbates on surfaces we have developed a theory to calculate both reaction rates and pathways. The method uses the T-matrix to describe excitations of vibrational states by the electrons of the substrate, adsorbate, and tunneling electrons from a scanning tunneling probe. In addition to reaction rates, the theory also provides the reaction pathways by going beyond the harmonic approximation and using the full potential energy surface of the adsorbate which contains local minima corresponding to the adsorbates different configurations. To describe the theory, we reproduce the experimental results in [T. Kumagai et al., Phys. Rev. B 79, 035423 (2009), 10.1103/PhysRevB.79.035423], where the hydrogen/deuterium atom of an adsorbed hydroxyl (OH/OD) exhibits back and forth flipping between two equivalent configurations on a Cu(110) surface at T =6 K. We estimate the potential energy surface and the reaction barrier, ˜160 meV, from DFT calculations. The calculated flipping processes arise from (i) at low bias, tunneling of the hydrogen through the barrier, (ii) intermediate bias, tunneling electrons excite the vibrations increasing the reaction rate although over the barrier processes are rare, and (iii) higher bias, overtone excitations increase the reaction rate further.

Dispersion engineering with plasmonic nano structures for enhanced surface plasmon resonance sensing.

PubMed

Arora, Pankaj; Talker, Eliran; Mazurski, Noa; Levy, Uriel

2018-06-13

We demonstrate numerically and experimentally the enhancement of Surface Plasmon Resonance (SPR) sensing via dispersion engineering of the plasmonic response using plasmonic nanograting. Following their design and optimization, the plasmonic nanograting structures are fabricated using e-beam lithography and lift-off process and integrated into conventional prism based Kretschmann configuration. The presence of absorptive nanograting near the metal film, provides strong field enhancement with localization and allows to control the dispersion relation which was originally dictated by a conventional SPR structure. This contributes to the enhancement in Q factor which is found to be 3-4 times higher as compared to the conventional Kretschmann configuration. The influence of the incident angle on resonance wavelength is also demonstrated both numerically and experimentally, where, only a negligible wavelength shift is observed with increasing the incident angles for plasmonic nanograting configuration. This surprising feature may be helpful for studying and utilizing light-matter interaction between plasmons and narrow linewidth media (e.g. Rb atom or molecule) having nonlocalities in their susceptibility-momentum relation. Finally, we analyze the role of plasmonic nanograting in enhancing the performance of an SPR sensor. Our results indicate that the integrated SPR-nanograting device shows a great promise as a sensor for various types of analytes.

Atomic radii for atoms with the 6s shell outermost: The effective atomic radius and the van der Waals radius from {sub 55}Cs to {sub 80}Hg

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tatewaki, Hiroshi, E-mail: htatewak@nsc.nagoya-cu.ac.jp; Institute of Advanced Studies in Artificial Intelligence, Chukyo University, Toyota, Aichi 470-0393; Hatano, Yasuyo

We consider, for atoms from {sub 55}Cs to {sub 80}Hg, the effective atomic radius (r{sub ear}), which is defined as the distance from the nucleus at which the magnitude of the electric field is equal to that in He at one half of the equilibrium bond length of He{sub 2}. The values of r{sub ear} are about 50% larger than the mean radius of the outermost occupied orbital of 6s, . The value of r{sub ear} decreases from {sub 55}Cs to {sub 56}Ba and undergoes increases and decreases with rising nuclear charge from {sub 57}La to {sub 70}Y b. Inmore » fact r{sub ear} is understood as comprising two interlaced sequences; one consists of {sub 57}La, {sub 58}Ce, and {sub 64}Gd, which have electronic configuration (4f{sup n−1})(5d{sup 1})(6s{sup 2}), and the remaining atoms have configuration (4f{sup n})(6s{sup 2}). The sphere defined by r{sub ear} contains 85%–90% of the 6s electrons. From {sub 71}Lu to {sub 80}Hg the radius r{sub ear} also involves two sequences, corresponding to the two configurations 5d{sup n+1}6s{sup 1} and 5d{sup n}6s{sup 2}. The radius r{sub ear} according to the present methodology is considerably larger than r{sub vdW} obtained by other investigators, some of who have found values of r{sub vdW} close to .« less

Fine- and hyperfine structure investigations of even configuration system of atomic terbium

NASA Astrophysics Data System (ADS)

Stefanska, D.; Elantkowska, M.; Ruczkowski, J.; Furmann, B.

2017-03-01

In this work a parametric study of the fine structure (fs) and the hyperfine structure (hfs) for the even-parity configurations of atomic terbium (Tb I) is presented, based in considerable part on the new experimental results. Measurements on 134 spectral lines were performed by laser induced fluorescence (LIF) in a hollow cathode discharge lamp; on this basis, the hyperfine structure constants A and B were determined for 52 even-parity levels belonging to the configurations 4f85d6s2, 4f85d26s or 4f96s6p; in all the cases those levels were involved in the transitions investigated as the lower levels. For 40 levels the hfs was examined for the first time, and for the remaining 12 levels the new measurements supplement our earlier results. As a by-product, also preliminary values of the hfs constants for 84 odd-parity levels were determined (the investigations of the odd-parity levels system in the terbium atom are still in progress). This huge amount of new experimental data, supplemented by our earlier published results, were considered for the fine and hyperfine structure analysis. A multi-configuration fit of 7 configurations was performed, taking into account second-order of perturbation theory, including the effects of closed shell-open shell excitations. Predicted values of the level energies, as well as of magnetic dipole and electric quadrupole hyperfine structure constants A and B, are quoted in cases when no experimental values are available. By combining our experimental data with our own semi-empirical procedure it was possible to identify correctly the lower and upper level of the line 544.1440 nm measured by Childs with the use of the atomic-beam laser-rf double-resonance technique (Childs, J Opt Soc Am B 9;1992:191-6).

A sequence-dependent rigid-base model of DNA

NASA Astrophysics Data System (ADS)

Gonzalez, O.; Petkevičiutė, D.; Maddocks, J. H.

2013-02-01

A novel hierarchy of coarse-grain, sequence-dependent, rigid-base models of B-form DNA in solution is introduced. The hierarchy depends on both the assumed range of energetic couplings, and the extent of sequence dependence of the model parameters. A significant feature of the models is that they exhibit the phenomenon of frustration: each base cannot simultaneously minimize the energy of all of its interactions. As a consequence, an arbitrary DNA oligomer has an intrinsic or pre-existing stress, with the level of this frustration dependent on the particular sequence of the oligomer. Attention is focussed on the particular model in the hierarchy that has nearest-neighbor interactions and dimer sequence dependence of the model parameters. For a Gaussian version of this model, a complete coarse-grain parameter set is estimated. The parameterized model allows, for an oligomer of arbitrary length and sequence, a simple and explicit construction of an approximation to the configuration-space equilibrium probability density function for the oligomer in solution. The training set leading to the coarse-grain parameter set is itself extracted from a recent and extensive database of a large number of independent, atomic-resolution molecular dynamics (MD) simulations of short DNA oligomers immersed in explicit solvent. The Kullback-Leibler divergence between probability density functions is used to make several quantitative assessments of our nearest-neighbor, dimer-dependent model, which is compared against others in the hierarchy to assess various assumptions pertaining both to the locality of the energetic couplings and to the level of sequence dependence of its parameters. It is also compared directly against all-atom MD simulation to assess its predictive capabilities. The results show that the nearest-neighbor, dimer-dependent model can successfully resolve sequence effects both within and between oligomers. For example, due to the presence of frustration, the model can successfully predict the nonlocal changes in the minimum energy configuration of an oligomer that are consequent upon a local change of sequence at the level of a single point mutation.

Reaction pathways in remote plasma nitridation of ultrathin SiO2 films

NASA Astrophysics Data System (ADS)

Niimi, Hiro; Khandelwal, Amit; Lamb, H. Henry; Lucovsky, Gerald

2002-01-01

Low-temperature nitridation of 3 nm SiO2 films using He/N2 and N2 remote radio frequency (rf) plasmas was investigated. On-line Auger electron spectroscopy and angle-resolved x-ray photoelectron spectroscopy (ARXPS) were employed to determine the concentration, spatial distribution, and local chemical bonding of nitrogen in the resultant films. Experiments were performed using a substrate temperature of 300 °C and 30 W rf power. Nitridation using an upstream He/N2 remote plasma at 0.1 Torr incorporates nitrogen at the top surface of the SiO2 film. In contrast, a lower concentration of nitrogen distributed throughout the film is obtained when the process pressure is increased to 0.3 Torr. ARXPS indicates a N-Si3 local bonding configuration, irrespective of the spatial distribution of N atoms. Slightly more nitrogen is incorporated using a downstream He/N2 plasma at each process pressure. By comparison, nitridation of SiO2 films using a N2 remote plasma at 0.1 Torr is very slow. Optical emission spectroscopy indicates that He dilution enhances the generation of N2+(B 2Σu+) species by altering the plasma electron energy distribution and by providing an additional kinetic pathway (Penning ionization). Changing the He/N2 remote plasma configuration from upstream to downstream (at 0.1 and 0.3 Torr) also enhances N2+(B 2Σu+) generation. For upstream He/N2 remote plasmas, the intensity of N2 first positive emission from N2(B 3Πg) states increases with pressure, whereas the N2+ first negative emission from N2+(B 2Σu+) states decreases. We infer from these observations that N2+ species are primarily responsible for top surface nitridation at 0.1 Torr, and that neutral species [N2(A 3Σu+) metastables and N atoms] are associated with sub-surface nitrogen incorporation.

A sequence-dependent rigid-base model of DNA.

PubMed

Gonzalez, O; Petkevičiūtė, D; Maddocks, J H

2013-02-07

A novel hierarchy of coarse-grain, sequence-dependent, rigid-base models of B-form DNA in solution is introduced. The hierarchy depends on both the assumed range of energetic couplings, and the extent of sequence dependence of the model parameters. A significant feature of the models is that they exhibit the phenomenon of frustration: each base cannot simultaneously minimize the energy of all of its interactions. As a consequence, an arbitrary DNA oligomer has an intrinsic or pre-existing stress, with the level of this frustration dependent on the particular sequence of the oligomer. Attention is focussed on the particular model in the hierarchy that has nearest-neighbor interactions and dimer sequence dependence of the model parameters. For a Gaussian version of this model, a complete coarse-grain parameter set is estimated. The parameterized model allows, for an oligomer of arbitrary length and sequence, a simple and explicit construction of an approximation to the configuration-space equilibrium probability density function for the oligomer in solution. The training set leading to the coarse-grain parameter set is itself extracted from a recent and extensive database of a large number of independent, atomic-resolution molecular dynamics (MD) simulations of short DNA oligomers immersed in explicit solvent. The Kullback-Leibler divergence between probability density functions is used to make several quantitative assessments of our nearest-neighbor, dimer-dependent model, which is compared against others in the hierarchy to assess various assumptions pertaining both to the locality of the energetic couplings and to the level of sequence dependence of its parameters. It is also compared directly against all-atom MD simulation to assess its predictive capabilities. The results show that the nearest-neighbor, dimer-dependent model can successfully resolve sequence effects both within and between oligomers. For example, due to the presence of frustration, the model can successfully predict the nonlocal changes in the minimum energy configuration of an oligomer that are consequent upon a local change of sequence at the level of a single point mutation.

Point Defects in Quenched and Mechanically-Milled Intermetallic Compounds

NASA Astrophysics Data System (ADS)

Sinha, Praveen

Investigations were made of structural and thermal point defects in the highly-ordered B2 compound PdIn and deformation-induced defects in PdIn and NiAl. The defects were detected through the quadrupole interactions they induce at nearby ^{111}In/Cd probe atoms using the technique of perturbed gamma-gamma angular correlations (PAC). Measurements on annealed PdIn on both sides of stoichiometry show structural defects that are the Pd vacancies on the Pd-poor side of the stoichiometry and Pd antisite atoms on the Pd-rich side. Signals were attributed to various defect configurations near the In/Cd probes. In addition to the first-shell Pd vacancy and second-shell Pd antisite atom configurations previously observed by Hahn and Muller, we observed two Pd-divacancy configurations in the first shell, a fourth-shell Pd vacancy, a second-shell In vacancy and the combination of a first -shell Pd vacancy and fourth-shell Pd vacancy. Vacancies on both the Pd and In sublattices were detected after quenching. Fractions of probe atoms having each type of neighboring vacancy defect were observed to increase monotonically with quenching temperature over the range 825-1500 K. For compositions very close to 50.15 at.% Pd, nearly equal site fractions were observed for Pd and In vacancies, indicating that the Schottky vacancy-pair defect is the thermal defect at high temperature. The formation enthalpy of the Schottky defect was determined from measurements of the Pd-vacancy site fraction to be 1.30(18) eV from analysis of quenching data in the range 825-1200 K, using the law of mass action and assuming a random distribution. Above 1200 K, the Pd-vacancy concentration was observed to be saturated at a value of 1.3(2) atomic percent. For more Pd-rich compositions, evidence was also obtained for a defect reaction in which a Pd antisite atom and Pd vacancy react to form an In vacancy, thereby increasing the In vacancy concentration and decreasing the Pd vacancy concentration. Analysis of defect concentrations allowed the conclusion that the In vacancy signal was due to second-shell and not third-shell defects. PAC spectroscopy was applied to study deformation -induced defects in PdIn and NiAl after mechanically milling in a SPEX 8000 vibrator mill for periods of up to four hours. For PdIn, the Pd vacancy concentration increased rapidly for short milling times and was observed to saturate at a value of 3.5(5) at.% after 10 minutes of milling when milling was carried out using a WC vial to avoid sample contamination. Such a large vacancy concentration accounts for 4.41(63) kJ mol-1 excess-stored energy in milled PdIn and implies a high density of "broken bonds" which may lead to mechanical instability of the lattice. Milling also produced In antisite atoms on the Pd sublattice. The antisite-atom concentration increased linearly with milling time, reaching a value of 4.0(7) at.% after 2 hours of milling. The Ni vacancy concentration in NiAl was also observed to increase with milling and to saturate after two hours of milling. Here, the "local" Ni vacancy concentration in the first-neighbor shell of the probe, deduced from the vacancy site fraction, was in excess of values that should occur if defects were located at random. This is attributed to binding between the Ni vacancy and the In/Cd probe, which is known from other work to be 0.22 eV.

High-precision two-dimensional atom localization from four-wave mixing in a double-Λ four-level atomic system

NASA Astrophysics Data System (ADS)

Shui, Tao; Yang, Wen-Xing; Chen, Ai-Xi; Liu, Shaopeng; Li, Ling; Zhu, Zhonghu

2018-03-01

We propose a scheme for high-precision two-dimensional (2D) atom localization via the four-wave mixing (FWM) in a four-level double-Λ atomic system. Due to the position-dependent atom-field interaction, the 2D position information of the atoms can be directly determined by the measurement of the normalized light intensity of output FWM-generated field. We further show that, when the position-dependent generated FWM field has become sufficiently intense, efficient back-coupling to the FWM generating state becomes important. This back-coupling pathway leads to competitive multiphoton destructive interference of the FWM generating state by three supplied and one internally generated fields. We find that the precision of 2D atom localization can be improved significantly by the multiphoton destructive interference and depends sensitively on the frequency detunings and the pump field intensity. Interestingly enough, we show that adjusting the frequency detunings and the pump field intensity can modify significantly the FWM efficiency, and consequently lead to a redistribution of the atoms. As a result, the atom can be localized in one of four quadrants with holding the precision of atom localization.

Intrinsic retrieval efficiency for quantum memories: A three-dimensional theory of light interaction with an atomic ensemble

NASA Astrophysics Data System (ADS)

Gujarati, Tanvi P.; Wu, Yukai; Duan, Luming

2018-03-01

Duan-Lukin-Cirac-Zoller quantum repeater protocol, which was proposed to realize long distance quantum communication, requires usage of quantum memories. Atomic ensembles interacting with optical beams based on off-resonant Raman scattering serve as convenient on-demand quantum memories. Here, a complete free space, three-dimensional theory of the associated read and write process for this quantum memory is worked out with the aim of understanding intrinsic retrieval efficiency. We develop a formalism to calculate the transverse mode structure for the signal and the idler photons and use the formalism to study the intrinsic retrieval efficiency under various configurations. The effects of atomic density fluctuations and atomic motion are incorporated by numerically simulating this system for a range of realistic experimental parameters. We obtain results that describe the variation in the intrinsic retrieval efficiency as a function of the memory storage time for skewed beam configuration at a finite temperature, which provides valuable information for optimization of the retrieval efficiency in experiments.

Forbidden line emission from highly ionized atoms in tokamak plasmas

NASA Technical Reports Server (NTRS)

Feldman, U.; Doschek, G. A.; Bhatia, A. K.

1982-01-01

Considerable interest in the observation of forbidden spectral lines from highly ionized atoms in tokamak plasmas is related to the significance of such observations for plasma diagnostic applications. Atomic data for the elements Ti Cr, Mn, Fe, Ni, and Kr have been published by Feldman et al. (1980) and Bhatia et al. (1980). The present investigation is concerned with collisional excitation rate coefficients and radiative decay rates, which are interpolated for ions of elements between calcium, and krypton and for levels of the 2s2 2pk, 2s 2p(k+1), and 2p(k+2) configurations, and for the O I, N I, C I, B I, and Be I isoelectronic sequences. The provided interpolated atomic data can be employed to calculate level populations and relative line intensities for ions of the considered sequences, taking into account levels of the stated configurations. Important plasma diagnostic information provided by the forbidden lines includes the ion temperature

Atomic Data for the CHIANTI Database

NASA Technical Reports Server (NTRS)

Bhatia, Anand K.; Landi, E.

2012-01-01

The CHIANTI spectral code consists of an atomic database and a suite of computer programs to calculate the optically thin spectrum of astrophysical objects and to carry out spectroscopic plasma diagnostics. The database includes atomic energy levels, wavelengths, radiative transition rates, collisional excitation, ionization and recombination rate coefficients, as well as data to calculate free-free, free-bound and two-photon continuum emission. In recent years, we have been pursuing a program to calculate atomic data for ions whose lines have been observed in astrophysical spectra but have been neglected in the literature, and to provide CHIANTI with all the data necessary to predict line intensities. There are two types of such ions: those for which calculations are available for low-energy configurations but not for high-energy configurations (i.e., C-like, N-like, O-like systems), and ions that have never or only seldom been studied. This poster will summarize the current status of this project and indicate the future activities .

Low-pressure hydrogen discharge maintenance in a large-size plasma source with localized high radio-frequency power deposition

DOE Office of Scientific and Technical Information (OSTI.GOV)

Todorov, D.; Shivarova, A., E-mail: ashiva@phys.uni-sofia.bg; Paunska, Ts.

2015-03-15

The development of the two-dimensional fluid-plasma model of a low-pressure hydrogen discharge, presented in the study, is regarding description of the plasma maintenance in a discharge vessel with the configuration of the SPIDER source. The SPIDER source, planned for the neutral-beam-injection plasma-heating system of ITER, is with localized high RF power deposition to its eight drivers (cylindrical-coil inductive discharges) and a large-area second chamber, common for all the drivers. The continuity equations for the charged particles (electrons and the three types of positive ions) and for the neutral species (atoms and molecules), their momentum equations, the energy balance equations formore » electrons, atoms and molecules and the Poisson equations are involved in the discharge description. In addition to the local processes in the plasma volume, the surface processes of particle reflection and conversion on the walls as well as for a heat exchange with the walls are included in the model. The analysis of the results stresses on the role of the fluxes (particle and energy fluxes) in the formation of the discharge structure. The conclusion is that the discharge behavior is completely obeyed to non-locality. The latter is displayed by: (i) maximum values of plasma parameters (charged particle densities and temperatures of the neutral species) outside the region of the RF power deposition, (ii) shifted maxima of the electron density and temperature, of the plasma potential and of the electron production, (iii) an electron flux, with a vortex structure, strongly exceeding the total ion flux which gives evidence of a discharge regime of non-ambipolarity and (iv) a spatial distribution of the densities of the neutral species resulting from their fluxes.« less

Design of graphene nanoparticle undergoing axial compression: quantum study

NASA Astrophysics Data System (ADS)

Glukhova, O. E.; Kirillova, I. V.; Saliy, I. N.; Kolesnikova, A. S.; Slepchenkov, M. M.

2011-03-01

We report the results of quantum mechanical investigations of the atomic structure and deformations of graphene nanoparticle undergoing axial compression. We applied the tight-binding (TB) method. Our transferable tightbinding potential correctly reproduced tight-binding changes in the electronic configuration as a function of the local bonding geometry around each carbon atom. The tight-binding method applied provided the consideration and calculation of the rehybridization between σ- and π-orbitals. To research nanoribbons using tight-binding potential our own program was used. We adapted TB method to be able to run the algorithm on a parallel computing machine (computer cluster). To simulate axial compression of graphene nanoparticles the atoms on the ends were fixed on the plates. The plates were moved towards each other to decrease the length at some percent. Plane atomic network undergoing axial compression became wave-like. The amplitude of wave and its period were not constant and changed along axis. This is a phase transition. The strain energy collapse occurs at the value of axial compression 0.03-0.04. The strain energy increased up to the quantity compression 0.03, then collapsed sharply and decreased. So according to our theoretical investigation, the elasticity of graphene nanoparticles is more than the elasticity of nanotubes the same width and length. The curvature of the atomic network because of compression will decrease the reactivity of graphene nanoparticles. We have calculated the atomic structure and electronic structure of the compression graphene nanopaticle at each step of strain of axial compression. We have come to the conclusion that the wave-like graphenes adsorbing protein and nucleic acid are the effective nanosensors and bionanosensors.

Investigation on structure, electronic and magnetic properties of Cr doped (ZnO)12 clusters: First-principles calculations

NASA Astrophysics Data System (ADS)

Liu, Huan; Zhang, Jian-Min

2018-05-01

The structural, electronic, and magnetic properties of (ZnO)12 clusters doped with Cr atoms have been investigated by using spin-polarized first-principles calculations. The exohedral a3 isomer is favorable than endohedral a2 isomer. The isomer a1 and a5 respectively have the narrowest and biggest gap between highest unoccupied molecular orbital and the lowest unoccupied molecular orbital (HOMO-LUMO) of 0.473 and 1.291 eV among these five monodoped isomers. The magnetic moment may be related to the local environment around the Cr atom that the a2 isomer whose total magnetic moment is 6 μB while the other monodoped isomers which all isomers have nearly total magnetic moments 4 μB . For Cr-doped (ZnO)12 on a1 or a3 isomer, the DOS of spin-up channel cross the Fermi level EF showing a finite magnitude near the Fermi level which might be useful for half metallic character. For the bidoped cases, the exohedral isomers are found to be most favorable. Including all bipoed isomers of substitutional, exohedral and endohedral bidoped clusters, the total magnetic moment of the ferromagnetic (antiferromagnetic) state is 8 (0) μB and the HOMO-LUMO gap of antiferromagnetic state is slightly larger than that of ferromagnetic state. The magnetic coupling between the Cr atoms in bidoped configurations is mainly governed by the competition between direct Cr and Cr atoms antiferromagnetic interaction and the ferromagnetic interaction between two Cr atoms via O atom due to strong p-d hybridization. Most importantly, we show that the exohedral bidoped (ZnO)12 clusters favor the ferromagnetic state, which may have the future applications in spin-dependent magneto-optical and magneto-electrical devices.

Hyperfine structure of atomic fluorine (F I)

NASA Astrophysics Data System (ADS)

Huo, Xiaoxue; Deng, Lunhua; Windholz, L.; Mu, Xiuli; Wang, Hailing

2018-01-01

A high resolution absorption spectrum of neutral fluorine(F I) was observed around 800 nm using concentration modulation absorption spectroscopy with a tunable Ti : Sapphire laser. The fluorine atoms were produced by discharging the mixed gases of helium and sulfur hexafluoride (SF6) in a glass tube. Thirty four hyperfine structure (hfs) resolved transitions were analyzed to obtain 23 magnetic dipole hfs constants A for 2p4(3P)3s, 2p4(3P)3p and 2p4(3P)3d configurations. The hfs constants in 2p4(3P)3s and 2p4(3P)3p configurations were compared with those obtained from experiments and calculations. Fifteen constants in 2p4(3P)3d configuration were reported - to our knowledge - for the first time.

Local structural aspects of metal-metal transition in IrTe2 from x-ray PDF

NASA Astrophysics Data System (ADS)

Yu, Runze; Abeykoon, Milinda; Zhou, Haidong; Yin, Weiguo; Bozin, Emil S.

Evolution of local atomic structure across the metal-metal transition in IrTe2 is explored by pair distribution function (PDF) analysis of x-ray total scattering data over 80 K

Dirac electrons in Moiré superlattice: From two to three dimensions

NASA Astrophysics Data System (ADS)

Hu, Chen; Michaud-Rioux, Vincent; Kong, Xianghua; Guo, Hong

2017-11-01

Moiré patterns in van der Waals (vdW) heterostructures bring novel physical effects to the materials. We report theoretical investigations of the Moiré pattern formed by graphene (Gr) on hexagonal boron nitride (h BN). For both the two-dimensional (2D) flat-sheet and the freestanding three-dimensional (3D) wavelike film geometries, the behaviors of Dirac electrons are strongly modulated by the local high-symmetry stacking configurations of the Moiré pattern. In the 2D flat sheet, the secondary Dirac cone (SDC) dispersion emerges due to the stacking-selected localization of SDC wave functions, while the original Dirac cone (ODC) gap is suppressed due to an overall effect of ODC wave functions. In the freestanding 3D wavelike Moiré structure, we predict that a specific local stacking in the Moiré superlattice is promoted at the expense of other local stackings, leading to an electronic structure more similar to that of the perfectly matching flat Gr/h BN than that of the flat-sheet 2D Moiré pattern. To capture the overall picture of the Moiré superlattice, supercells containing 12 322 atoms are simulated by first principles.

Calculation of the spin-polarized electronic structure of an interstitial iron impurity in silicon

NASA Astrophysics Data System (ADS)

Katayama-Yoshida, H.; Zunger, Alex

1985-06-01

We apply our self-consistent, all-electron, spin-polarized Green's-function method within an impurity-centered, dynamic basis set to study the interstitial iron impurity in silicon. We use two different formulations of the interelectron interactions: the local-spin-density (LSD) formalism and the self-interaction-corrected (SIC) local-spin-density (SIC-LSD) formalism. We find that the SIC-LSD approach is needed to obtain the correct high-spin ground state of Si:Fe+. We propose a quantitative explanation to the observed donor ionization energy and the high-spin ground states for Si:Fe+ within the SIC-LSD approach. For both Si:Fe0 and Si:Fe+, this approach leads to a hyperfine field, contact spin density, and ionization energy in better agreement with experiments than the simple LSD approach. The apparent dichotomy between the covalently delocalized nature of Si:Fe as suggested on the one hand by its reduced hyperfine field (relative to the free atom) and extended spin density and by the occurrence of two closely spaced, stable charge states (within 0.4 eV) and on the other hand by the atomically localized picture (suggested, for example, by the stability of a high-spin, ground-state configuration) is resolved. We find a large reduction in the hyperfine field and contact spin density due to the covalent hybridization between the impurity 3d orbitals and the tails of the delocalized sp3 hybrid orbitals of the surrounding silicon atoms. Using the calculated results, we discuss (i) the underlying mechanism for the stability and plurality of charged states, (ii) the covalent reduction in the hyperfine field, (iii) the remarkable constancy of the impurity Mössbauer isomer shift for different charged states, (iv) comparison with the multiple charged states in ionic crystals, and (v) some related speculation about the mechanism of (Fe2+/Fe3+) oxidation-reduction ionizations in heme proteins and electron-transporting biological systems.

Towards the blackbox computation of magnetic exchange coupling parameters in polynuclear transition-metal complexes: theory, implementation, and application.

PubMed

Phillips, Jordan J; Peralta, Juan E

2013-05-07

We present a method for calculating magnetic coupling parameters from a single spin-configuration via analytic derivatives of the electronic energy with respect to the local spin direction. This method does not introduce new approximations beyond those found in the Heisenberg-Dirac Hamiltonian and a standard Kohn-Sham Density Functional Theory calculation, and in the limit of an ideal Heisenberg system it reproduces the coupling as determined from spin-projected energy-differences. Our method employs a generalized perturbative approach to constrained density functional theory, where exact expressions for the energy to second order in the constraints are obtained by analytic derivatives from coupled-perturbed theory. When the relative angle between magnetization vectors of metal atoms enters as a constraint, this allows us to calculate all the magnetic exchange couplings of a system from derivatives with respect to local spin directions from the high-spin configuration. Because of the favorable computational scaling of our method with respect to the number of spin-centers, as compared to the broken-symmetry energy-differences approach, this opens the possibility for the blackbox exploration of magnetic properties in large polynuclear transition-metal complexes. In this work we outline the motivation, theory, and implementation of this method, and present results for several model systems and transition-metal complexes with a variety of density functional approximations and Hartree-Fock.

Novel optical properties of CdS:Zn rocksalt system (a theoretical study)

NASA Astrophysics Data System (ADS)

Khan, M. Junaid Iqbal; Nauman Usmani, M.; Kanwal, Zarfishan

2017-11-01

In present computational study, we focus on optical properties of Zn doped CdS for 1  ×  1  ×  2 and 2  ×  2  ×  2 supercell configurations. Cd atoms are substituted with Zn atoms and results for optical properties demonstrate different trends due to interaction of Zn with S atoms. The study has been performed by PBE-GGA approach using Wien2K within framework of DFT. TDOS and PDOS represent that S-3p states are responsible for conduction. For large supercell configuration, a tremendous change in optical properties has been observed due to different bonding. Optical absorption tends to increase in visible range which supports candidacy of Zn doped CdS for enhanced optoelectronic and nanotechnology applications.

NLTE atomic kinetics modeling in ICF target simulations

NASA Astrophysics Data System (ADS)

Patel, Mehul V.; Mauche, Christopher W.; Scott, Howard A.; Jones, Ogden S.; Shields, Benjamin T.

2017-10-01

Radiation hydrodynamics (HYDRA) simulations using recently developed 1D spherical and 2D cylindrical hohlraum models have enabled a reassessment of the accuracy of energetics modeling across a range of NIF target configurations. Higher-resolution hohlraum calculations generally find that the X-ray drive discrepancies are greater than previously reported. We identify important physics sensitivities in the modeling of the NLTE wall plasma and highlight sensitivity variations between different hohlraum configurations (e.g. hohlraum gas fill). Additionally, 1D capsule only simulations show the importance of applying a similar level of rigor to NLTE capsule ablator modeling. Taken together, these results show how improved target performance predictions can be achieved by performing inline atomic kinetics using more complete models for the underlying atomic structure and transitions. Prepared by LLNL under Contract DE-AC52-07NA27344.

The Intrinsic Ferromagnetism in a MnO2 Monolayer.

PubMed

Kan, M; Zhou, J; Sun, Q; Kawazoe, Y; Jena, P

2013-10-17

The Mn atom, because of its special electronic configuration of 3d(5)4s(2), has been widely used as a dopant in various two-dimensional (2D) monolayers such as graphene, BN, silicene and transition metal dichalcogenides (TMDs). The distributions of doped Mn atoms in these systems are highly sensitive to the synthesis process and conditions, thus suffering from problems of low solubility and surface clustering. Here we show for the first time that the MnO2 monolayer, synthetized 10 years ago, where Mn ions are individually held at specific sites, exhibits intrinsic ferromagnetism with a Curie temperature of 140 K, comparable to the highest TC value achieved experimentally for Mn-doped GaAs. The well-defined atomic configuration and the intrinsic ferromagnetism of the MnO2 monolayer suggest that it is superior to other magnetic monolayer materials.

Effects of configurational disorder on the elastic properties of icosahedral boron-rich alloys based on B{sub 6}O, B{sub 13}C{sub 2}, and B{sub 4}C, and their mixing thermodynamics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ektarawong, A., E-mail: anekt@ifm.liu.se; Hultman, L.; Birch, J.

The elastic properties of alloys between boron suboxide (B{sub 6}O) and boron carbide (B{sub 13}C{sub 2}), denoted by (B{sub 6}O){sub 1−x}(B{sub 13}C{sub 2}){sub x}, as well as boron carbide with variable carbon content, ranging from B{sub 13}C{sub 2} to B{sub 4}C are calculated from first-principles. Furthermore, the mixing thermodynamics of (B{sub 6}O){sub 1−x}(B{sub 13}C{sub 2}){sub x} is studied. A superatom-special quasirandom structure approach is used for modeling different atomic configurations, in which effects of configurational disorder between the carbide and suboxide structural units, as well as between boron and carbon atoms within the units, are taken into account. Elastic propertiesmore » calculations demonstrate that configurational disorder in B{sub 13}C{sub 2}, where a part of the C atoms in the CBC chains substitute for B atoms in the B{sub 12} icosahedra, drastically increase the Young’s and shear modulus, as compared to an atomically ordered state, B{sub 12}(CBC). These calculated elastic moduli of the disordered state are in excellent agreement with experiments. Configurational disorder between boron and carbon can also explain the experimentally observed almost constant elastic moduli of boron carbide as the carbon content is changed from B{sub 4}C to B{sub 13}C{sub 2}. The elastic moduli of the (B{sub 6}O){sub 1−x}(B{sub 13}C{sub 2}){sub x} system are also practically unchanged with composition if boron-carbon disorder is taken into account. By investigating the mixing thermodynamics of the alloys, in which the Gibbs free energy is determined within the mean-field approximation for the configurational entropy, we outline the pseudo-binary phase diagram of (B{sub 6}O){sub 1−x}(B{sub 13}C{sub 2}){sub x}. The phase diagram reveals the existence of a miscibility gap at all temperatures up to the melting point. Also, the coexistence of B{sub 6}O-rich as well as ordered or disordered B{sub 13}C{sub 2}-rich domains in the material prepared through equilibrium routes is predicted.« less

Intrinsic Folding Proclivities in Cyclic β-Peptide Building Blocks: Configuration and Heteroatom Effects Analyzed by Conformer-Selective Spectroscopy and Quantum Chemistry.

PubMed

Alauddin, Mohammad; Gloaguen, Eric; Brenner, Valérie; Tardivel, Benjamin; Mons, Michel; Zehnacker-Rentien, Anne; Declerck, Valérie; Aitken, David J

2015-11-09

This work describes the use of conformer-selective laser spectroscopy following supersonic expansion to probe the local folding proclivities of four-membered ring cyclic β-amino acid building blocks. Emphasis is placed on stereochemical effects as well as on the structural changes induced by the replacement of a carbon atom of the cycle by a nitrogen atom. The amide A IR spectra are obtained and interpreted with the help of quantum chemistry structure calculations. Results provide evidence that the building block with a trans-substituted cyclobutane ring has a predilection to form strong C8 hydrogen bonds. Nitrogen-atom substitution in the ring induces the formation of the hydrazino turn, with a related but distinct hydrogen-bonding network: the structure is best viewed as a bifurcated C8/C5 bond with the N heteroatom lone electron pair playing a significant acceptor role, which supports recent observations on the hydrazino turn structure in solution. Surprisingly, this study shows that the cis-substituted cyclobutane ring derivative also gives rise predominantly to a C8 hydrogen bond, although weaker than in the two former cases, a feature that is not often encountered for this building block. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Spectroscopic Non-LTE Modeling of Highly Charged Gold Plasma

NASA Astrophysics Data System (ADS)

Dasgupta, A.; Ouart, N. D.; Giuliani, J. L.; Obenschain, S. P.; Clark, R. W.; Aglitskiy, Y.

2013-10-01

An X-ray spectrometer is under development at the Naval Research Laboratory (NRL) to investigate emissions from gold targets irradiated by the NIKE KrF facility. This effort is in support of the indirect drive campaign on the National Ignition Facility (NIF). To analyze and interpret the NIKE experimental spectra, we are theoretically exploring line emissions from a gold plasma in the M-band, i.e., 1.5 to 3.5 keV. We employ a detailed Non-LTE atomic model for ions near Ni-like gold by including an adequate number of configurations to obtain spectroscopic details in this range. The atomic states are coupled both collisionally and radiatively, including all dominant atomic processes that have significant contributions to the ionization and emitted synthetic spectra. In particular, we will investigate the effect of dielectronic recombination, which can have a dominant effect on level populations for highly ionized high Z plasmas. Since the radiation field can affect level populations through photoionization and photoexcitation, our collisional-radiative model will include non-local radiation transport. The line shapes of the strong overlapping lines will be resolved by a multifrequency radiation transport method. Synthetic spectra with radiation transport, including resonant photo-pumping, will be generated for realistic densities and temperatures to compare with the NIKE data. Work supported by DOE/NNSA.

Computational study of configurational and vibrational contributions to the thermodynamics of substitutional alloys: The case of Ni3Al

NASA Astrophysics Data System (ADS)

Michelon, M. F.; Antonelli, A.

2010-03-01

We have developed a methodology to study the thermodynamics of order-disorder transformations in n -component substitutional alloys that combines nonequilibrium methods, which can efficiently compute free energies, with Monte Carlo simulations, in which configurational and vibrational degrees of freedom are simultaneously considered on an equal footing basis. Furthermore, with this methodology one can easily perform simulations in the canonical and in the isobaric-isothermal ensembles, which allow the investigation of the bulk volume effect. We have applied this methodology to calculate configurational and vibrational contributions to the entropy of the Ni3Al alloy as functions of temperature. The simulations show that when the volume of the system is kept constant, the vibrational entropy does not change upon transition while constant-pressure calculations indicate that the volume increase at the order-disorder transition causes a vibrational entropy increase of 0.08kB/atom . This is significant when compared to the configurational entropy increase of 0.27kB/atom . Our calculations also indicate that the inclusion of vibrations reduces in about 30% the order-disorder transition temperature determined solely considering the configurational degrees of freedom.

Short-wavelength out-of-band EUV emission from Sn laser-produced plasma

NASA Astrophysics Data System (ADS)

Torretti, F.; Schupp, R.; Kurilovich, D.; Bayerle, A.; Scheers, J.; Ubachs, W.; Hoekstra, R.; Versolato, O. O.

2018-02-01

We present the results of spectroscopic measurements in the extreme ultraviolet regime (7-17 nm) of molten tin microdroplets illuminated by a high-intensity 3 J, 60 ns Nd:YAG laser pulse. The strong 13.5 nm emission from this laser-produced plasma (LPP) is of relevance for next-generation nanolithography machines. Here, we focus on the shorter wavelength features between 7 and 12 nm which have so far remained poorly investigated despite their diagnostic relevance. Using flexible atomic code calculations and local thermodynamic equilibrium arguments, we show that the line features in this region of the spectrum can be explained by transitions from high-lying configurations within the Sn{}8+-Sn{}15+ ions. The dominant transitions for all ions but Sn{}8+ are found to be electric-dipole transitions towards the n = 4 ground state from the core-excited configuration in which a 4p electron is promoted to the 5s subshell. Our results resolve some long-standing spectroscopic issues and provide reliable charge state identification for Sn LPP, which could be employed as a useful tool for diagnostic purposes.

Experimental and numerical investigation on thermal fluid-structure interaction on ceramic plates in high enthalpy flow

NASA Astrophysics Data System (ADS)

Willems, Sebastian; Esser, Burkard; Gülhan, Ali

2015-12-01

A detailed knowledge of the fluid-structure interaction in hypersonic flows is important for the design of future space transportation systems. The thermal aspect of such an interaction was investigated with the help of a generic model in the arc-heated wind tunnel L3K at the German Aerospace Center in Cologne. Flat and curved panels of the fibre-reinforced ceramics C/C-SiC with and without anti-oxidation coating where used. Several configurations with and without back plane insulation were tested at 10° and 20° angle of attack. The panel heating was measured with an infrared camera, several thermocouples and pyrometers. The experimental results show the influence of the shape as well as of radiation cooling and radiation heating. The experiments also reveal the effect of additional heating due to recombination of atomic oxygen on the surface. At certain configurations a local temperature peak moved over the panel. This thermal wave is also influenced by the silicon carbide coating. The analysis is supported by coupled fluid and structure simulations.

Atomistic structures of nano-engineered SiC and radiation-induced amorphization resistance

NASA Astrophysics Data System (ADS)

Imada, Kenta; Ishimaru, Manabu; Sato, Kazuhisa; Xue, Haizhou; Zhang, Yanwen; Shannon, Steven; Weber, William J.

2015-10-01

Nano-engineered 3C-SiC thin films, which possess columnar structures with high-density stacking faults and twins, were irradiated with 2 MeV Si ions at cryogenic and room temperatures. From cross-sectional transmission electron microscopy observations in combination with Monte Carlo simulations based on the Stopping and Range of Ions in Matter code, it was found that their amorphization resistance is six times greater than bulk crystalline SiC at room temperature. High-angle bright-field images taken by spherical aberration corrected scanning transmission electron microscopy revealed that the distortion of atomic configurations is localized near the stacking faults. The resultant strain field probably contributes to the enhancement of radiation tolerance of this material.

Roman coloured and opaque glass: a chemical and spectroscopic study

NASA Astrophysics Data System (ADS)

Arletti, R.; Dalconi, M. C.; Quartieri, S.; Triscari, M.; Vezzalini, G.

2006-05-01

This work reports the results of an archaeometrical investigation of opaque Roman glass and is mainly focussed on the role of configuration and oxidation state of copper on the colour and opacity of red and green opaque finds (mosaic tesserae, game counters, and glass artefacts) from Sicily and Pompeii excavations. The glass fragments were characterised by EMPA, SEM-EDS, TEM, and XRPD analyses and the copper local environment was investigated using X-ray absorption spectroscopy. The analyses of high-resolution Cu-K edge XANES and EXAFS spectra suggest that, in red samples, copper is present as monovalent cations coordinated to the oxygen atoms of the glass framework, accompanied by metallic clusters. In green samples all the copper cations are incorporated in the glass matrix.

Soft X-ray spectroscopy of transition metal compounds: a theoretical perspective

NASA Astrophysics Data System (ADS)

Bokarev, S. I.; Hilal, R.; Aziz, S. G.; Kühn, O.

2017-01-01

To date, X-ray spectroscopy has become a routine tool that can reveal highly local and element-specific information on the electronic structure of atoms in complex environments. Here, we report on the development of an efficient and versatile theoretical methodology for the treatment of soft X-ray spectra of transition metal compounds based on the multi-configurational self-consistent field electronic structure theory. A special focus is put on the L-edge photon-in/photon-out and photon-in/electron-out processes, i.e. X-ray absorption, resonant inelastic scattering, partial fluorescence yield, and photoelectron spectroscopy, all treated on the same theoretical footing. The investigated systems range from small prototypical coordination compounds and catalysts to aggregates of biomolecules.

Hierarchical Multiscale Modeling of Macromolecules and their Assemblies

PubMed Central

Ortoleva, P.; Singharoy, A.; Pankavich, S.

2013-01-01

Soft materials (e.g., enveloped viruses, liposomes, membranes and supercooled liquids) simultaneously deform or display collective behaviors, while undergoing atomic scale vibrations and collisions. While the multiple space-time character of such systems often makes traditional molecular dynamics simulation impractical, a multiscale approach has been presented that allows for long-time simulation with atomic detail based on the co-evolution of slowly-varying order parameters (OPs) with the quasi-equilibrium probability density of atomic configurations. However, this approach breaks down when the structural change is extreme, or when nearest-neighbor connectivity of atoms is not maintained. In the current study, a self-consistent approach is presented wherein OPs and a reference structure co-evolve slowly to yield long-time simulation for dynamical soft-matter phenomena such as structural transitions and self-assembly. The development begins with the Liouville equation for N classical atoms and an ansatz on the form of the associated N-atom probability density. Multiscale techniques are used to derive Langevin equations for the coupled OP-configurational dynamics. The net result is a set of equations for the coupled stochastic dynamics of the OPs and centers of mass of the subsystems that constitute a soft material body. The theory is based on an all-atom methodology and an interatomic force field, and therefore enables calibration-free simulations of soft matter, such as macromolecular assemblies. PMID:23671457

Automatic selection of atomic fingerprints and reference configurations for machine-learning potentials

NASA Astrophysics Data System (ADS)

Imbalzano, Giulio; Anelli, Andrea; Giofré, Daniele; Klees, Sinja; Behler, Jörg; Ceriotti, Michele

2018-06-01

Machine learning of atomic-scale properties is revolutionizing molecular modeling, making it possible to evaluate inter-atomic potentials with first-principles accuracy, at a fraction of the costs. The accuracy, speed, and reliability of machine learning potentials, however, depend strongly on the way atomic configurations are represented, i.e., the choice of descriptors used as input for the machine learning method. The raw Cartesian coordinates are typically transformed in "fingerprints," or "symmetry functions," that are designed to encode, in addition to the structure, important properties of the potential energy surface like its invariances with respect to rotation, translation, and permutation of like atoms. Here we discuss automatic protocols to select a number of fingerprints out of a large pool of candidates, based on the correlations that are intrinsic to the training data. This procedure can greatly simplify the construction of neural network potentials that strike the best balance between accuracy and computational efficiency and has the potential to accelerate by orders of magnitude the evaluation of Gaussian approximation potentials based on the smooth overlap of atomic positions kernel. We present applications to the construction of neural network potentials for water and for an Al-Mg-Si alloy and to the prediction of the formation energies of small organic molecules using Gaussian process regression.

Atomic-Scale Origin of the Quasi-One-Dimensional Metallic Conductivity in Strontium Niobates with Perovskite-Related Layered Structures.

PubMed

Chen, Chunlin; Yin, Deqiang; Inoue, Kazutoshi; Lichtenberg, Frank; Ma, Xiuliang; Ikuhara, Yuichi; Bednorz, Johannes Georg

2017-12-26

The quasi-one-dimensional (1D) metallic conductivity of the perovskite-related Sr n Nb n O 3n+2 compounds is of continuing fundamental physical interest as well as being important for developing advanced electronic devices. The Sr n Nb n O 3n+2 compounds can be derived by introducing additional oxygen into the SrNbO 3 perovskite. However, the physical origin for the transition of electrical properties from the three-dimensional (3D) isotropic conductivity in SrNbO 3 to the quasi-1D metallic conductivity in Sr n Nb n O 3n+2 requires more in-depth clarification. Here we combine advanced transmission electron microscopy with atomistic first-principles calculations to unambiguously determine the atomic and electronic structures of the Sr n Nb n O 3n+2 compounds and reveal the underlying mechanism for their quasi-1D metallic conductivity. We demonstrate that the local electrical conductivity in the Sr n Nb n O 3n+2 compounds directly depends on the configuration of the NbO 6 octahedra in local regions. These findings will shed light on the realization of two-dimensional (2D) electrical conductivity from a bulk material, namely by segmenting a 3D conductor into a stack of 2D conducting thin layers.

Electrostatics of proteins in dielectric solvent continua. I. Newton's third law marries qE forces

NASA Astrophysics Data System (ADS)

Stork, Martina; Tavan, Paul

2007-04-01

The authors reformulate and revise an electrostatic theory treating proteins surrounded by dielectric solvent continua [B. Egwolf and P. Tavan, J. Chem. Phys. 118, 2039 (2003)] to make the resulting reaction field (RF) forces compatible with Newton's third law. Such a compatibility is required for their use in molecular dynamics (MD) simulations, in which the proteins are modeled by all-atom molecular mechanics force fields. According to the original theory the RF forces, which are due to the electric field generated by the solvent polarization and act on the partial charges of a protein, i.e., the so-called qE forces, can be quite accurately computed from Gaussian RF dipoles localized at the protein atoms. Using a slightly different approximation scheme also the RF energies of given protein configurations are obtained. However, because the qE forces do not account for the dielectric boundary pressure exerted by the solvent continuum on the protein, they do not obey the principle that actio equals reactio as required by Newton's third law. Therefore, their use in MD simulations is severely hampered. An analysis of the original theory has led the authors now to a reformulation removing the main difficulties. By considering the RF energy, which represents the dominant electrostatic contribution to the free energy of solvation for a given protein configuration, they show that its negative configurational gradient yields mean RF forces obeying the reactio principle. Because the evaluation of these mean forces is computationally much more demanding than that of the qE forces, they derive a suggestion how the qE forces can be modified to obey Newton's third law. Various properties of the thus established theory, particularly issues of accuracy and of computational efficiency, are discussed. A sample application to a MD simulation of a peptide in solution is described in the following paper [M. Stork and P. Tavan, J. Chem. Phys., 126, 165106 (2007).

Correspondence: Reply to ‘Phantom phonon localization in relaxors’

DOE PAGES

Manley, Michael E.; Abernathy, Douglas L.; Budai, John D.

2017-12-05

The Correspondence by Gehring et al. mistakes Anderson phonon localization for the concept of an atomic-scale local mode. An atomic-scale local mode refers to a single atom vibrating on its own within a crystal. Such a local mode will have an almost flat intensity profile, but this is not the same as phonon localization. Anderson localization is a wave interference effect in a disordered system that results in waves becoming spatially localized. The length scale of the localized waves is set by the wavelength, which is approximately 2 nm in this case. This larger length scale in real space meansmore » narrower intensity profiles in reciprocal space. Here, we conclude that the claims in the Correspondence by Gehring et al. are incorrect because they mistakenly assume that the length scale for Anderson localization is atomic, and because the experimental observations rule out multiple scattering as the origin.« less

Correspondence: Reply to ‘Phantom phonon localization in relaxors’

DOE Office of Scientific and Technical Information (OSTI.GOV)

Manley, Michael E.; Abernathy, Douglas L.; Budai, John D.

The Correspondence by Gehring et al. mistakes Anderson phonon localization for the concept of an atomic-scale local mode. An atomic-scale local mode refers to a single atom vibrating on its own within a crystal. Such a local mode will have an almost flat intensity profile, but this is not the same as phonon localization. Anderson localization is a wave interference effect in a disordered system that results in waves becoming spatially localized. The length scale of the localized waves is set by the wavelength, which is approximately 2 nm in this case. This larger length scale in real space meansmore » narrower intensity profiles in reciprocal space. Here, we conclude that the claims in the Correspondence by Gehring et al. are incorrect because they mistakenly assume that the length scale for Anderson localization is atomic, and because the experimental observations rule out multiple scattering as the origin.« less

Metallic nanoparticle-based strain sensors elaborated by atomic layer deposition

NASA Astrophysics Data System (ADS)

Puyoo, E.; Malhaire, C.; Thomas, D.; Rafaël, R.; R'Mili, M.; Malchère, A.; Roiban, L.; Koneti, S.; Bugnet, M.; Sabac, A.; Le Berre, M.

2017-03-01

Platinum nanoparticle-based strain gauges are elaborated by means of atomic layer deposition on flexible polyimide substrates. Their electro-mechanical response is tested under mechanical bending in both buckling and conformational contact configurations. A maximum gauge factor of 70 is reached at a strain level of 0.5%. Although the exponential dependence of the gauge resistance on strain is attributed to the tunneling effect, it is shown that the majority of the junctions between adjacent Pt nanoparticles are in a short circuit state. Finally, we demonstrate the feasibility of an all-plastic pressure sensor integrating Pt nanoparticle-based strain gauges in a Wheatstone bridge configuration.

Electromagnetically-induced-absorption resonance with high contrast and narrow width in the Hanle configuration

NASA Astrophysics Data System (ADS)

Brazhnikov, D. V.; Taichenachev, A. V.; Tumaikin, A. M.; Yudin, V. I.

2014-12-01

The method for observing the high-contrast and narrow-width resonances of electromagnetically induced absorption (EIA) in the Hanle configuration under counter-propagating pump and probe light waves is proposed. Here, as an example, we study a ‘dark’ type of atomic dipole transition {{F}\\text{g}}={1}\\to {{F}\\text{e}}={1} in D1 line of 87Rb, where usually the electromagnetically induced transparency can be observed. To obtain the EIA signal one should properly choose the polarizations of light waves and intensities. In contrast to regular schemes for observing EIA signals (under a single traveling light wave in the Hanle configuration or under a bichromatic light field consisting of two traveling waves), the proposed scheme allows one to use buffer gas for significantly improving the properties of the resonance. Also the dramatic influence of atomic transition openness on the contrast of the resonance is revealed, which is advantageous in comparison with cyclic atomic transitions. The nonlinear resonances in a probe-wave transmitted signal with contrast close to 100% and sub-kHz widths can be obtained. The results are interesting in high-resolution spectroscopy, nonlinear and magneto-optics.

Density functional study of H2O molecule adsorption on α-U(001) surface.

PubMed

Huang, Shanqisong; Zeng, Xiu-Lin; Zhao, Feng-Qi; Ju, Xuehai

2016-04-01

Periodic density functional theory (DFT) calculations were performed to investigate the adsorption of H2O on U(001) surface. The metallic nature of uranium atom and different adsorption sites of U(001) surface play key roles in the H2O molecular dissociate reaction. The long-bridge site is the most favorable site of H2O-U(001) adsorption configuration. The triangle-center site of the H atom is the most favorable site of HOH-U(001) adsorption configuration. The interaction between H2O and U surface is more evident on the first layer than that on any other two sub-layers. The dissociation energy of one hydrogen atom from H2O is -1.994 to -2.215 eV on U(001) surface, while the dissociating energy decreases to -3.351 to -3.394 eV with two hydrogen atoms dissociating from H2O. These phenomena also indicate that the Oads can promote the dehydrogenation of H2O. A significant charge transfer from the first layer of the uranium surface to the H and O atoms is also found to occur, making the bonding partly ionic.

Interactions of atomic hydrogen with amorphous SiO2

NASA Astrophysics Data System (ADS)

Yue, Yunliang; Wang, Jianwei; Zhang, Yuqi; Song, Yu; Zuo, Xu

2018-03-01

Dozens of models are investigated by the first-principles calculations to simulate the interactions of an atomic hydrogen with a defect-free random network of amorphous SiO2 (a-SiO2) and oxygen vacancies. A wide variety of stable configurations are discovered due to the disorder of a-SiO2, and their structures, charges, magnetic moments, spin densities, and density of states are calculated. The atomic hydrogen interacts with the defect-free a-SiO2 in positively or negatively charged state, and produces the structures absent in crystalline SiO2. It passivates the neutral oxygen vacancies and generates two neutral hydrogenated E‧ centers with different Si dangling bond projections. Electron spin resonance parameters, including Fermi contacts, and g-tensors, are calculated for these centers. The atomic hydrogen interacts with the positive oxygen vacancies in dimer configuration, and generate four different positive hydrogenated defects, two of which are puckered like the Eγ‧ centers. This research helps to understand the interactions between an atomic hydrogen, and defect-free a-SiO2 and oxygen vacancies, which may generate the hydrogen-complexed defects that play a key role in the degeneration of silicon/silica-based microelectronic devices.

Transition metal decorated graphene-like zinc oxide monolayer: A first-principles investigation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lei, Jie; School of Science, Qilu University of Technology, Jinan, Shandong 250353; Xu, Ming-Chun

Transition metal (TM) atoms have been extensively employed to decorate the two-dimensional materials, endowing them with promising physical properties. Here, we have studied the adsorption of TM atoms (V, Cr, Mn, Fe, and Co) on graphene-like zinc oxide monolayer (g-ZnO) and the substitution of Zn by TM using first-principles calculations to search for the most likely configurations when TM atoms are deposited on g-ZnO. We found that when a V atom is initially placed on the top of Zn atom, V will squeeze out Zn from the two-dimensional plane then substitute it, which is a no barrier substitution process. Formore » heavier elements (Cr to Co), although the substitution configurations are more stable than the adsorption ones, there is an energy barrier for the adsorption-substitution transition with the height of tens to hundreds meV. Therefore, Cr to Co prefers to be adsorbed on the hollow site or the top of oxygen, which is further verified by the molecular dynamics simulations. The decoration of TM is revealed to be a promising approach in terms of tuning the work function of g-ZnO in a large energy range.« less

Transition metal decorated graphene-like zinc oxide monolayer: A first-principles investigation

NASA Astrophysics Data System (ADS)

Lei, Jie; Xu, Ming-Chun; Hu, Shu-Jun

2015-09-01

Transition metal (TM) atoms have been extensively employed to decorate the two-dimensional materials, endowing them with promising physical properties. Here, we have studied the adsorption of TM atoms (V, Cr, Mn, Fe, and Co) on graphene-like zinc oxide monolayer (g-ZnO) and the substitution of Zn by TM using first-principles calculations to search for the most likely configurations when TM atoms are deposited on g-ZnO. We found that when a V atom is initially placed on the top of Zn atom, V will squeeze out Zn from the two-dimensional plane then substitute it, which is a no barrier substitution process. For heavier elements (Cr to Co), although the substitution configurations are more stable than the adsorption ones, there is an energy barrier for the adsorption-substitution transition with the height of tens to hundreds meV. Therefore, Cr to Co prefers to be adsorbed on the hollow site or the top of oxygen, which is further verified by the molecular dynamics simulations. The decoration of TM is revealed to be a promising approach in terms of tuning the work function of g-ZnO in a large energy range.

Friction of atomically stepped surfaces

NASA Astrophysics Data System (ADS)

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

2017-03-01

The friction behavior of atomically stepped metal surfaces under contact loading is studied using molecular dynamics simulations. While real rough metal surfaces involve roughness at multiple length scales, the focus of this paper is on understanding friction of the smallest scale of roughness: atomic steps. To this end, periodic stepped Al surfaces with different step geometry are brought into contact and sheared at room temperature. Contact stress that continuously tries to build up during loading, is released with fluctuating stress drops during sliding, according to the typical stick-slip behavior. Stress release occurs not only through local slip, but also by means of step motion. The steps move along the contact, concurrently resulting in normal migration of the contact. The direction of migration depends on the sign of the step, i.e., its orientation with respect to the shearing direction. If the steps are of equal sign, there is a net migration of the entire contact accompanied by significant vacancy generation at room temperature. The stick-slip behavior of the stepped contacts is found to have all the characteristic of a self-organized critical state, with statistics dictated by step density. For the studied step geometries, frictional sliding is found to involve significant atomic rearrangement through which the contact roughness is drastically changed. This leads for certain step configurations to a marked transition from jerky sliding motion to smooth sliding, making the final friction stress approximately similar to that of a flat contact.

Atomic-scale dynamics of a model glass-forming metallic liquid: Dynamical crossover, dynamical decoupling, and dynamical clustering

DOE PAGES

Jaiswal, Abhishek; Egami, Takeshi; Zhang, Yang

2015-04-01

The phase behavior of multi-component metallic liquids is exceedingly complex because of the convoluted many-body and many-elemental interactions. Herein, we present systematic studies of the dynamic aspects of such a model ternary metallic liquid Cu 40Zr 51Al 9 using molecular dynamics simulation with embedded atom method. We observed a dynamical crossover from Arrhenius to super-Arrhenius behavior in the transport properties (diffusion coefficient, relaxation times, and shear viscosity) bordered at T x ~1300K. Unlike in many molecular and macromolecular liquids, this crossover phenomenon occurs in the equilibrium liquid state well above the melting temperature of the system (T m ~ 900K),more » and the crossover temperature is roughly twice of the glass-transition temperature (T g). Below T x, we found the elemental dynamics decoupled and the Stokes-Einstein relation broke down, indicating the onset of heterogeneous spatially correlated dynamics in the system mediated by dynamic communications among local configurational excitations. To directly characterize and visualize the correlated dynamics, we employed a non-parametric, unsupervised machine learning technique and identified dynamical clusters of atoms with similar atomic mobility. The revealed average dynamical cluster size shows an accelerated increase below T x and mimics the trend observed in other ensemble averaged quantities that are commonly used to quantify the spatially heterogeneous dynamics such as the non-Gaussian parameter and the four-point correlation function.« less

Convex central configurations for the n-body problem

NASA Astrophysics Data System (ADS)

Xia, Zhihong

We give a simple proof of a classical result of MacMillan and Bartky (Trans. Amer. Math. Soc. 34 (1932) 838) which states that, for any four positive masses and any assigned order, there is a convex planar central configuration. Moreover, we show that the central configurations we find correspond to local minima of the potential function with fixed moment of inertia. This allows us to show that there are at least six local minimum central configurations for the planar four-body problem. We also show that for any assigned order of five masses, there is at least one convex spatial central configuration of local minimum type. Our method also applies to some other cases.

A nanoscale study of charge extraction in organic solar cells: the impact of interfacial molecular configurations.

PubMed

Tang, Fu-Ching; Wu, Fu-Chiao; Yen, Chia-Te; Chang, Jay; Chou, Wei-Yang; Gilbert Chang, Shih-Hui; Cheng, Horng-Long

2015-01-07

In the optimization of organic solar cells (OSCs), a key problem lies in the maximization of charge carriers from the active layer to the electrodes. Hence, this study focused on the interfacial molecular configurations in efficient OSC charge extraction by theoretical investigations and experiments, including small molecule-based bilayer-heterojunction (sm-BLHJ) and polymer-based bulk-heterojunction (p-BHJ) OSCs. We first examined a well-defined sm-BLHJ model system of OSC composed of p-type pentacene, an n-type perylene derivative, and a nanogroove-structured poly(3,4-ethylenedioxythiophene) (NS-PEDOT) hole extraction layer. The OSC with NS-PEDOT shows a 230% increment in the short circuit current density compared with that of the conventional planar PEDOT layer. Our theoretical calculations indicated that small variations in the microscopic intermolecular interaction among these interfacial configurations could induce significant differences in charge extraction efficiency. Experimentally, different interfacial configurations were generated between the photo-active layer and the nanostructured charge extraction layer with periodic nanogroove structures. In addition to pentacene, poly(3-hexylthiophene), the most commonly used electron-donor material system in p-BHJ OSCs was also explored in terms of its possible use as a photo-active layer. Local conductive atomic force microscopy was used to measure the nanoscale charge extraction efficiency at different locations within the nanogroove, thus highlighting the importance of interfacial molecular configurations in efficient charge extraction. This study enriches understanding regarding the optimization of the photovoltaic properties of several types of OSCs by conducting appropriate interfacial engineering based on organic/polymer molecular orientations. The ultimate power conversion efficiency beyond at least 15% is highly expected when the best state-of-the-art p-BHJ OSCs are combined with present arguments.

A Review on Resistive Switching in High-k Dielectrics: A Nanoscale Point of View Using Conductive Atomic Force Microscope

PubMed Central

Lanza, Mario

2014-01-01

Metal-Insulator-Metal (MIM) structures have raised as the most promising configuration for next generation information storage, leading to great performance and fabrication-friendly Resistive Random Access Memories (RRAM). In these cells, the memory concept is no more based on the charge storage, but on tuning the electrical resistance of the insulating layer by applying electrical stresses to reach a high resistive state (HRS or “0”) and a low resistive state (LRS or “1”), which makes the memory point. Some high-k dielectrics show this unusual property and in the last years high-k based RRAM have been extensively analyzed, especially at the device level. However, as resistance switching (in the most promising cells) is a local phenomenon that takes place in areas of ~100 nm2, the use of characterization tools with high lateral spatial resolution is necessary. In this paper the status of resistive switching in high-k materials is reviewed from a nanoscale point of view by means of conductive atomic force microscope analyses. PMID:28788561

Effect of intermixing at CdS/CdTe interface on defect properties

NASA Astrophysics Data System (ADS)

Park, Ji-Sang; Yang, Ji-Hui; Barnes, Teresa; Wei, Su-Huai

2016-07-01

We investigated the stability and electronic properties of defects in CdTe1-xSx that can be formed at the CdS/CdTe interface. As the anions mix at the interface, the defect properties are significantly affected, especially those defects centered at cation sites like Cd vacancy, VCd, and Te on Cd antisite, TeCd, because the environment surrounding the defect sites can have different configurations. We show that at a given composition, the transition energy levels of VCd and TeCd become close to the valence band maximum when the defect has more S atoms in their local environment, thus improving the device performance. Such beneficial role is also found at the grain boundaries when the Te atom is replaced by S in the Te-Te wrong bonds, reducing the energy of the grain boundary level. On the other hand, the transition levels with respect to the valence band edge of CdTe1-xSx increases with the S concentration as the valence band edge decreases with the S concentration, resulting in the reduced p-type doping efficiency.

Modeling Aggregation Processes of Lennard-Jones particles Via Stochastic Networks

NASA Astrophysics Data System (ADS)

Forman, Yakir; Cameron, Maria

2017-07-01

We model an isothermal aggregation process of particles/atoms interacting according to the Lennard-Jones pair potential by mapping the energy landscapes of each cluster size N onto stochastic networks, computing transition probabilities from the network for an N-particle cluster to the one for N+1, and connecting these networks into a single joint network. The attachment rate is a control parameter. The resulting network representing the aggregation of up to 14 particles contains 6427 vertices. It is not only time-irreversible but also reducible. To analyze its transient dynamics, we introduce the sequence of the expected initial and pre-attachment distributions and compute them for a wide range of attachment rates and three values of temperature. As a result, we find the configurations most likely to be observed in the process of aggregation for each cluster size. We examine the attachment process and conduct a structural analysis of the sets of local energy minima for every cluster size. We show that both processes taking place in the network, attachment and relaxation, lead to the dominance of icosahedral packing in small (up to 14 atom) clusters.

Relativistic opacities for astrophysical applications

DOE PAGES

Fontes, Christopher John; Fryer, Christopher Lee; Hungerford, Aimee L.; ...

2015-06-29

Here, we report on the use of the Los Alamos suite of relativistic atomic physics codes to generate radiative opacities for the modeling of astrophysically relevant plasmas under local thermodynamic equilibrium (LTE) conditions. The atomic structure calculations are carried out in fine-structure detail, including full configuration interaction. Three example applications are considered: iron opacities at conditions relevant to the base of the solar convection zone, nickel opacities for the modeling of stellar envelopes, and samarium opacities for the modeling of light curves produced by neutron star mergers. In the first two examples, comparisons are made between opacities that are generatedmore » with the fully and semi-relativistic capabilities in the Los Alamos suite of codes. As expected for these highly charged, iron-peak ions, the two methods produce reasonably similar results, providing confidence that the numerical methods have been correctly implemented. However, discrepancies greater than 10% are observed for nickel and investigated in detail. In the final application, the relativistic capability is used in a preliminary investigation of the complicated absorption spectrum associated with cold lanthanide elements.« less

Sterically allowed configuration space for amino acid dipeptides

NASA Astrophysics Data System (ADS)

Caballero, Diego; Maatta, Jukka; Sammalkorpi, Maria; O'Hern, Corey; Regan, Lynne

2014-03-01

Despite recent improvements in computational methods for protein design, we still lack a quantitative, predictive understanding of the intrinsic propensities for amino acids to be in particular backbone or side-chain conformations. This question has remained unsettled for years because of the discrepancies between different experimental approaches. To address it, I performed all-atom hard-sphere simulations of hydrophobic residues with stereo-chemical constraints and non-attractive steric interactions between non-bonded atoms for ALA, ILE, LEU and VAL dipeptide mimetics. For these hard-sphere MD simulations, I show that transitions between α-helix and β-sheet structures only occur when the bond angle τ(N -Cα - C) >110° , and the probability distribution of bond angles for structures in the `bridge' region of ϕ- ψ space is shifted to larger angles compared to that in other regions. In contrast, the relevant bond-angle distributions obtained from most molecular dynamics packages are broader and shifter to larger values. I encounter similar correlations between bond angles and side-chain dihedral angles. The success of these studies is an argument for re-incorporating local stereochemical constraints into computational protein design methodology.

Phospholipid dynamics in graphene of different topologies: predictive modeling

NASA Astrophysics Data System (ADS)

Glukhova, O. E.; Slepchenkov, M. M.

2017-02-01

The subject of our scientific interest is the dynamics of the phospholipid molecules into a corrugated graphene sheet. According to our assumption by changing the topology of graphene properly it is possible to find the ways for management of the selective localization of phospholipid molecules to form the desired configuration of these structures. We considered DPPC (dipalmitoylphosphatidylcholine) phospholipids, which are the part of cell membranes and lipoproteins. We investigated the behavior of the phospholipids on the graphene sheet consisting of 1710 atoms with the size of 6.9 nm along the zigzag edge and 6.25 nm along the armchair edge. The numerical experiment was carried out using the original AMBER/AIREBO hybrid method with Lennard-Jones potential to describe the interaction between unbound atoms of different structures. The temperature was maintained at 300 K during the numerical experiment. All numerical experiments were performed using KVAZAR software system. We considered several cases of corrugated graphene with different width and dept of the corrugation. Special attention in our work was paid to the orientation of the phospholipids in the plane of graphene sheet.

Electrically-inactive phosphorus re-distribution during low temperature annealing

NASA Astrophysics Data System (ADS)

Peral, Ana; Youssef, Amanda; Dastgheib-Shirazi, Amir; Akey, Austin; Peters, Ian Marius; Hahn, Giso; Buonassisi, Tonio; del Cañizo, Carlos

2018-04-01

An increased total dose of phosphorus (P dose) in the first 40 nm of a phosphorus diffused emitter has been measured after Low Temperature Annealing (LTA) at 700 °C using the Glow Discharge Optical Emission Spectrometry technique. This evidence has been observed in three versions of the same emitter containing different amounts of initial phosphorus. A stepwise chemical etching of a diffused phosphorus emitter has been carried out to prepare the three types of samples. The total P dose in the first 40 nm increases during annealing by 1.4 × 1015 cm-2 for the sample with the highly doped emitter, by 0.8 × 1015 cm-2 in the middle-doped emitter, and by 0.5 × 1015 cm-2 in the lowest-doped emitter. The presence of surface dislocations in the first few nanometers of the phosphorus emitter might play a role as preferential sites of local phosphorus gettering in phosphorus re-distribution, because the phosphorus gettering to the first 40 nm is lower when this region is etched stepwise. This total increase in phosphorus takes place even though the calculated electrically active phosphorus concentration shows a reduction, and the measured sheet resistance shows an increase after annealing at a low temperature. The reduced electrically active P dose is around 0.6 × 1015 cm-2 for all the emitters. This can be explained with phosphorus-atoms diffusing towards the surface during annealing, occupying electrically inactive configurations. An atomic-scale visual local analysis is carried out with needle-shaped samples of tens of nm in diameter containing a region of the highly doped emitter before and after LTA using Atom Probe Tomography, showing phosphorus precipitates of 10 nm and less before annealing and an increased density of larger precipitates after annealing (25 nm and less).

Structural, electronic and vibrational properties of GexCy (x+y=2-5) nanoclusters: A B3LYP-DFT study

NASA Astrophysics Data System (ADS)

Goswami, Sohini; Saha, Sushmita; Yadav, R. K.

2015-11-01

An ab-initio study of the stability, structural and electronic properties has been made for 84 germanium carbide nanoclusters, GexCy (x+y=2-5). The configuration possessing the maximum value of final binding energy (FBE), among the various configurations corresponding to a fixed x+y=n value, is named as the most stable structure. The vibrational and optical properties have been investigated only for the most stable structures. A B3LYP-DFT/6-311G(3df) method has been employed to optimize fully the geometries of the nanoclusters. The binding energies (BE), highest-occupied and lowest-unoccupied molecular orbital (HOMO-LUMO) gaps have been obtained for all the clusters and the bond lengths have been reported for the most stable clusters. We have considered the zero point energy (ZPE) corrections. The adiabatic and vertical ionization potentials (IPs) and electron affinities (EAs), charge on atoms, dipole moments, vibrational frequencies, infrared intensities (IR Int.), relative infrared intensities (Rel. IR Int.) and Raman scattering activities have also been investigated for the most stable structures. The configurations containing the carbon atoms in majority are seen to be the most stable structures. The strong C-C bond has important role in stabilizing the clusters. For the clusters containing one germanium atom and all the other as carbon atoms, the BE increases monotonically with the number of the carbon atoms. The HOMO-LUMO gap, IPs and EAs fluctuates with increase in the number of atoms. The nanoclusters containing even number of carbon atoms have large HOMO-LUMO gaps and IPs, whereas the nanoclusters containing even number of carbon atoms have small EAs. In general, the adiabatic IP (EA) is smaller (greater) than the vertical IP (EA). The optical absorption spectrum or electron energy loss spectrum (EELS) is unique for every cluster, and may be used to characterize a specific cluster. All the predicted physical quantities are in good agreement with the experimental data wherever available. The growth of these most stable structures should be possible in the experiments.

Multireference configuration interaction calculations of the first six ionization potentials of the uranium atom

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bross, David H.; Parmar, Payal; Peterson, Kirk A., E-mail: kipeters@wsu.edu

The first 6 ionization potentials (IPs) of the uranium atom have been calculated using multireference configuration interaction (MRCI+Q) with extrapolations to the complete basis set limit using new all-electron correlation consistent basis sets. The latter was carried out with the third-order Douglas-Kroll-Hess Hamiltonian. Correlation down through the 5s5p5d electrons has been taken into account, as well as contributions to the IPs due to the Lamb shift. Spin-orbit coupling contributions calculated at the 4-component Kramers restricted configuration interaction level, as well as the Gaunt term computed at the Dirac-Hartree-Fock level, were added to the best scalar relativistic results. The final ionizationmore » potentials are expected to be accurate to at least 5 kcal/mol (0.2 eV) and thus more reliable than the current experimental values of IP{sub 3} through IP{sub 6}.« less

An orbital localization criterion based on the theory of "fuzzy" atoms.

PubMed

Alcoba, Diego R; Lain, Luis; Torre, Alicia; Bochicchio, Roberto C

2006-04-15

This work proposes a new procedure for localizing molecular and natural orbitals. The localization criterion presented here is based on the partitioning of the overlap matrix into atomic contributions within the theory of "fuzzy" atoms. Our approach has several advantages over other schemes: it is computationally inexpensive, preserves the sigma/pi-separability in planar systems and provides a straightforward interpretation of the resulting orbitals in terms of their localization indices and atomic occupancies. The corresponding algorithm has been implemented and its efficiency tested on selected molecular systems. (c) 2006 Wiley Periodicals, Inc.

Opacity of iron, nickel, and copper plasmas in the x-ray wavelength range: Theoretical interpretation of 2p-3d absorption spectra

DOE Office of Scientific and Technical Information (OSTI.GOV)

Blenski, T.; Loisel, G.; Poirier, M.

2011-09-15

This paper deals with theoretical studies on the 2p-3d absorption in iron, nickel, and copper plasmas related to LULI2000 (Laboratoire pour l'Utilisation des Lasers Intenses, 2000J facility) measurements in which target temperatures were of the order of 20 eV and plasma densities were in the range 0.004-0.01 g/cm{sup 3}. The radiatively heated targets were close to local thermodynamic equilibrium (LTE). The structure of 2p-3d transitions has been studied with the help of the statistical superconfiguration opacity code sco and with the fine-structure atomic physics codes hullac and fac. A new mixed version of the sco code allowing one to treatmore » part of the configurations by detailed calculation based on the Cowan's code rcg has been also used in these comparisons. Special attention was paid to comparisons between theory and experiment concerning the term features which cannot be reproduced by sco. The differences in the spin-orbit splitting and the statistical (thermal) broadening of the 2p-3d transitions have been investigated as a function of the atomic number Z. It appears that at the conditions of the experiment the role of the term and configuration broadening was different in the three analyzed elements, this broadening being sensitive to the atomic number. Some effects of the temperature gradients and possible non-LTE effects have been studied with the help of the radiative-collisional code scric. The sensitivity of the 2p-3d structures with respect to temperature and density in medium-Z plasmas may be helpful for diagnostics of LTE plasmas especially in future experiments on the {Delta}n=0 absorption in medium-Z plasmas for astrophysical applications.« less

A half-metallic half-Heusler alloy having the largest atomic-like magnetic moment at optimized lattice constant

DOE PAGES

Zhang, R. L.; Damewood, L.; Fong, C. Y.; ...

2016-11-02

For half-Heusler alloys, the general formula is XYZ, where X can be a transition or alkali metal element, Y is another transition metal element, typically Mn or Cr, and Z is a group IV element or a pnicitide. The atomic arrangements within a unit-cell show three configurations. Before this study, most of the predictions of half-metallic properties of half-Heusler alloys at the lattice constants differing from their optimized lattice constant. Based on the electropositivity of X and electronegativity of Z for half-Heusler alloys, we found that one of the configurations of LiCrS exhibits half-metallic properties at its optimized lattice constantmore » of 5.803Å, and has the maximum atomic-like magnetic moment of 5μ B. In conclusion, the challenges of its growth and the effects of the spin-orbit effect in this alloy will be discussed.« less

A study of QM/Langevin-MD simulation for oxygen-evolving center of photosystem II

DOE Office of Scientific and Technical Information (OSTI.GOV)

Uchida, Waka; Kimura, Yoshiro; Wakabayashi, Masamitsu

2013-12-10

We have performed three QM/Langevin-MD simulations for oxygen-evolving complex (OEC) and surrounding residues, which are different configurations of the oxidation numbers on Mn atoms in the Mn{sub 4}O{sub 5}Ca cluster. By analyzing these trajectories, we have observed sensitivity of the change to the configuration of Mn oxidation state on O atoms of carboxyl on three amino acids, Glu354, Ala344, and Glu333. The distances from Mn to O atoms in residues contacting with the Mn{sub 4}O{sub 5}Ca cluster were analyzed for the three trajectories. We found the good correlation of the distances among the simulations. However, the distances with Glu354, Ala344,more » and Glu333 have not shown the correlation. These residues can be sensitive index of the changes of Mn oxidation numbers.« less

Transmission Magnitude and Phase Control for Polarization-Preserving Reflectionless Metasurfaces

NASA Astrophysics Data System (ADS)

Kwon, Do-Hoon; Ptitcyn, Grigorii; Díaz-Rubio, Ana; Tretyakov, Sergei A.

2018-03-01

For transmissive applications of electromagnetic metasurfaces, an array of subwavelength Huygens' meta-atoms are typically used to eliminate reflection and achieve a high-transmission power efficiency together with a wide transmission phase coverage. We show that the underlying principle of low reflection and full control over transmission is asymmetric scattering into the specular reflection and transmission directions that results from a superposition of symmetric and antisymmetric scattering components, with Huygens' meta-atoms being one example configuration. Available for oblique illumination in TM polarization, a meta-atom configuration comprising normal and tangential electric polarizations is presented, which is capable of reflectionless, full-power transmission and a 2 π transmission phase coverage as well as full absorption. For lossy metasurfaces, we show that a complete phase coverage is still available for reflectionless designs for any value of absorptance. Numerical examples in the microwave and optical regimes are provided.

Local bonding structure of tellurium and antimony in the phase change chalcogenides germanium-antimony-tellurium: A nuclear magnetic resonance study

NASA Astrophysics Data System (ADS)

Bobela, David C.

Recent technological applications of some chalcogenide materials, compounds containing a group VI atom, have prompted studies of the local atomic structure of the amorphous phase. In the case of Ge2Sb2Te 5, metastability in the local bonding structure is responsible for its usefulness as a phase-change memory material. There is no consensus on the exact phase-change mechanism, which is partly due to the inadequacy of standard scattering techniques to probe the structure of the amorphous phase. Nuclear magnetic resonance methods, on the other hand, are well suited to study local structural order even in the absence of a periodic lattice. In this technique, structural information is encoded as an oscillating voltage caused by the nuclear spin. For the tellurium isotope, 125Te (spin = 1/2 in the ground state), the dominant interaction comes from the core and valence electrons that carry angular momentum. This interaction is helpful in identifying Te sites of different local coordination since the number of neighboring atoms should markedly change the local electronic structure. The antimony isotope 125Sb has a spin = 5/2 in the ground state and possesses an asymmetric nuclear charge. This quadrupole moment will interact with an electric field gradient at the nuclear site, which is provided by an asymmetric electron cloud surrounding the nucleus. The frequency-space spectra will reflect the strength of the interaction as well as the symmetry of the local electronic environment. This work investigates the nuclear magnetic resonance spectrum of 125Te and 125Sb in the crystalline and amorphous forms of several GexSbyTe 1-x-y compounds where 0 < (x, y) < 1. Results from the crystalline phase 125Te data show a trend in the spectral position that can be related to the tellurium bonded to three and six neighbors. In the amorphous phase, the same trend is observed, and the nuclear magnetic resonance fingerprint of two-fold and three-fold coordinated tellurium is obtained. It is concluded, based upon this comparison that the Te atoms see a dramatically different bonding environment depending on which phase the lattice has. The 125Sb data for the crystalline phase indicate electric field gradients that are consistent with similarly bonded quadrupolar nuclei, such as Sb atoms in crystalline Sb or five-fold coordinated Sb in crystalline MnSb. The NMR data exemplify the consequences of combinatorial disorder on the spectra via the absence of certain line-shape features. In the amorphous phase, the electric field gradients are approximately seven times larger, and the fingerprints of both highly-symmetric and asymmetric antimony sites emerge. Details of field gradient, i.e. the magnitude and symmetry, are remarkably similar to those found in Sb containing compounds where the Sb sites are three-fold pyramidal, such as in crystalline Sb2X3 where X = O, S, or Se. The observations from the NMR data provide a critical litmus test for recent structural models of the amorphous phase. In particular, the amorphous phase data provides clear evidence that the Te atoms are two-fold and three-fold coordinated while the Sb atoms are most likely bonded in three-fold pyramidal configurations. These observations imply a structural model of the amorphous phase that agrees best with a models based upon the "8 minus n", or "8-n" rule for chemical bonding in amorphous semiconductors. Thus, the lattice of these compounds is arranged such that the constituent elements have enough bonds, on average, to satisfy their valence requirement. The implications of the NMR data on theoretical modeling data are immediate. Theoretical models of these systems must possess some aspect of the "8-n" mentality. With this idea as a foundation for physically realistic representations of the amorphous phase, the origin of the phase-change mechanism may be unraveled, which will ultimately speed the process of compositional optimization of phase-change materials.

Local lattice distortion in high-entropy alloys

NASA Astrophysics Data System (ADS)

Song, Hongquan; Tian, Fuyang; Hu, Qing-Miao; Vitos, Levente; Wang, Yandong; Shen, Jiang; Chen, Nanxian

2017-07-01

The severe local lattice distortion, induced mainly by the large atomic size mismatch of the alloy components, is one of the four core effects responsible for the unprecedented mechanical behaviors of high-entropy alloys (HEAs). In this work, we propose a supercell model, in which every lattice site has similar local atomic environment, to describe the random distributions of the atomic species in HEAs. Using these supercells in combination with ab initio calculations, we investigate the local lattice distortion of refractory HEAs with body-centered-cubic structure and 3 d HEAs with face-centered-cubic structure. Our results demonstrate that the local lattice distortion of the refractory HEAs is much more significant than that of the 3 d HEAs. We show that the atomic size mismatch evaluated with the empirical atomic radii is not accurate enough to describe the local lattice distortion. Both the lattice distortion energy and the mixing entropy contribute significantly to the thermodynamic stability of HEAs. However the local lattice distortion has negligible effect on the equilibrium lattice parameter and bulk modulus.

Method for localizing heating in tumor tissue

DOEpatents

Doss, James D.; McCabe, Charles W.

1977-04-12

A method for a localized tissue heating of tumors is disclosed. Localized radio frequency current fields are produced with specific electrode configurations. Several electrode configurations are disclosed, enabling variations in electrical and thermal properties of tissues to be exploited.

Efficient atom localization via probe absorption in an inverted-Y atomic system

NASA Astrophysics Data System (ADS)

Wu, Jianchun; Wu, Bo; Mao, Jiejian

2018-06-01

The behaviour of atom localization in an inverted-Y atomic system is theoretically investigated. For the atoms interacting with a weak probe field and several orthogonal standing-wave fields, their position information can be obtained by measuring the probe absorption. Compared with the traditional scheme, we couple the probe field to the transition between the middle and top levels. It is found that the probe absorption sensitively depends on the detuning and strength of the relevant light fields. Remarkably, the atom can be localized at a particular position in the standing-wave fields by coupling a microwave field to the transition between the two ground levels.

On the elimination of the electronic structure bottleneck in on the fly nonadiabatic dynamics for small to moderate sized (10-15 atom) molecules using fit diabatic representations based solely on ab initio electronic structure data: The photodissociation of phenol

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhu, Xiaolei, E-mail: virtualzx@gmail.com; Yarkony, David R., E-mail: yarkony@jhu.edu

2016-01-14

In this work, we demonstrate that for moderate sized systems, here a system with 13 atoms, global coupled potential energy surfaces defined for several electronic states over a wide energy range and for distinct regions of nuclear coordinate space characterized by distinct electron configurations, can be constructed with precise energetics and an excellent description of non-adiabatic interactions in all regions. This is accomplished using a recently reported algorithm for constructing quasi-diabatic representations, H{sup d}, of adiabatic electronic states coupled by conical intersections. In this work, the algorithm is used to construct an H{sup d} to describe the photodissociation of phenolmore » from its first and second excited electronic states. The representation treats all 33 internal degrees of freedom in an even handed manner. The ab initio adiabatic electronic structure data used to construct the fit are obtained exclusively from multireference configuration interaction with single and double excitation wave functions comprised of 88 × 10{sup 6} configuration state functions, at geometries determined by quasi-classical trajectories. Since the algorithm uses energy gradients and derivative couplings in addition to electronic energies to construct H{sup d}, data at only 7379 nuclear configurations are required to construct a representation, which describes all nuclear configurations involved in H atom photodissociation to produce the phenoxyl radical in its ground or first excited electronic state, with a mean unsigned energy error of 202.9 cm{sup −1} for electronic energies <60 000 cm{sup −1}.« less

Local Structures of High-Entropy Alloys (HEAs) on Atomic Scales: An Overview

DOE PAGES

Diao, Haoyan; Santodonato, Louis J.; Tang, Zhi; ...

2015-08-29

The high-entropy alloys (HEAs), containing several elements mixed in equimolar or near-equimolar ratios, have shown exceptional engineering properties. Local structures on atomic level are essential to understand the mechanical behaviors and related mechanisms. In this paper, the local structure and stress on the atomic level are reviewed by the pair-distribution function (PDF) of neutron-diffraction data, ab-initio-molecular-dynamics (AIMD) simulations, and atomic-probe microscopy (APT).

Concentration-dependent and configuration-dependent interactions of monovalent ions with an RNA tetraloop

DOE Office of Scientific and Technical Information (OSTI.GOV)

Miner, Jacob Carlson; Garcia, Angel Enrique

Monovalent salt solutions have strongly coupled interactions with biopolymers, from large polyelectrolytes to small RNA oligomers. High salt concentrations have been known to induce transitions in the structure of RNA, producing non-canonical configurations and even driving RNA to precipitate out of solution. Using all-atom molecular dynamics simulations, we model a monovalent salt species (KCL) at high concentrations (0.1–3m) and calculate the equilibrium distributions of water and ions around a small tetraloop-forming RNA oligomer in a variety of structural arrangements: folded A-RNA (canonical) and Z-RNA (non-canonical) tetraloops and unfolded configurations. From these data, we calculate the ion preferential binding coefficients andmore » Donnan coefficients for the RNA oligomer as a function of concentration and structure. We find that cation accumulation is highest around non-canonical Z-RNA configurations at concentrations below 0.5m, while unfolded configurations accumulate the most co-ions in all concentrations. By contrast, canonical A-RNA structures consistently show the lowest accumulations for all ion species. Water distributions vary markedly with RNA configuration but show little dependency on KCL concentration. Based on Donnan coefficient calculations, the net charge of the solution at the surface of the RNA decreases linearly as a function of salt concentration and becomes net-neutral near 2.5–3m KCL for folded configurations, while unfolded configurations still show a positive solution charge. Our findings show that all-atom molecular dynamics can describe the equilibrium distributions of monovalent salt in the presence of small RNA oligomers at KCL concentrations where ion correlation effects become important. Furthermore, these results provide valuable insights into the distributions of water and ions near the RNA oligomer surface as a function of structural configuration.« less

Concentration-dependent and configuration-dependent interactions of monovalent ions with an RNA tetraloop

DOE PAGES

Miner, Jacob Carlson; Garcia, Angel Enrique

2018-05-29

Monovalent salt solutions have strongly coupled interactions with biopolymers, from large polyelectrolytes to small RNA oligomers. High salt concentrations have been known to induce transitions in the structure of RNA, producing non-canonical configurations and even driving RNA to precipitate out of solution. Using all-atom molecular dynamics simulations, we model a monovalent salt species (KCL) at high concentrations (0.1–3m) and calculate the equilibrium distributions of water and ions around a small tetraloop-forming RNA oligomer in a variety of structural arrangements: folded A-RNA (canonical) and Z-RNA (non-canonical) tetraloops and unfolded configurations. From these data, we calculate the ion preferential binding coefficients andmore » Donnan coefficients for the RNA oligomer as a function of concentration and structure. We find that cation accumulation is highest around non-canonical Z-RNA configurations at concentrations below 0.5m, while unfolded configurations accumulate the most co-ions in all concentrations. By contrast, canonical A-RNA structures consistently show the lowest accumulations for all ion species. Water distributions vary markedly with RNA configuration but show little dependency on KCL concentration. Based on Donnan coefficient calculations, the net charge of the solution at the surface of the RNA decreases linearly as a function of salt concentration and becomes net-neutral near 2.5–3m KCL for folded configurations, while unfolded configurations still show a positive solution charge. Our findings show that all-atom molecular dynamics can describe the equilibrium distributions of monovalent salt in the presence of small RNA oligomers at KCL concentrations where ion correlation effects become important. Furthermore, these results provide valuable insights into the distributions of water and ions near the RNA oligomer surface as a function of structural configuration.« less

Concentration-dependent and configuration-dependent interactions of monovalent ions with an RNA tetraloop

NASA Astrophysics Data System (ADS)

Miner, Jacob Carlson; García, Angel Enrique

2018-06-01

Monovalent salt solutions have strongly coupled interactions with biopolymers, from large polyelectrolytes to small RNA oligomers. High salt concentrations have been known to induce transitions in the structure of RNA, producing non-canonical configurations and even driving RNA to precipitate out of solution. Using all-atom molecular dynamics simulations, we model a monovalent salt species (KCL) at high concentrations (0.1-3m) and calculate the equilibrium distributions of water and ions around a small tetraloop-forming RNA oligomer in a variety of structural arrangements: folded A-RNA (canonical) and Z-RNA (non-canonical) tetraloops and unfolded configurations. From these data, we calculate the ion preferential binding coefficients and Donnan coefficients for the RNA oligomer as a function of concentration and structure. We find that cation accumulation is highest around non-canonical Z-RNA configurations at concentrations below 0.5m, while unfolded configurations accumulate the most co-ions in all concentrations. By contrast, canonical A-RNA structures consistently show the lowest accumulations for all ion species. Water distributions vary markedly with RNA configuration but show little dependency on KCL concentration. Based on Donnan coefficient calculations, the net charge of the solution at the surface of the RNA decreases linearly as a function of salt concentration and becomes net-neutral near 2.5-3m KCL for folded configurations, while unfolded configurations still show a positive solution charge. Our findings show that all-atom molecular dynamics can describe the equilibrium distributions of monovalent salt in the presence of small RNA oligomers at KCL concentrations where ion correlation effects become important. Furthermore, these results provide valuable insights into the distributions of water and ions near the RNA oligomer surface as a function of structural configuration.

Concentration-dependent and configuration-dependent interactions of monovalent ions with an RNA tetraloop.

PubMed

Miner, Jacob Carlson; García, Angel Enrique

2018-06-14

Monovalent salt solutions have strongly coupled interactions with biopolymers, from large polyelectrolytes to small RNA oligomers. High salt concentrations have been known to induce transitions in the structure of RNA, producing non-canonical configurations and even driving RNA to precipitate out of solution. Using all-atom molecular dynamics simulations, we model a monovalent salt species (KCL) at high concentrations (0.1-3m) and calculate the equilibrium distributions of water and ions around a small tetraloop-forming RNA oligomer in a variety of structural arrangements: folded A-RNA (canonical) and Z-RNA (non-canonical) tetraloops and unfolded configurations. From these data, we calculate the ion preferential binding coefficients and Donnan coefficients for the RNA oligomer as a function of concentration and structure. We find that cation accumulation is highest around non-canonical Z-RNA configurations at concentrations below 0.5m, while unfolded configurations accumulate the most co-ions in all concentrations. By contrast, canonical A-RNA structures consistently show the lowest accumulations for all ion species. Water distributions vary markedly with RNA configuration but show little dependency on KCL concentration. Based on Donnan coefficient calculations, the net charge of the solution at the surface of the RNA decreases linearly as a function of salt concentration and becomes net-neutral near 2.5-3m KCL for folded configurations, while unfolded configurations still show a positive solution charge. Our findings show that all-atom molecular dynamics can describe the equilibrium distributions of monovalent salt in the presence of small RNA oligomers at KCL concentrations where ion correlation effects become important. Furthermore, these results provide valuable insights into the distributions of water and ions near the RNA oligomer surface as a function of structural configuration.

Density functional theory calculations establish the experimental evidence of the DX center atomic structure in CdTe.

PubMed

Lany, Stephan; Wolf, Herbert; Wichert, Thomas

2004-06-04

The In DX center and the DX-like configuration of the Cd host atom in CdTe are investigated using density functional theory. The simultaneous calculation of the atomic structure and the electric field gradient (EFG) allows one to correlate the theoretically predicted structure of the DX center with an experimental observable, namely, the EFG obtained from radioactive 111In/111Cd probe atoms in In doped CdTe. In this way, the experimental identification of the DX center structure is established.

Equation-of-motion coupled-cluster method for ionised states with spin-orbit coupling using open-shell reference wavefunction

NASA Astrophysics Data System (ADS)

Wang, Zhifan; Wang, Fan

2018-04-01

The equation-of-motion coupled-cluster method for ionised states at the singles and doubles level (EOM-IP-CCSD) with spin-orbit coupling (SOC) included in post-Hartree-Fock (HF) steps is extended to spatially non-degenerate open-shell systems such as high spin states of s1, p3, σ1 or π2 configuration in this work. Pseudopotentials are employed to treat relativistic effects and spin-unrestricted scalar relativistic HF determinant is adopted as reference in calculations. Symmetry is not exploited in the implementation since both time-reversal and spatial symmetry is broken due to SOC. IPs with the EOM-IP-CCSD approach are those from the 3Σ1- states for high spin state of π2 configuration, while the ground state is the 3Σ0- state. When removing an electron from the high spin state of p3 configuration, only the 3P2 state can be reached. The open-shell EOM-IP-CCSD approach with SOC was employed in calculating IPs of some open-shell atoms with s1 configuration, diatomic molecules with π2 configuration and SOC splitting of the ionised π1 state, as well as IPs of VA atoms with p3 configuration. Our results demonstrate that this approach can be applied to ionised states of spatially non-degenerate open-shell states containing heavy elements with reasonable accuracy.

Early differential sensitivity of evoked-potentials to local and global shape during the perception of three-dimensional objects.

PubMed

Leek, E Charles; Roberts, Mark; Oliver, Zoe J; Cristino, Filipe; Pegna, Alan J

2016-08-01

Here we investigated the time course underlying differential processing of local and global shape information during the perception of complex three-dimensional (3D) objects. Observers made shape matching judgments about pairs of sequentially presented multi-part novel objects. Event-related potentials (ERPs) were used to measure perceptual sensitivity to 3D shape differences in terms of local part structure and global shape configuration - based on predictions derived from hierarchical structural description models of object recognition. There were three types of different object trials in which stimulus pairs (1) shared local parts but differed in global shape configuration; (2) contained different local parts but shared global configuration or (3) shared neither local parts nor global configuration. Analyses of the ERP data showed differential amplitude modulation as a function of shape similarity as early as the N1 component between 146-215ms post-stimulus onset. These negative amplitude deflections were more similar between objects sharing global shape configuration than local part structure. Differentiation among all stimulus types was reflected in N2 amplitude modulations between 276-330ms. sLORETA inverse solutions showed stronger involvement of left occipitotemporal areas during the N1 for object discrimination weighted towards local part structure. The results suggest that the perception of 3D object shape involves parallel processing of information at local and global scales. This processing is characterised by relatively slow derivation of 'fine-grained' local shape structure, and fast derivation of 'coarse-grained' global shape configuration. We propose that the rapid early derivation of global shape attributes underlies the observed patterns of N1 amplitude modulations. Copyright © 2016 The Authors. Published by Elsevier Ltd.. All rights reserved.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhu, Jia, E-mail: jia-zhu@jxnu.edu.cn, E-mail: zhangyf@fzu.edu.cn; Zhang, Hui; Tong, Yawen

The structures and electronic properties of bimetallic oxide CrW{sub 2}O{sub 9} clusters supported on the perfect and defective MgO(001) surfaces with three different color centers, F{sub S}{sup 0}, F{sub S}{sup +}, and F{sub S}{sup 2+} centers, respectively, have been investigated by density functional theory calculations. Our results show that the configurations, adsorption energies, charge transfers, and bonding modes of dispersed CrW{sub 2}O{sub 9} clusters are sensitive to the charge states of the F{sub S} centers. Compared with the gas-phase configuration, the CrW{sub 2}O{sub 9} clusters supported on the defective surfaces are distorted dramatically, which exhibit different chain structures. On themore » perfect MgO surface, the depositions of clusters do not involve obvious charge transfer, while the situation is quite different on the defective MgO(001) surfaces in which significant electron transfer occurs from the surface to the cluster. Interestingly, this effect becomes more remarkable for electron-rich oxygen vacancies (F{sub S}{sup 0} center) than that for electron-poor oxygen vacancies (F{sub S}{sup +} and F{sub S}{sup 2+} centers). Furthermore, our work reveals a progressive Brønsted acid sites where spin density preferentially localized around the Cr atoms not the W atoms for all kinds of F{sub S}-centers, indicating the better catalytic activities can be expected for CrW{sub 2}O{sub 9} cluster on defective MgO(001) surfaces with respect to the W{sub 3}O{sub 9} cluster.« less

Interface science of virtual GaN substrates on Si(111) via Sc2O3/Y2O3 buffers: Experiment and theory

NASA Astrophysics Data System (ADS)

Tarnawska, L.; Dabrowski, J.; Grzela, T.; Lehmann, M.; Niermann, T.; Paszkiewicz, R.; Storck, P.; Schroeder, T.

2013-06-01

The final film quality of GaN on foreign substrates is known to crucially depend on the initial GaN interface and nucleation characteristics. To shed light on these characteristics of recently pioneered virtual, hexagonal GaN(0001) substrates on Si(111) via step graded Sc2O3(111)/Y2O3(111) buffers, a complex GaN(0001)/Sc2O3(111) interface structure model and the initial nucleation scenario is derived from a combined experimental (reflection high energy electron diffraction and X-ray photoelectron spectroscopy) and theoretical ab initio study. It is shown that the GaN/Sc2O3 interface chemistry is determined by a N-Ga-O-Sc atomic arrangement leading to N-polar GaN films. However, the atomic GaN(0001)/Sc2O3(111) interface configuration is complex and local perturbations might be at the origin of Ga-polar inversion domains in the mainly N-polar GaN films. The initial growth of GaN on Sc2O3 is characterized by an ultrathin N-Ga-O-Sc wetting layer which carries tensile strain and relaxes with increasing thickness. Further GaN deposition results in the formation of 3D islands which fully relax before island coalescence occurs. The implications of the GaN/Sc2O3 interface configuration, the 3D nucleation growth mode, and the coalescence process of misaligned islands are discussed with respect to the defect characteristics (inversion domains, cubic inclusions, threading dislocations) of the final GaN layer.

Measurement-Based Entanglement of Noninteracting Bosonic Atoms

NASA Astrophysics Data System (ADS)

Lester, Brian J.; Lin, Yiheng; Brown, Mark O.; Kaufman, Adam M.; Ball, Randall J.; Knill, Emanuel; Rey, Ana M.; Regal, Cindy A.

2018-05-01

We demonstrate the ability to extract a spin-entangled state of two neutral atoms via postselection based on a measurement of their spatial configuration. Typically, entangled states of neutral atoms are engineered via atom-atom interactions. In contrast, in our Letter, we use Hong-Ou-Mandel interference to postselect a spin-singlet state after overlapping two atoms in distinct spin states on an effective beam splitter. We verify the presence of entanglement and determine a bound on the postselected fidelity of a spin-singlet state of (0.62 ±0.03 ). The experiment has direct analogy to creating polarization entanglement with single photons and hence demonstrates the potential to use protocols developed for photons to create complex quantum states with noninteracting atoms.

Measurement-Based Entanglement of Noninteracting Bosonic Atoms.

PubMed

Lester, Brian J; Lin, Yiheng; Brown, Mark O; Kaufman, Adam M; Ball, Randall J; Knill, Emanuel; Rey, Ana M; Regal, Cindy A

2018-05-11

We demonstrate the ability to extract a spin-entangled state of two neutral atoms via postselection based on a measurement of their spatial configuration. Typically, entangled states of neutral atoms are engineered via atom-atom interactions. In contrast, in our Letter, we use Hong-Ou-Mandel interference to postselect a spin-singlet state after overlapping two atoms in distinct spin states on an effective beam splitter. We verify the presence of entanglement and determine a bound on the postselected fidelity of a spin-singlet state of (0.62±0.03). The experiment has direct analogy to creating polarization entanglement with single photons and hence demonstrates the potential to use protocols developed for photons to create complex quantum states with noninteracting atoms.

Demonstration of Double EIT Using Coupled Harmonic Oscillators and RLC Circuits

ERIC Educational Resources Information Center

Harden, Joshua; Joshi, Amitabh; Serna, Juan D.

2011-01-01

Single and double electromagnetically induced transparencies (EIT) in a medium, consisting of four-level atoms in the inverted-Y configuration, are discussed using mechanical and electrical analogies. A three-coupled spring-mass system subject to damping and driven by an external force is used to represent the four-level atom mechanically. The…

A New Method for Obtaining Russell-Saunders Terms

ERIC Educational Resources Information Center

Liu, Ying; Liu, Yue; Liu, Bihui

2011-01-01

A new method for obtaining Russell-Saunders terms of atomic configurations is reported. This new method is significantly different from, while at the same time complementary to, previously published methods for obtaining atomic terms. This novel procedure is elicited by the method used to determine the splitting of S, P, D terms in weak ligand…

Atomic structure calculations for F-like tungsten

NASA Astrophysics Data System (ADS)

Sunny, Aggarwal

2014-09-01

Energy levels, wavefunction compositions and lifetimes have been computed for all levels of 1s22s22p5, 1s22s2p6, 1s22s22p43s, 1s22s22p43p, and 1s22s22p43d configurations in highly charged F-like tungsten ion. The multiconfigurational Dirac—Fock method (MCDF) is adopted to generate the wavefunctions. We have also presented the transition wavelengths, oscillator strengths, transition probabilities, and line strengths for the electric dipole (E1) and magnetic quadrupole (M2) transition from the 1s22s22p5 ground configuration. We have performed parallel calculations with the flexible atomic code (FAC) for comparing the atomic data. The reliability of present data is assessed by comparison with other theoretical and experimental data available in the literature. Good agreement is found between our results and those obtained using different approaches confirm the quality of our results. Additionally, we have predicted some new atomic data for F-like W that were not available so far and may be important for plasma diagnostic analysis in fusion plasma.

Steady bipartite coherence induced by non-equilibrium environment

NASA Astrophysics Data System (ADS)

Huangfu, Yong; Jing, Jun

2018-01-01

We study the steady state of two coupled two-level atoms interacting with a non-equilibrium environment that consists of two heat baths at different temperatures. Specifically, we analyze four cases with respect to the configuration about the interactions between atoms and heat baths. Using secular approximation, the conventional master equation usually neglects steady-state coherence, even when the system is coupled with a non-equilibrium environment. When employing the master equation with no secular approximation, we find that the system coherence in our model, denoted by the off-diagonal terms in the reduced density matrix spanned by the eigenvectors of the system Hamiltonian, would survive after a long-time decoherence evolution. The absolute value of residual coherence in the system relies on different configurations of interaction channels between the system and the heat baths. We find that a large steady quantum coherence term can be achieved when the two atoms are resonant. The absolute value of quantum coherence decreases in the presence of additional atom-bath interaction channels. Our work sheds new light on the mechanism of steady-state coherence in microscopic quantum systems in non-equilibrium environments.

Real-space imaging of a topologically protected edge state with ultracold atoms in an amplitude-chirped optical lattice

PubMed Central

Leder, Martin; Grossert, Christopher; Sitta, Lukas; Genske, Maximilian; Rosch, Achim; Weitz, Martin

2016-01-01

To describe a mobile defect in polyacetylene chains, Su, Schrieffer and Heeger formulated a model assuming two degenerate energy configurations that are characterized by two different topological phases. An immediate consequence was the emergence of a soliton-type edge state located at the boundary between two regions of different configurations. Besides giving first insights in the electrical properties of polyacetylene materials, interest in this effect also stems from its close connection to states with fractional charge from relativistic field theory. Here, using a one-dimensional optical lattice for cold rubidium atoms with a spatially chirped amplitude, we experimentally realize an interface between two spatial regions of different topological order in an atomic physics system. We directly observe atoms confined in the edge state at the intersection by optical real-space imaging and characterize the state as well as the size of the associated energy gap. Our findings hold prospects for the spectroscopy of surface states in topological matter and for the quantum simulation of interacting Dirac systems. PMID:27767054

The reaction efficiency of thermal energy oxygen atoms with polymeric materials

NASA Technical Reports Server (NTRS)

Koontz, S. L.; Nordine, Paul

1990-01-01

The reaction efficiency of several polymeric materials with thermal-energy (0.04 eV translational energy), ground-state (O3P) oxygen atoms was determined by exposing the materials to a room temperature gas containing a known concentration of atomic oxygen. The reaction efficiency measurements were conducted in two flowing afterglow systems of different configuration. Atomic oxygen concentration measurements, flow, transport and surface dose analysis is presented in this paper. The measured reaction efficiencies of Kapton, Mylar, polyethylene, D4-polyethylene and Tedlar are .001 to .0001 those determined with high-energy ground-state oxygen atoms in low earth orbit or in a high-velocity atom beam. D4-polyethylene exhibits a large kinetic isotope effect with atomic oxygen at thermal but not hyperthermal atom energies.

Entangling two transportable neutral atoms via local spin exchange.

PubMed

Kaufman, A M; Lester, B J; Foss-Feig, M; Wall, M L; Rey, A M; Regal, C A

2015-11-12

To advance quantum information science, physical systems are sought that meet the stringent requirements for creating and preserving quantum entanglement. In atomic physics, robust two-qubit entanglement is typically achieved by strong, long-range interactions in the form of either Coulomb interactions between ions or dipolar interactions between Rydberg atoms. Although such interactions allow fast quantum gates, the interacting atoms must overcome the associated coupling to the environment and cross-talk among qubits. Local interactions, such as those requiring substantial wavefunction overlap, can alleviate these detrimental effects; however, such interactions present a new challenge: to distribute entanglement, qubits must be transported, merged for interaction, and then isolated for storage and subsequent operations. Here we show how, using a mobile optical tweezer, it is possible to prepare and locally entangle two ultracold neutral atoms, and then separate them while preserving their entanglement. Ground-state neutral atom experiments have measured dynamics consistent with spin entanglement, and have detected entanglement with macroscopic observables; we are now able to demonstrate position-resolved two-particle coherence via application of a local gradient and parity measurements. This new entanglement-verification protocol could be applied to arbitrary spin-entangled states of spatially separated atoms. The local entangling operation is achieved via spin-exchange interactions, and quantum tunnelling is used to combine and separate atoms. These techniques provide a framework for dynamically entangling remote qubits via local operations within a large-scale quantum register.

Configurable unitary transformations and linear logic gates using quantum memories.

PubMed

Campbell, G T; Pinel, O; Hosseini, M; Ralph, T C; Buchler, B C; Lam, P K

2014-08-08

We show that a set of optical memories can act as a configurable linear optical network operating on frequency-multiplexed optical states. Our protocol is applicable to any quantum memories that employ off-resonant Raman transitions to store optical information in atomic spins. In addition to the configurability, the protocol also offers favorable scaling with an increasing number of modes where N memories can be configured to implement arbitrary N-mode unitary operations during storage and readout. We demonstrate the versatility of this protocol by showing an example where cascaded memories are used to implement a conditional cz gate.

Synthesis of borophenes: Anisotropic, two-dimensional boron polymorphs

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mannix, A. J.; Zhou, X. -F.; Kiraly, B.

At the atomic-cluster scale, pure boron is markedly similar to carbon, forming simple planar molecules and cage-like fullerenes. Theoretical studies predict that two-dimensional (2D) boron sheets will adopt an atomic configuration similar to that of boron atomic clusters. We synthesized atomically thin, crystalline 2D boron sheets (i.e., borophene) on silver surfaces under ultrahigh-vacuum conditions. Atomic-scale characterization, supported by theoretical calculations, revealed structures reminiscent of fused boron clusters with multiple scales of anisotropic, out-of-plane buckling. Unlike bulk boron allotropes, borophene shows metallic characteristics that are consistent with predictions of a highly anisotropic, 2D metal.

Demonstration of improved sensitivity of echo interferometers to gravitational acceleration

NASA Astrophysics Data System (ADS)

Mok, C.; Barrett, B.; Carew, A.; Berthiaume, R.; Beattie, S.; Kumarakrishnan, A.

2013-08-01

We have developed two configurations of an echo interferometer that rely on standing-wave excitation of a laser-cooled sample of rubidium atoms. Both configurations can be used to measure acceleration a along the axis of excitation. For a two-pulse configuration, the signal from the interferometer is modulated at the recoil frequency and exhibits a sinusoidal frequency chirp as a function of pulse spacing. In comparison, for a three-pulse stimulated-echo configuration, the signal is observed without recoil modulation and exhibits a modulation at a single frequency as a function of pulse spacing. The three-pulse configuration is less sensitive to effects of vibrations and magnetic field curvature, leading to a longer experimental time scale. For both configurations of the atom interferometer (AI), we show that a measurement of acceleration with a statistical precision of 0.5% can be realized by analyzing the shape of the echo envelope that has a temporal duration of a few microseconds. Using the two-pulse AI, we obtain measurements of acceleration that are statistically precise to 6 parts per million (ppm) on a 25 ms time scale. In comparison, using the three-pulse AI, we obtain measurements of acceleration that are statistically precise to 0.4 ppm on a time scale of 50 ms. A further statistical enhancement is achieved by analyzing the data across the echo envelope so that the statistical error is reduced to 75 parts per billion (ppb). The inhomogeneous field of a magnetized vacuum chamber limited the experimental time scale and resulted in prominent systematic effects. Extended time scales and improved signal-to-noise ratio observed in recent echo experiments using a nonmagnetic vacuum chamber suggest that echo techniques are suitable for a high-precision measurement of gravitational acceleration g. We discuss methods for reducing systematic effects and improving the signal-to-noise ratio. Simulations of both AI configurations with a time scale of 300 ms suggest that an optimized experiment with improved vibration isolation and atoms selected in the mF=0 state can result in measurements of g statistically precise to 0.3 ppb for the two-pulse AI and 0.6 ppb for the three-pulse AI.

Enhanced Sampling of an Atomic Model with Hybrid Nonequilibrium Molecular Dynamics-Monte Carlo Simulations Guided by a Coarse-Grained Model.

PubMed

Chen, Yunjie; Roux, Benoît

2015-08-11

Molecular dynamics (MD) trajectories based on a classical equation of motion provide a straightforward, albeit somewhat inefficient approach, to explore and sample the configurational space of a complex molecular system. While a broad range of techniques can be used to accelerate and enhance the sampling efficiency of classical simulations, only algorithms that are consistent with the Boltzmann equilibrium distribution yield a proper statistical mechanical computational framework. Here, a multiscale hybrid algorithm relying simultaneously on all-atom fine-grained (FG) and coarse-grained (CG) representations of a system is designed to improve sampling efficiency by combining the strength of nonequilibrium molecular dynamics (neMD) and Metropolis Monte Carlo (MC). This CG-guided hybrid neMD-MC algorithm comprises six steps: (1) a FG configuration of an atomic system is dynamically propagated for some period of time using equilibrium MD; (2) the resulting FG configuration is mapped onto a simplified CG model; (3) the CG model is propagated for a brief time interval to yield a new CG configuration; (4) the resulting CG configuration is used as a target to guide the evolution of the FG system; (5) the FG configuration (from step 1) is driven via a nonequilibrium MD (neMD) simulation toward the CG target; (6) the resulting FG configuration at the end of the neMD trajectory is then accepted or rejected according to a Metropolis criterion before returning to step 1. A symmetric two-ends momentum reversal prescription is used for the neMD trajectories of the FG system to guarantee that the CG-guided hybrid neMD-MC algorithm obeys microscopic detailed balance and rigorously yields the equilibrium Boltzmann distribution. The enhanced sampling achieved with the method is illustrated with a model system with hindered diffusion and explicit-solvent peptide simulations. Illustrative tests indicate that the method can yield a speedup of about 80 times for the model system and up to 21 times for polyalanine and (AAQAA)3 in water.

Enhanced Sampling of an Atomic Model with Hybrid Nonequilibrium Molecular Dynamics—Monte Carlo Simulations Guided by a Coarse-Grained Model

PubMed Central

2015-01-01

Molecular dynamics (MD) trajectories based on a classical equation of motion provide a straightforward, albeit somewhat inefficient approach, to explore and sample the configurational space of a complex molecular system. While a broad range of techniques can be used to accelerate and enhance the sampling efficiency of classical simulations, only algorithms that are consistent with the Boltzmann equilibrium distribution yield a proper statistical mechanical computational framework. Here, a multiscale hybrid algorithm relying simultaneously on all-atom fine-grained (FG) and coarse-grained (CG) representations of a system is designed to improve sampling efficiency by combining the strength of nonequilibrium molecular dynamics (neMD) and Metropolis Monte Carlo (MC). This CG-guided hybrid neMD-MC algorithm comprises six steps: (1) a FG configuration of an atomic system is dynamically propagated for some period of time using equilibrium MD; (2) the resulting FG configuration is mapped onto a simplified CG model; (3) the CG model is propagated for a brief time interval to yield a new CG configuration; (4) the resulting CG configuration is used as a target to guide the evolution of the FG system; (5) the FG configuration (from step 1) is driven via a nonequilibrium MD (neMD) simulation toward the CG target; (6) the resulting FG configuration at the end of the neMD trajectory is then accepted or rejected according to a Metropolis criterion before returning to step 1. A symmetric two-ends momentum reversal prescription is used for the neMD trajectories of the FG system to guarantee that the CG-guided hybrid neMD-MC algorithm obeys microscopic detailed balance and rigorously yields the equilibrium Boltzmann distribution. The enhanced sampling achieved with the method is illustrated with a model system with hindered diffusion and explicit-solvent peptide simulations. Illustrative tests indicate that the method can yield a speedup of about 80 times for the model system and up to 21 times for polyalanine and (AAQAA)3 in water. PMID:26574442

Conformational analysis investigation into the influence of nano-porosity of ultra-permeable ultra-selective polyimides on its diffusivity as potential membranes for use in the "green" separation of natural gases

NASA Astrophysics Data System (ADS)

Madkour, Tarek M.

2013-08-01

Nano-porous polymers of intrinsic microporosity, PIM, have exhibited excellent permeability and selectivity characteristics that could be utilized in an environmentally friendly gas separation process. A full understanding of the mechanism through which these membranes effectively and selectively allow for the permeation of specific gases will lead to further development of these membranes. Three factors obviously influenced the conformational behavior of these polymers, which are the presence of electronegative atoms, the presence of non-linearity in the polymeric backbones (backbone kinks) and the presence of bulky side groups on the polymeric chains. The dipole moment increased sharply with the presence of backbone kinks more than any other factor. Replacing the fluorine atoms with bulky alkyl groups didn't influence the dipole moment greatly indicating that the size of the side chains had much less dramatic influence on the dipole moment than having a bent backbone. Similarly, the presence of the backbone kinks in the polymeric chains influenced the polymeric chains to assume less extended configuration causing the torsional angles around the interconnecting bonds unable to cross the high potential energy barriers. The presence of the bulky side groups also caused the energy barriers of the cis-configurations to increase dramatically, which prevented the polymeric segments from experiencing full rotation about the connecting bonds. For these polymers, it was clear that the fully extended configurations are the preferred configurations in the absence of strong electronegative atoms, backbones kinks or bulky side groups. The addition of any of these factors to the polymeric structures resulted in the polymeric chains being forced to assume less extended configurations. Rather interestingly, the length or bulkiness of the side groups didn't affect the end-to-end distance distribution to a great deal since the presence of quite large bulky side chain such as the pentyl group has caused the polymeric chains to revert back to the fully extended configurations possibly due to the quite high potential energy barriers that the chains have to cross to reach the less extended configurational states.

Molecular dynamics investigation of dynamical heterogeneity and local structure in the supercooled liquid and glass states of Al

NASA Astrophysics Data System (ADS)

Li, Maozhi; Wang, Cai-Zhuang; Mendelev, Mikhail I.; Ho, Kai-Ming

2008-05-01

Molecular dynamics simulations are performed to study the structure and dynamical heterogeneity in the liquid and glass states of Al using a frequently employed embedded atom potential. While the pair correlation function of the glass and liquid states displays only minor differences, the icosahedral short-range order (ISRO) and the dynamics of the two states are very different. The ISRO is much stronger in the glass than in the liquid. It is also found that both the most mobile and the most immobile atoms in the glass state tend to form clusters, and the clusters formed by the immobile atoms are more compact. In order to investigate the local environment of each atom in the liquid and glass states, a local density is defined to characterize the local atomic packing. There is a strong correlation between the local packing density and the mobility of the atoms. These results indicate that dynamical heterogeneity in glasses is directly correlated to the local structure. We also analyze the diffusion mechanisms of atoms in the liquid and glass states. It is found that for the mobile atoms in the glass state, initially they are confined in the cages formed by their nearest neighbors and vibrating. On the time scale of β relaxation, the mobile atoms try to break up the cage confinement and hop into new cages. In the supercooled liquid states, however, atoms continuously diffuse. Furthermore, it is found that on the time scale of β relaxation, some of the mobile atoms in the glass state cooperatively hop, which is facilitated by the stringlike cluster structures. On the longer time scale, it is found that a certain fraction of atoms can simultaneously hop, although they are not nearest neighbors. Further analysis shows that these hopping atoms form big and more compact clusters than the characterized most mobile atoms. The cooperative rearrangement of these big compact clusters might facilitate the simultaneous hopping of atoms in the glass states on the long time scale.

EIT in resonator chains: similarities and differences with atomic media

NASA Technical Reports Server (NTRS)

Matsko, A. B.; Maleki, L.; Savchenkov, A. A.; Ilchenko, V. S.

2004-01-01

We theoretically study a parallel configuration of two interacting whispering gallery mode optical resonators and show a narrow-band modal structure as a basis for a widely tunable delay line. For the optimum coupling configuration the system can possess an unusually narrow spectral feature with a much narrower bandwidth than the loaded bandwidth of each individual resonator.

Generation of non-classical correlated photon pairs via a ladder-type atomic configuration: theory and experiment.

PubMed

Ding, Dong-Sheng; Zhou, Zhi-Yuan; Shi, Bao-Sen; Zou, Xu-Bo; Guo, Guang-Can

2012-05-07

We experimentally generate a non-classical correlated two-color photon pair at 780 and 1529.4 nm in a ladder-type configuration using a hot 85Rb atomic vapor with the production rate of ~10(7)/s. The non-classical correlation between these two photons is demonstrated by strong violation of Cauchy-Schwarz inequality by the factor R = 48 ± 12. Besides, we experimentally investigate the relations between the correlation and some important experimental parameters such as the single-photon detuning, the powers of pumps. We also make a theoretical analysis in detail and the theoretical predictions are in reasonable agreement with our experimental results.

Atomic-Scale Variations of the Mechanical Response of 2D Materials Detected by Noncontact Atomic Force Microscopy.

PubMed

de la Torre, B; Ellner, M; Pou, P; Nicoara, N; Pérez, Rubén; Gómez-Rodríguez, J M

2016-06-17

We show that noncontact atomic force microscopy (AFM) is sensitive to the local stiffness in the atomic-scale limit on weakly coupled 2D materials, as graphene on metals. Our large amplitude AFM topography and dissipation images under ultrahigh vacuum and low temperature resolve the atomic and moiré patterns in graphene on Pt(111), despite its extremely low geometric corrugation. The imaging mechanisms are identified with a multiscale model based on density-functional theory calculations, where the energy cost of global and local deformations of graphene competes with short-range chemical and long-range van der Waals interactions. Atomic contrast is related with short-range tip-sample interactions, while the dissipation can be understood in terms of global deformations in the weakly coupled graphene layer. Remarkably, the observed moiré modulation is linked with the subtle variations of the local interplanar graphene-substrate interaction, opening a new route to explore the local mechanical properties of 2D materials at the atomic scale.

Probing the localization of magnetic dichroism by atomic-size astigmatic and vortex electron beams.

PubMed

Negi, Devendra Singh; Idrobo, Juan Carlos; Rusz, Ján

2018-03-05

We report localization of a magnetic dichroic signal on atomic columns in electron magnetic circular dichroism (EMCD), probed by beam distorted by four-fold astigmatism and electron vortex beam. With astigmatic probe, magnetic signal to noise ratio can be enhanced by blocking the intensity from the central part of probe. However, the simulations show that for atomic resolution magnetic measurements, vortex beam is a more effective probe, with much higher magnetic signal to noise ratio. For all considered beam shapes, the optimal SNR constrains the signal detection at low collection angles of approximately 6-8 mrad. Irrespective of the material thickness, the magnetic signal remains strongly localized within the probed atomic column with vortex beam, whereas for astigmatic probes, the magnetic signal originates mostly from the nearest neighbor atomic columns. Due to excellent signal localization at probing individual atomic columns, vortex beams are predicted to be a strong candidate for studying the crystal site specific magnetic properties, magnetic properties at interfaces, or magnetism arising from individual atomic impurities.

3D atom microscopy in the presence of Doppler shift

NASA Astrophysics Data System (ADS)

Rahmatullah; Chuang, You-Lin; Lee, Ray-Kuang; Qamar, Sajid

2018-03-01

The interaction of hot atoms with laser fields produces a Doppler shift, which can severely affect the precise spatial measurement of an atom. We suggest an experimentally realizable scheme to address this issue in the three-dimensional position measurement of a single atom in vapors of rubidium atoms. A three-level Λ-type atom-field configuration is considered where a moving atom interacts with three orthogonal standing-wave laser fields and spatial information of the atom in 3D space is obtained via an upper-level population using a weak probe laser field. The atom moves with velocity v along the probe laser field, and due to the Doppler broadening the precision of the spatial information deteriorates significantly. It is found that via a microwave field, precision in the position measurement of a single hot rubidium atom can be attained, overcoming the limitation posed by the Doppler shift.

Atom-by-atom assembly of defect-free one-dimensional cold atom arrays.

PubMed

Endres, Manuel; Bernien, Hannes; Keesling, Alexander; Levine, Harry; Anschuetz, Eric R; Krajenbrink, Alexandre; Senko, Crystal; Vuletic, Vladan; Greiner, Markus; Lukin, Mikhail D

2016-11-25

The realization of large-scale fully controllable quantum systems is an exciting frontier in modern physical science. We use atom-by-atom assembly to implement a platform for the deterministic preparation of regular one-dimensional arrays of individually controlled cold atoms. In our approach, a measurement and feedback procedure eliminates the entropy associated with probabilistic trap occupation and results in defect-free arrays of more than 50 atoms in less than 400 milliseconds. The technique is based on fast, real-time control of 100 optical tweezers, which we use to arrange atoms in desired geometric patterns and to maintain these configurations by replacing lost atoms with surplus atoms from a reservoir. This bottom-up approach may enable controlled engineering of scalable many-body systems for quantum information processing, quantum simulations, and precision measurements. Copyright © 2016, American Association for the Advancement of Science.

Born Oppenheimer potential energy for interaction of antihydrogen with molecular hydrogen

NASA Astrophysics Data System (ADS)

Strasburger, Krzysztof

2005-09-01

Inelastic collisions with hydrogen molecules are claimed to be an important channel of antihydrogen (\\overlineH) losses (Armour and Zeman 1999 Int. J. Quantum Chem. 74 645). In the present work, interaction energies for the H_{2}\\--\\overlineH system in the ground state have been calculated within the Born-Oppenheimer approximation. The leptonic problem was solved variationally with the basis of explicitly correlated Gaussian functions. The geometry of H2 was fixed at equilibrium geometry and the \\overlineH atom approached the molecule from two directions—along or perpendicularly to the bond axis. Purely attractive potential energy curve has been obtained for the first nuclear configuration, while a local maximum (lower than the energy at infinite separation) has been found for the second one.

Atomistic structures of nano-engineered SiC and radiation-induced amorphization resistance

DOE PAGES

Imada, Kenta; Ishimaru, Manabu; Sato, Kazuhisa; ...

2015-06-18

In this paper, nano-engineered 3C–SiC thin films, which possess columnar structures with high-density stacking faults and twins, were irradiated with 2 MeV Si ions at cryogenic and room temperatures. From cross-sectional transmission electron microscopy observations in combination with Monte Carlo simulations based on the Stopping and Range of Ions in Matter code, it was found that their amorphization resistance is six times greater than bulk crystalline SiC at room temperature. High-angle bright-field images taken by spherical aberration corrected scanning transmission electron microscopy revealed that the distortion of atomic configurations is localized near the stacking faults. Finally, the resultant strain fieldmore » probably contributes to the enhancement of radiation tolerance of this material.« less

Robert Curl, Jr. and the Discovery of Fullerenes

Science.gov Websites

produced thousands of variations of the buckyball, including carbon sheets one atom thick and microscopic equilibrium in the carbon vapor that allowed the group to identify a unique, 60-atom configuration of carbon Interview with Robert F. Curl, Jr., nobelprize.org (video) Interview with Robert Curl (video) Buckyballs

FAST TRACK COMMUNICATION: Generalized geometrical model for photoionization of polarized atoms: II. Magnetic dichroism in the 3p photoemission from the K 3p64s 2S1/2 ground state

NASA Astrophysics Data System (ADS)

Grum-Grzhimailo, A. N.; Cubaynes, D.; Heinecke, E.; Hoffmann, P.; Zimmermann, P.; Meyer, M.

2010-10-01

The generalized geometrical model for photoionization from polarized atoms is extended to include mixing of configurations in the initial atomic and/or the final photoion states. The theoretical results for angle-resolved linear and circular magnetic dichroism are in good agreement with new high-resolution photoelectron data for 3p-1 photoionization of potassium atoms polarized in the K 3p64s 2S1/2 ground state by laser optical pumping.

GAPD: a GPU-accelerated atom-based polychromatic diffraction simulation code.

PubMed

E, J C; Wang, L; Chen, S; Zhang, Y Y; Luo, S N

2018-03-01

GAPD, a graphics-processing-unit (GPU)-accelerated atom-based polychromatic diffraction simulation code for direct, kinematics-based, simulations of X-ray/electron diffraction of large-scale atomic systems with mono-/polychromatic beams and arbitrary plane detector geometries, is presented. This code implements GPU parallel computation via both real- and reciprocal-space decompositions. With GAPD, direct simulations are performed of the reciprocal lattice node of ultralarge systems (∼5 billion atoms) and diffraction patterns of single-crystal and polycrystalline configurations with mono- and polychromatic X-ray beams (including synchrotron undulator sources), and validation, benchmark and application cases are presented.

Microcavities coupled to multilevel atoms

NASA Astrophysics Data System (ADS)

Schmid, Sandra Isabelle; Evers, Jörg

2011-11-01

A three-level atom in the Λ configuration coupled to a microcavity is studied. The two transitions of the atom are assumed to couple to different counterpropagating mode pairs in the cavity. We analyze the dynamics both in the strong-coupling and the bad-cavity limits. We find that, compared to a two-level setup, the third atomic state and the additional control field modes crucially modify the system dynamics and enable more advanced control schemes. All results are explained using appropriate dressed-state and eigenmode representations. As potential applications, we discuss optical switching and turnstile operations and detection of particles close to the resonator surface.

Distortion of Local Atomic Structures in Amorphous Ge-Sb-Te Phase Change Materials

NASA Astrophysics Data System (ADS)

Hirata, A.; Ichitsubo, T.; Guan, P. F.; Fujita, T.; Chen, M. W.

2018-05-01

The local atomic structures of amorphous Ge-Sb-Te phase-change materials have yet to be clarified and the rapid crystal-amorphous phase change resulting in distinct optical contrast is not well understood. We report the direct observation of local atomic structures in amorphous Ge2Sb2Te5 using "local" reverse Monte Carlo modeling dedicated to an angstrom-beam electron diffraction analysis. The results corroborated the existence of local structures with rocksalt crystal-like topology that were greatly distorted compared to the crystal symmetry. This distortion resulted in the breaking of ideal octahedral atomic environments, thereby forming local disordered structures that basically satisfied the overall amorphous structure factor. The crystal-like distorted octahedral structures could be the main building blocks in the formation of the overall amorphous structure of Ge-Sb-Te.

Thermalization dynamics in a quenched many-body state

NASA Astrophysics Data System (ADS)

Kaufman, Adam; Preiss, Philipp; Tai, Eric; Lukin, Alex; Rispoli, Matthew; Schittko, Robert; Greiner, Markus

2016-05-01

Quantum and classical many-body systems appear to have disparate behavior due to the different mechanisms that govern their evolution. The dynamics of a classical many-body system equilibrate to maximally entropic states and quickly re-thermalize when perturbed. The assumptions of ergodicity and unbiased configurations lead to a successful framework of describing classical systems by a sampling of thermal ensembles that are blind to the system's microscopic details. By contrast, an isolated quantum many-body system is governed by unitary evolution: the system retains memory of past dynamics and constant global entropy. However, even with differing characteristics, the long-term behavior for local observables in quenched, non-integrable quantum systems are often well described by the same thermal framework. We explore the onset of this convergence in a many-body system of bosonic atoms in an optical lattice. Our system's finite size allows us to verify full state purity and measure local observables. We observe rapid growth and saturation of the entanglement entropy with constant global purity. The combination of global purity and thermalized local observables agree with the Eigenstate Thermalization Hypothesis in the presence of a near-volume law in the entanglement entropy.

Absolute configurations of organometallic compounds. III. Structure and absolute configuration of the square-pyramidal complex ((+)/sub 579/-(C/sub 5/H/sub 5/)Mo(CO)/sub 2/(NN*))PF/sub 6/(NN* = Schiff base derived from pyridine-2-carbaldehyde and (S)-(-)-. cap alpha. -phenylethylamine)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bernal, I.; LaPlaca, S.J.; Korp, J.

The structure of (+)/sub 579/-(eta/sup 5/-C/sub 5/H/sub 5/Mo(CO)/sub 2/(NN*))PF/sub 6/ with NN* = the Schiff base derived from pyridine-2-carbaldehyde and (S)-(--)-..cap alpha..-phenylethylamine was determined using standard single-crystal x-ray diffraction methods. The absolute configuration was determined by refinement of the data using the anomalous scattering contributions of Mo and P to a final R(F) = 0.056 for 2634 independent reflections having I greater than 3 sigma (I). The substance crystallizes in the space group P2/sub 1/2/sub 1/2/sub 1/ with unit cell dimensions of a = 12.249 (4), b = 9.236 (3), and c = 20.692 (9) A and Z = 4more » molecules/unit cell. The square-pyramidal coordination of the Mo atom is defined by two carbonyl carbons and two Schiff base nitrogens occupying the four basal plane sites and the five carbons of the eta/sup 5/-C/sub 5/H/sub 5/ ligand in the axial position. The Mo--ligand distances and the bond lengths and angles within the ligands are normal and compare closely with those of recent structure determinations of comparable precision. The Mo atom is 0.95 A above the plane formed by the four basal plane ligands. The conformation of the (S)-..cap alpha..-phenylethyl group with respect to the ligand plane, defined by the pyridine ring, the imine system, and the Mo atom, is discussed. The configuration at the metal atom in the (+)/sub 579/ isomer is specified as (S). The PF/sub 6//sup -/ anion executes large amplitude torsional motion in the lattice, as is commonly the case for this anion when not hydrogen bonded.« less

Crystallized and amorphous vortices in rotating atomic-molecular Bose-Einstein condensates

PubMed Central

Liu, Chao-Fei; Fan, Heng; Gou, Shih-Chuan; Liu, Wu-Ming

2014-01-01

Vortex is a topological defect with a quantized winding number of the phase in superfluids and superconductors. Here, we investigate the crystallized (triangular, square, honeycomb) and amorphous vortices in rotating atomic-molecular Bose-Einstein condensates (BECs) by using the damped projected Gross-Pitaevskii equation. The amorphous vortices are the result of the considerable deviation induced by the interaction of atomic-molecular vortices. By changing the atom-molecule interaction from attractive to repulsive, the configuration of vortices can change from an overlapped atomic-molecular vortices to carbon-dioxide-type ones, then to atomic vortices with interstitial molecular vortices, and finally into independent separated ones. The Raman detuning can tune the ratio of the atomic vortex to the molecular vortex. We provide a phase diagram of vortices in rotating atomic-molecular BECs as a function of Raman detuning and the strength of atom-molecule interaction. PMID:24573303

Structural and electronic properties of multilayer graphene on monolayer hexagonal boron nitride/nickel (111) interface system: A van der Waals density functional study

NASA Astrophysics Data System (ADS)

Yelgel, Celal

2016-02-01

The structural and electronic properties of multilayer graphene adsorbed on monolayer hexagonal boron nitride (h-BN)/Ni(111) interface system are investigated using the density functional theory with a recently developed non-local van der Waals density functional (rvv10). The most energetically favourable configuration for a monolayer h-BN/Ni(111) interface is found to be N atom atop the Ni atoms and B atom in fcc site with the interlayer distance of 2.04 Å and adsorption energy of 302 meV/BN. Our results show that increasing graphene layers on a monolayer h-BN/Ni(111) interface leads to a weakening of the interfacial interaction between the monolayer h-BN and Ni(111) surface. The adsorption energy of graphene layers on the h-BN/Ni(111) interface is found to be in the range of the 50-120 meV/C atom as the vertical distance from h-BN to the bottommost graphene layers decreases. With the adsorption of a multilayer graphene on the monolayer h-BN/Ni(111) interface system, the band gap of 0.12 eV and 0.25 eV opening in monolayer graphene and bilayer graphene near the K point is found with an upward shifting of the Fermi level. However, a stacking-sensitive band gap is opened in trilayer graphene. We obtain the band gap of 0.35 eV close to the K point with forming a Mexican hat band structure for ABC-stacked trilayer graphene.

Molecular dynamics and quasidynamics simulations of the annealing of bulk and near-surface interstitials formed in molecular-beam epitaxial Si due to low-energy particle bombardment during deposition

NASA Technical Reports Server (NTRS)

Kitabatake, M.; Fons, P.; Greene, J. E.

1991-01-01

The relaxation, diffusion, and annihilation of split and hexagonal interstitials resulting from 10 eV Si irradiation of (2x1)-terminated Si(100) are investigated. Molecular dynamics and quasidynamics simulations, utilizing the Tersoff many-body potential are used in the investigation. The interstitials are created in layers two through six, and stable atomic configurations and total potential energies are derived as a function of site symmetry and layer depth. The interstitial Si atoms are allowed to diffuse, and the total potential energy changes are calculated. Lattice configurations along each path, as well as the starting configurations, are relaxed, and minimum energy diffusion paths are derived. The results show that the minimum energy paths are toward the surface and generally involved tetrahedral sites. The calculated interstitial migration activation energies are always less than 1.4 eV and are much lower in the near-surface region than in the bulk.

Multireference configuration interaction calculations of the first six ionization potentials of the uranium atom

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bross, David H.; Parmar, Payal; Peterson, Kirk A.

The first 6 ionization potentials (IPs) of the uranium atom have been calculated using multireference configuration interaction (MRCI+Q) with extrapolations to the complete basis set (CBS) limit using new all-electron correlation consistent basis sets. The latter were carried out with the third-order Douglas-Kroll-Hess Hamiltonian. Correlation down through the 5s5p5d electrons have been taken into account, as well as contributions to the IPs due to the Lamb shift. Spin-orbit coupling contributions calculated at the 4-component Kramers restricted configuration interaction level, as well as the Gaunt term computed at the Dirac-Hartree-Fock level, were added to the best scalar relativistic results. As amore » result, the final ionization potentials are expected to be accurate to at least 5 kcal/mol (0.2 eV), and thus more reliable than the current experimental values of IP 3 through IP 6.« less

Hyperfine Structure Constants of Energetically High-lying Levels of Odd Parity of Atomic Vanadium

NASA Astrophysics Data System (ADS)

Güzelçimen, F.; Yapıcı, B.; Demir, G.; Er, A.; Öztürk, I. K.; Başar, Gö.; Kröger, S.; Tamanis, M.; Ferber, R.; Docenko, D.; Başar, Gü.

2014-09-01

High-resolution Fourier transform spectra of a vanadium-argon plasma have been recorded in the wavelength range of 365-670 nm (15,000-27,400 cm-1). Optical bandpass filters were used in the experimental setup to enhance the sensitivity of the Fourier transform spectrometer. In total, 138 atomic vanadium spectral lines showing resolved or partially resolved hyperfine structure have been analyzed to determine the magnetic dipole hyperfine structure constants A of the involved energy levels. One of the investigated lines has not been previously classified. As a result, the magnetic dipole hyperfine structure constants A for 90 energy levels are presented: 35 of them belong to the configuration 3d 34s4p and 55 to the configuration 3d 44p. Of these 90 constants, 67 have been determined for the first time, with 23 corresponding to the configuration 3d 34s4p and 44 to 3d 44p.

Velocity selection for ultracold atoms using mazer action in a bimodal cavity

NASA Astrophysics Data System (ADS)

Irshad, Afshan; Qamar, Sajid; Qamar, Shahid

2010-01-01

In this paper, we discuss the velocity selection of ultracold three-level atoms in Λ configuration using a mazer. Our model is the same as discussed by Arun et al. [R. Arun, G.S. Agarwal, M.O. Scully, H. Walther, Phys. Rev. A 62 (2000) 023809] for mazer action in a bimodal cavity. We show that the initial Maxwellian velocity distribution of ultracold atoms can be narrowed due to the presence of resonances in the transmission through dressed-state potential. When the atoms are initially prepared in one of the two lower atomic states then significantly better velocity selectivity is obtained due to the presence of dark states.

Synthesis of borophenes: Anisotropic, two-dimensional boron polymorphs.

PubMed

Mannix, Andrew J; Zhou, Xiang-Feng; Kiraly, Brian; Wood, Joshua D; Alducin, Diego; Myers, Benjamin D; Liu, Xiaolong; Fisher, Brandon L; Santiago, Ulises; Guest, Jeffrey R; Yacaman, Miguel Jose; Ponce, Arturo; Oganov, Artem R; Hersam, Mark C; Guisinger, Nathan P

2015-12-18

At the atomic-cluster scale, pure boron is markedly similar to carbon, forming simple planar molecules and cage-like fullerenes. Theoretical studies predict that two-dimensional (2D) boron sheets will adopt an atomic configuration similar to that of boron atomic clusters. We synthesized atomically thin, crystalline 2D boron sheets (i.e., borophene) on silver surfaces under ultrahigh-vacuum conditions. Atomic-scale characterization, supported by theoretical calculations, revealed structures reminiscent of fused boron clusters with multiple scales of anisotropic, out-of-plane buckling. Unlike bulk boron allotropes, borophene shows metallic characteristics that are consistent with predictions of a highly anisotropic, 2D metal. Copyright © 2015, American Association for the Advancement of Science.

Self-organization of atoms coupled to a chiral reservoir

NASA Astrophysics Data System (ADS)

Eldredge, Zachary; Jarzynski, Christopher; Chang, Darrick; Gorshkov, Alexey

2016-05-01

Tightly confined modes of light, as in optical nanofibers or photonics crystal waveguides, can lead to large optical coupling in atomic systems, which mediates long-range interactions between atoms. These one-dimensional systems can naturally possess couplings which are asymmetric between modes in different directions. In this poster, we examine the self-organizing behavior of atoms in one dimension coupled to a chiral reservoir. We determine the behavior of the self-organized solution to the equations of motion in different parameter regimes, relative to both the detuning of the pump laser and the degree of reservoir chirality. In addition to the spatial configuration of self-organized atoms, we calculate possible experimental signatures.

Probing the localization of magnetic dichroism by atomic-size astigmatic and vortex electron beams

DOE PAGES

Negi, Devendra Singh; Idrobo, Juan Carlos; Rusz, Ján

2018-03-05

We report localization of a magnetic dichroic signal on atomic columns in electron magnetic circular dichroism (EMCD), probed by beam distorted by four-fold astigmatism and electron vortex beam. With astigmatic probe, magnetic signal to noise ratio can be enhanced by blocking the intensity from the central part of probe. However, the simulations show that for atomic resolution magnetic measurements, vortex beam is a more effective probe, with much higher magnetic signal to noise ratio. For all considered beam shapes, the optimal SNR constrains the signal detection at low collection angles of approximately 6–8 mrad. Irrespective of the material thickness, themore » magnetic signal remains strongly localized within the probed atomic column with vortex beam, whereas for astigmatic probes, the magnetic signal originates mostly from the nearest neighbor atomic columns. Due to excellent signal localization at probing individual atomic columns, vortex beams are predicted to be a strong candidate for studying the crystal site specific magnetic properties, magnetic properties at interfaces, or magnetism arising from individual atomic impurities.« less

Probing the localization of magnetic dichroism by atomic-size astigmatic and vortex electron beams

DOE Office of Scientific and Technical Information (OSTI.GOV)

Negi, Devendra Singh; Idrobo, Juan Carlos; Rusz, Ján

We report localization of a magnetic dichroic signal on atomic columns in electron magnetic circular dichroism (EMCD), probed by beam distorted by four-fold astigmatism and electron vortex beam. With astigmatic probe, magnetic signal to noise ratio can be enhanced by blocking the intensity from the central part of probe. However, the simulations show that for atomic resolution magnetic measurements, vortex beam is a more effective probe, with much higher magnetic signal to noise ratio. For all considered beam shapes, the optimal SNR constrains the signal detection at low collection angles of approximately 6–8 mrad. Irrespective of the material thickness, themore » magnetic signal remains strongly localized within the probed atomic column with vortex beam, whereas for astigmatic probes, the magnetic signal originates mostly from the nearest neighbor atomic columns. Due to excellent signal localization at probing individual atomic columns, vortex beams are predicted to be a strong candidate for studying the crystal site specific magnetic properties, magnetic properties at interfaces, or magnetism arising from individual atomic impurities.« less

Atomic-Scale Lightning Rod Effect in Plasmonic Picocavities: A Classical View to a Quantum Effect.

PubMed

Urbieta, Mattin; Barbry, Marc; Zhang, Yao; Koval, Peter; Sánchez-Portal, Daniel; Zabala, Nerea; Aizpurua, Javier

2018-01-23

Plasmonic gaps are known to produce nanoscale localization and enhancement of optical fields, providing small effective mode volumes of about a few hundred nm 3 . Atomistic quantum calculations based on time-dependent density functional theory reveal the effect of subnanometric localization of electromagnetic fields due to the presence of atomic-scale features at the interfaces of plasmonic gaps. Using a classical model, we explain this as a nonresonant lightning rod effect at the atomic scale that produces an extra enhancement over that of the plasmonic background. The near-field distribution of atomic-scale hot spots around atomic features is robust against dynamical screening and spill-out effects and follows the potential landscape determined by the electron density around the atomic sites. A detailed comparison of the field distribution around atomic hot spots from full quantum atomistic calculations and from the local classical approach considering the geometrical profile of the atoms' electronic density validates the use of a classical framework to determine the effective mode volume in these extreme subnanometric optical cavities. This finding is of practical importance for the community of surface-enhanced molecular spectroscopy and quantum nanophotonics, as it provides an adequate description of the local electromagnetic fields around atomic-scale features with use of simplified classical methods.

Configuration-interaction relativistic-many-body-perturbation-theory calculations of photoionization cross sections from quasicontinuum oscillator strengths

DOE PAGES

Savukov, I. M.; Filin, D. V.

2014-12-29

Many applications are in need of accurate photoionization cross sections, especially in the case of complex atoms. Configuration-interaction relativistic-many-body-perturbation theory (CI-RMBPT) has been successful in predicting atomic energies, matrix elements between discrete states, and other properties, which is quite promising, but it has not been applied to photoionization problems owing to extra complications arising from continuum states. In this paper a method that will allow the conversion of discrete CI-(R)MPBT oscillator strengths (OS) to photoionization cross sections with minimal modifications of the codes is introduced and CI-RMBPT cross sections of Ne, Ar, Kr, and Xe are calculated. A consistent agreementmore » with experiment is found. RMBPT corrections are particularly significant for Ar, Kr, and Xe and improve agreement with experimental results compared to the particle-hole CI method. As a result, the demonstrated conversion method can be applied to CI-RMBPT photoionization calculations for a large number of multivalence atoms and ions.« less

Critical assessment of Pt surface energy - An atomistic study

NASA Astrophysics Data System (ADS)

Kim, Jin-Soo; Seol, Donghyuk; Lee, Byeong-Joo

2018-04-01

Despite the fact that surface energy is a fundamental quantity in understanding surface structure of nanoparticle, the results of experimental measurements and theoretical calculations for the surface energy of pure Pt show a wide range of scattering. It is necessary to further ensure the surface energy of Pt to find the equilibrium shape and atomic configuration in Pt bimetallic nanoparticles accurately. In this article, we critically assess and optimize the Pt surface energy using a semi-empirical atomistic approach based on the second nearest-neighbor modified embedded-atom method interatomic potential. That is, the interatomic potential of pure Pt was adjusted in a way that the surface segregation tendency in a wide range of Pt binary alloys is reproduced in accordance with experimental information. The final optimized Pt surface energy (mJ/m2) is 2036 for (100) surface, 2106 for (110) surface, and 1502 for (111) surface. The potential can be utilized to find the equilibrium shape and atomic configuration of Pt bimetallic nanoparticles more accurately.

MCDF calculations of Auger cascade processes

NASA Astrophysics Data System (ADS)

Beerwerth, Randolf; Fritzsche, Stephan

2017-10-01

We model the multiple ionization of near-neutral core-excited atoms where a cascade of Auger processes leads to the emission of several electrons. We utilize the multiconfiguration Dirac-Fock (MCDF) method to generate approximate wave functions for all fine-structure levels and to account for all decays between them. This approach allows to compute electron spectra, the population of final-states and ion yields, that are accessible in many experiments. Furthermore, our approach is based on the configuration interaction method. A careful treatment of correlation between electronic configurations enables one to model three-electron processes such as an Auger decay that is accompanied by an additional shake-up transition. Here, this model is applied to the triple ionization of atomic cadmium, where we show that the decay of inner-shell 4p holes to triply-charged final states is purely due to the shake-up transition of valence 5s electrons. Contribution to the Topical Issue "Atomic and Molecular Data and their Applications", edited by Gordon W.F. Drake, Jung-Sik Yoon, Daiji Kato, Grzegorz Karwasz.

Cd (II) and holodirected lead (II) 3D-supramolecular coordination polymers based on nicotinic acid: Structure, fluorescence property and photocatalytic activity

NASA Astrophysics Data System (ADS)

Etaiw, Safaa El-din H.; Abd El-Aziz, Dina M.; Marie, Hassan; Ali, Elham

2018-05-01

Two new supramolecular coordination polymers namely {[Cd(NA)2(H2O)]}, SCP 1 and {[Pb(NA)2]}, SCP 2, (NA = nicotinate ligand) were synthesized by self-assembly method and structurally characterized by different analytical and spectroscopic methods. Single-crystal X-ray diffraction showed that SCP 1 extend in three dimensions containing bore structure where the 3D- network is constructed via interweaving zigzag chains. The Cd atom coordinates to (O4N2) atoms forming distorted-octahedral configuration. The structure of SCP 2 extend down the projection of the b-axis creating parallel zigzag 1D-chains connected by μ2-O2 atoms and H-bonds forming a holodirected lead (II) hexagonal bi-pyramid configuration. SCP 2 extend to 3D-network via coordinate and hydrogen bonds. The thermal stability, photoluminescence properties, photocatalytic activity for the degradation of methylene blue dye (MB) under UV-irradiation and sunlight irradiation were also studied.

Low-frequency Raman fingerprints of two-dimensional metal dichalcogenide layer stacking configurations

DOE PAGES

Puretzky, Alexander A.; Liang, Liangbo; Li, Xufan; ...

2015-05-12

In this study, stacked monolayers of two-dimensional (2D) materials present a new class of hybrid materials with tunable optoelectronic properties determined by their stacking orientation, order, and atomic registry. Atomic-resolution Z-contrast scanning transmission electron microscopy (AR-Z-STEM) and electron energy loss spectroscopy (EELS) can be used to determine the exact atomic registration between different layers, in few-layer 2D stacks, however fast optical characterization techniques are essential for rapid development of the field. Here, using two- and three-layer MoSe 2 and WSe 2 crystals synthesized by chemical vapor deposition we show that the generally unexplored low frequency (LF) Raman modes (< 50more » cm -1) that originate from interlayer vibrations can serve as fingerprints to characterize not only the number of layers, but also their stacking configurations. Ab initio calculations and group theory analysis corroborate the experimental assignments determined by AR-Z-STEM and show that the calculated LF mode fingerprints are related to the 2D crystal symmetries.« less

Complex multireference configuration interaction calculations for the K-vacancy Auger states of N{sup q+} (q = 2-5) ions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Peng, Yi-Geng; Data Center for High Energy Density Physics, Institute of Applied Physics and Computational Mathematics, P.O. Box 8009, Beijing 100088; Wu, Yong, E-mail: wu-yong@iapcm.ac.cn

2016-02-07

K-vacancy Auger states of N{sup q+} (q = 2-5) ions are studied by using the complex multireference single- and double-excitation configuration interaction (CMRD-CI) method. The calculated resonance parameters are in good agreement with the available experimental and theoretical data. It shows that the resonance positions and widths converge quickly with the increase of the atomic basis sets in the CMRD-CI calculations; the standard atomic basis set can be employed to describe the atomic K-vacancy Auger states well. The strong correlations between the valence and core electrons play important roles in accurately determining those resonance parameters, Rydberg electrons contribute negligibly inmore » the calculations. Note that it is the first time that the complex scaling method has been successfully applied for the B-like nitrogen. CMRD-CI is readily extended to treat the resonance states of molecules in the near future.« less

A dark-line two-dimensional magneto-optical trap of 85Rb atoms with high optical depth.

PubMed

Zhang, Shanchao; Chen, J F; Liu, Chang; Zhou, Shuyu; Loy, M M T; Wong, G K L; Du, Shengwang

2012-07-01

We describe the apparatus of a dark-line two-dimensional (2D) magneto-optical trap (MOT) of (85)Rb cold atoms with high optical depth (OD). Different from the conventional configuration, two (of three) pairs of trapping laser beams in our 2D MOT setup do not follow the symmetry axes of the quadrupole magnetic field: they are aligned with 45° angles to the longitudinal axis. Two orthogonal repumping laser beams have a dark-line volume in the longitudinal axis at their cross over. With a total trapping laser power of 40 mW and repumping laser power of 18 mW, we obtain an atomic OD up to 160 in an electromagnetically induced transparency (EIT) scheme, which corresponds to an atomic-density-length product NL = 2.05 × 10(15) m(-2). In a closed two-state system, the OD can become as large as more than 600. Our 2D MOT configuration allows full optical access of the atoms in its longitudinal direction without interfering with the trapping and repumping laser beams spatially. Moreover, the zero magnetic field along the longitudinal axis allows the cold atoms maintain a long ground-state coherence time without switching off the MOT magnetic field, which makes it possible to operate the MOT at a high repetition rate and a high duty cycle. Our 2D MOT is ideal for atomic-ensemble-based quantum optics applications, such as EIT, entangled photon pair generation, optical quantum memory, and quantum information processing.

RF Shot Noise Measurements in Au Atomic-scale Junctions

NASA Astrophysics Data System (ADS)

Chen, Ruoyu

Conduction electrons are responsible for many physical or chemical phenomena in condensed matter systems, and their behavior can be directly studied by electronic transport measurements. In conventional transport measurements, conductance or resistance is usually the focus. Such a measurement can be as simple as a quick two terminal DC check by a multi-meter, or a more sophisticated lock-in measurement of multiple higher harmonic signals synchronized to different frequencies. Conductance carries direct information about the quasi-particle density of states and the local electronic distributions, which are usually Fermi-Dirac distribution. Conductance is modified or dominated by scattering from defacts or interfaces, and could also reflect the spin-spin exchange interactions or inelastic couplings with phonons and photons. Naturally one can ask the question: is there anything else we can measure electronically, which carries extra information that a conductance measurement does not provide? One answer to this question is the electronic noise. While the conductance reflects the average charge conduction ability of a system, noise describes how the physical quantities fluctuate around their average values. Some of the fluctuations carry information about their physical origins. This thesis will focus on one particular type of the electronic noise shot noise, but other types of noise will also be introduced and discussed. We choose to measure the radio frequency component of shot noise, combining with a modulated lock-in detection technique, which provides a method to largely get rid of other unwanted low-frequency noise signals. Au atomic-scale junctions are the systems we studied here. Au is relatively well understood and will not generate too many complications, so it's ideal as the first platform for us to understand both shot noise itself and our RF technique. On the other hand, the atomic scale raises fundamental questions about electronic transport and local energy exchange and dissipation, which make our measurements fundamentally interesting. We employed two different types of mechanical controlled Au break junctions: the Scanning Tunneling Microscope(STM)-style Au break junctions, and the mechanically bending Au break junctions. We studied shot noise behaviors of individual configurations or ensemble averages over all the accessible configurations. Measurements were conducted at both room temperature and liquid He temperature. High quality shot noise measurements were demonstrated. New phenomena like anomalous excess noise enhancement at high bias voltages and non-zero shot noise variance below 1G0 were seen. We also found shot noise to be surprisingly insensitive to temperatures between 4.2K and 100K, and can be well described by the non-interacting approximation.

Multi-point laser ignition device

DOEpatents

McIntyre, Dustin L.; Woodruff, Steven D.

2017-01-17

A multi-point laser device comprising a plurality of optical pumping sources. Each optical pumping source is configured to create pumping excitation energy along a corresponding optical path directed through a high-reflectivity mirror and into substantially different locations within the laser media thereby producing atomic optical emissions at substantially different locations within the laser media and directed along a corresponding optical path of the optical pumping source. An output coupler and one or more output lenses are configured to produce a plurality of lasing events at substantially different times, locations or a combination thereof from the multiple atomic optical emissions produced at substantially different locations within the laser media. The laser media is a single continuous media, preferably grown on a single substrate.

Laser-ranging long-baseline differential atom interferometers for space

NASA Astrophysics Data System (ADS)

Chiow, Sheng-wey; Williams, Jason; Yu, Nan

2015-12-01

High-sensitivity differential atom interferometers (AIs) are promising for precision measurements in science frontiers in space, including gravity-field mapping for Earth science studies and gravitational wave detection. Difficulties associated with implementing long-baseline differential AIs have previously included the need for a high optical power, large differential Doppler shifts, and narrow dynamic range. We propose a configuration of twin AIs connected by a laser-ranging interferometer (LRI-AI) to provide precise information of the displacements between the two AI reference mirrors and also to phase-lock the two independent interferometer lasers over long distances, thereby drastically improving the practical feasibility of long-baseline differential AI measurements. We show that a properly implemented LRI-AI can achieve equivalent functionality to the conventional differential AI measurement configuration.

Diazonium functionalized graphene: microstructure, electric, and magnetic properties.

PubMed

Huang, Ping; Jing, Long; Zhu, Huarui; Gao, Xueyun

2013-01-15

The unique honeycomb lattice structure of graphene gives rise to its outstanding electronic properties such as ultrahigh carrier mobility, ballistic transport, and more. However, a crucial obstacle to its use in the electronics industry is its lack of an energy bandgap. A covalent chemistry strategy could overcome this problem, and would have the benefits of being highly controllable and stable in the ambient environment. One possible approach is aryl diazonium functionalization. In this Account, we investigate the micromolecular/lattice structure, electronic structure, and electron-transport properties of nitrophenyl-diazonium-functionalized graphene. We find that nitrophenyl groups mainly adopt random and inhomogeneous configurations on the graphene basal plane, and that their bonding with graphene carbon atoms leads to slight elongation of the graphene lattice spacing. By contrast, hydrogenated graphene has a compressed lattice. Low levels of functionalization suppressed the electric conductivity of the resulting functionalized graphene, while highly functionalized graphene showed the opposite effect. This difference arises from the competition between the charge transfer effect and the scattering enhancement effect introduced by nitrophenyl groups bonding with graphene carbon atoms. Detailed electron transport measurements revealed that the nitrophenyl diazonium functionalization locally breaks the symmetry of graphene lattice, which leads to an increase in the density of state near the Fermi level, thus increasing the carrier density. On the other hand, the bonded nitrophenyl groups act as scattering centers, lowering the mean free path of the charge carriers and suppressing the carrier mobility. In rare cases, we observed ordered configurations of nitrophenyl groups in local domains on graphene flakes due to fluctuations in the reaction processes. We describe one example of such a superlattice, with a lattice constant nearly twice of that of pristine graphene. We performed comprehensive theoretical calculations to investigate the lattice and the electronic structure of the superlattice structure. Our results reveal that it is a thermodynamically stable, spin-polarized semiconductor with a bandgap of ∼0.5 eV. Our results demonstrate the possibility of controlling graphene's electronic properties using aryl diazonium functionalization. Asymmetric addition of aryl groups to different sublattices of graphene is a promising approach for producing ferromagnetic, semiconductive graphene, which will have broad applications in the electronic industry.

The Elusive Excited Quintet [superscript 5]D of Tb(III): A Source of Luminescence and Resonance Energy Transfer in Terbium Compounds

ERIC Educational Resources Information Center

Klier, Kamil

2010-01-01

The understanding of electronic structure of atomic and molecular term states involved in spectroscopic transitions is aided by projecting combinations of micro-configurations to multi-electron states with "good" quantum numbers of angular momenta. In rare-earth (RE) compounds, atomic term labels are justifiably carried over to compounds, because…

Transition metal intercalated bilayer silicene

NASA Astrophysics Data System (ADS)

Pandey, Dhanshree; Kamal, C.; Chakrabarti, Aparna

2018-04-01

We investigate the electronic and magnetic properties of Mn, Fe and Co-intercalated silicene bilayer with AA and AB stacking by using spin polarized density functional theory. The intercalation of Mn increases the gap between the two layers of silicene due to the larger atomic radii of Mn as compared to Fe and Co. Bader charge analysis has been performed to understand the bonding between the TM and Si atoms. This also helps in explaining the magnetic moment possessed by the composite systems after intercalating TM in between the layers of bilayer silicene system. This study reveals that a significant net magnetic moment is observed in cases of Mn-intercalated silicene bilayers, whereas Fe has a very small moment of 0.78 µB in the case of AA stacking configuration only. Co intercalation leads to net zero magnetic moment. Further, we find that Fe and Co marginally favor the AB stacking whereas Mn has a slight preference of the AA over the AB configuration. The composite systems, specifically when intercalated with Fe and Co atoms, favor a hybridization which is far away from sp3-like hybridization along the plane of Si atoms in bilayer silicene.

Copper-containing monooxygenases: enzymatic and biomimetic studies of the O-atom transfer catalysis.

PubMed

Blain, Ingrid; Slama, Patrick; Giorgi, Michel; Tron, Thierry; Réglier, Marius

2002-04-01

This review reports our recent studies or the mechanism of O-atom transfer to a benzylic C-H bond promoted by Dopamine beta-Hydroxylase (DBH) and its biomimetic models. We demonstrate that it is possible to carry out parallel and comparative studies on this enzyme (DBH) and its biomimetic models with the same substrate: 2-aminoindane (3). It was chosen because its two stereogenic centers, both in benzylic positions, make it very powerful for studying the stereochemistry of an O-atom transfer reaction. DBH-catalyzed hydroxylation of 3 produced exclusively 14% of trans-(1S,2S)-2-amino-1-indanol (4) (93% ee). Studies with stereospecifically deuterium-labeled 2-aminoindanes (1R,2S)-3b and (1S,2S)-3a showed that the formation of 4 was the rcsult of an overall process with retention of configuration where an O-atom is stereospecifically inserted in the trans pro-S position of the substrate. With copper(I) and (II) complexes of IndPY2 ligands we studied the reaction with dioxygen and observed an O-atom transfer to a benzylic C-H bond which was performed in the same manner as that of DBH. With the deuterium-labeled cis-2-d-IndPY2 ligand, we demonstrated that the reaction occurs by a stereospecific process with retention of configuration. In both cases (enzymatic vs. biomimetic) the O-atom transfers occur in a two-step process involving radical intermediates.

Assigning the Cerium Oxidation State for CH2CeF2 and OCeF2 Based on Multireference Wave Function Analysis.

PubMed

Mooßen, Oliver; Dolg, Michael

2016-06-09

The geometric and electronic structure of the recently experimentally studied molecules ZCeF2 (Z = CH2, O) was investigated by density functional theory (DFT) and wave function-based ab initio methods. Special attention was paid to the Ce-Z metal-ligand bonding, especially to the nature of the interaction between the Ce 4f and the Z 2p orbitals and the possible multiconfigurational character arising from it, as well as to the assignment of an oxidation state of Ce reflecting the electronic structure. Complete active space self-consistent field (CASSCF) calculations were performed, followed by orbital rotations in the active orbital space. The methylene compound CH2CeF2 has an open-shell singlet ground state, which is characterized by a two-configurational wave function in the basis of the strongly mixed natural CASSCF orbitals. The system can also be described in a very compact way by the dominant Ce 4f(1) C 2p(1) configuration, if nearly pure Ce 4f and C 2p orbitals are used. In the basis of these localized orbitals, the molecule is almost monoconfigurational and should be best described as a Ce(III) system. The singlet ground state of the oxygen OCeF2 complex is of closed-shell character when a monoconfigurational wave function with very strongly mixed Ce 4f and O 2p CASSCF natural orbitals is used for the description. The transformation to orbitals localized on the cerium and oxygen atoms leads to a multiconfigurational wave function and reveals characteristics of a mixed valent Ce(IV)/Ce(III) compound. Additionally, the interactions of the localized active orbitals were analyzed by evaluating the expectation values of the charge fluctuation operator and the local spin operator. The Ce 4f and C 2p orbital interaction of the CH2CeF2 compound is weakly covalent and resembles the interaction of the H 1s orbitals in a stretched hydrogen dimer. In contrast, the interaction of the localized active orbitals for OCeF2 shows ionic character. Calculated vibrational Ce-C and Ce-O stretching frequencies at the DFT, CASSCF, second-order Rayleigh-Schrödinger perturbation theory (RS2C), multireference configuration interaction (MRCI), as well as single, doubles, and perturbative triples coupled cluster (CCSD(T)) level are reported and compared to experimental infrared absorption data in a Ne and Ar matrix.

Rydberg blockade in three-atom systems

NASA Astrophysics Data System (ADS)

Barredo, Daniel; Ravets, Sylvain; Labuhn, Henning; Beguin, Lucas; Vernier, Aline; Chicireanu, Radu; Nogrette, Florence; Lahaye, Thierry; Browaeys, Antoine

2014-05-01

The control of individual neutral atoms in arrays of optical tweezers is a promising avenue for quantum science and technology. Here we demonstrate unprecedented control over a system of three Rydberg atoms arranged in linear and triangular configurations. The interaction between Rydberg atoms results in the observation of an almost perfect van der Waals blockade. When the single-atom Rabi frequency for excitation to the Rydberg state is comparable to the interaction energy, we directly observe the anisotropy of the interaction between nD-states. Using the independently measured two-body interaction energy shifts we fully reproduce the dynamics of the three-atom system with a model based on a master equation without any adjustable parameter. Combined with our ability to trap single atoms in arbitrary patterns of 2D arrays of up to 100 traps separated by a few microns, these results are very promising for a scalable implementation of quantum simulation of frustrated quantum magnetism with Rydberg atoms.

Diagnosing Students’ conception on atomic structure using open ended questions

NASA Astrophysics Data System (ADS)

Fitriza, Z.; Gazali, F.

2018-05-01

This study aims to diagnose students’ conception on atomic structure concepts using open ended questions. For this reason, a 7 items of assay test was administered to 135 senior high school students from different schools in West Sumatera. The data were collected using a an open ended test which is covering the concept used in the topic Atomic Structure. The open ended test of students’ conceptual was developed to identify the alternative conceptions that student might have regarding the concepts in Atomic Structure, to measure the level of students’ conceptions, and the way of students’ thinking concerning the concepts. The results showed that students find difficulties about some concepts of Atomic structure such as atom, atomic model, electron configuration, period and group.The result of this study illuminated the concepts to be underlined in developing teaching and learning approach concerning the topic of Atomic Structure.

Atomic structure of self-organizing iridium induced nanowires on Ge(001)

NASA Astrophysics Data System (ADS)

Kabanov, N. S.; Heimbuch, R.; Zandvliet, H. J. W.; Saletsky, A. M.; Klavsyuk, A. L.

2017-05-01

The atomic structure of self-organizing iridium (Ir) induced nanowires on Ge(001) is studied by density functional theory (DFT) calculations and variable-temperature scanning tunneling microscopy. The Ir induced nanowires are aligned in a direction perpendicular to the Ge(001) substrate dimer rows, have a width of two atoms and are completely kink-less. Density functional theory calculations show that the Ir atoms prefer to dive into the Ge(001) substrate and push up the neighboring Ge substrate atoms. The nanowires are composed of Ge atoms and not Ir atoms as previously assumed. The regions in the vicinity of the nanowires are very dynamic, even at temperatures as low as 77 K. Time-resolved scanning tunneling microscopy measurements reveal that this dynamics is caused by buckled Ge substrate dimers that flip back and forth between their two buckled configurations.

First-principles study of configurational disorder in B4C using a superatom-special quasirandom structure method

NASA Astrophysics Data System (ADS)

Ektarawong, A.; Simak, S. I.; Hultman, L.; Birch, J.; Alling, B.

2014-07-01

Configurationally disordered crystalline boron carbide, with the composition B4C, is studied using first-principles calculations. We investigate both dilute and high concentrations of carbon-boron substitutional defects. For the latter purpose, we suggest a superatom's picture of the complex structure and combine it with a special quasirandom structure approach for disorder. In this way, we model a random distribution of high concentrations of the identified low-energy defects: (1) bipolar defects and (2) rotation of icosahedral carbon among the three polar-up sites. Additionally, the substitutional disorder of the icosahedral carbon at all six polar sites, as previously discussed in the literature, is also considered. Two configurational phase transitions from the ordered to the disordered configurations are predicted to take place upon an increase in temperature using a mean-field approximation for the entropy. The first transition, at 870 K, induces substitutional disorder of the icosahedral carbon atoms among the three polar-up sites; meanwhile the second transition, at 2325 K, reveals the random substitution of the icosahedral carbon atoms at all six polar sites coexisting with bipolar defects. Already the first transition removes the monoclinic distortion existing in the ordered ground-state configuration and restore the rhombohedral system (R3m). The restoration of inversion symmetry yielding the full rhombohedral symmetry (R3¯m ) on average, corresponding to what is reported in the literature, is achieved after the second transition. Investigating the effects of high pressure on the configurational stability of the disordered B4C phases reveals a tendency to stabilize the ordered ground-state configuration as the configurationally ordering/disordering transition temperature increases with pressure exerted on B4C. The electronic density of states, obtained from the disordered phases, indicates a sensitivity of the band gap to the degree of configurational disorder in B4C.

Interactions between C and Cu atoms in single-layer graphene: direct observation and modelling.

PubMed

Kano, Emi; Hashimoto, Ayako; Kaneko, Tomoaki; Tajima, Nobuo; Ohno, Takahisa; Takeguchi, Masaki

2016-01-07

Metal doping into the graphene lattice has been studied recently to develop novel nanoelectronic devices and to gain an understanding of the catalytic activities of metals in nanocarbon structures. Here we report the direct observation of interactions between Cu atoms and single-layer graphene by transmission electron microscopy. We document stable configurations of Cu atoms in the graphene sheet and unique transformations of graphene promoted by Cu atoms. First-principles calculations based on density functional theory reveal a reduction of energy barrier that caused rotation of C-C bonds near Cu atoms. We discuss two driving forces, electron irradiation and in situ heating, and conclude that the observed transformations were mainly promoted by electron irradiation. Our results suggest that individual Cu atoms can promote reconstruction of single-layer graphene.

Optimizing qPlus sensor assemblies for simultaneous scanning tunneling and noncontact atomic force microscopy operation based on finite element method analysis

DOE PAGES

Dagdeviren, Omur E.; Schwarz, Udo D.

2017-03-20

Quartz tuning forks that have a probe tip attached to the end of one of its prongs while the other prong is arrested to a holder (“qPlus” configuration) have gained considerable popularity in recent years for high-resolution atomic force microscopy imaging. The small size of the tuning forks and the complexity of the sensor architecture, however, often impede predictions on how variations in the execution of the individual assembly steps affect the performance of the completed sensor. Extending an earlier study that provided numerical analysis of qPlus-style setups without tips, this work quantifies the influence of tip attachment on themore » operational characteristics of the sensor. The results using finite element modeling show in particular that for setups that include a metallic tip that is connected via a separate wire to enable the simultaneous collection of local forces and tunneling currents, the exact realization of this wire connection has a major effect on sensor properties such as spring constant, quality factor, resonance frequency, and its deviation from an ideal vertical oscillation.« less

Optimizing qPlus sensor assemblies for simultaneous scanning tunneling and noncontact atomic force microscopy operation based on finite element method analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dagdeviren, Omur E.; Schwarz, Udo D.

Quartz tuning forks that have a probe tip attached to the end of one of its prongs while the other prong is arrested to a holder (“qPlus” configuration) have gained considerable popularity in recent years for high-resolution atomic force microscopy imaging. The small size of the tuning forks and the complexity of the sensor architecture, however, often impede predictions on how variations in the execution of the individual assembly steps affect the performance of the completed sensor. Extending an earlier study that provided numerical analysis of qPlus-style setups without tips, this work quantifies the influence of tip attachment on themore » operational characteristics of the sensor. The results using finite element modeling show in particular that for setups that include a metallic tip that is connected via a separate wire to enable the simultaneous collection of local forces and tunneling currents, the exact realization of this wire connection has a major effect on sensor properties such as spring constant, quality factor, resonance frequency, and its deviation from an ideal vertical oscillation.« less

Combination of first-principles molecular dynamics and XANES simulations for LiCoO2-electrolyte interfacial reactions in a lithium-ion battery

NASA Astrophysics Data System (ADS)

Tamura, Tomoyuki; Kohyama, Masanori; Ogata, Shuji

2017-07-01

We performed a first-principles molecular dynamics (FPMD) simulation of the interfacial reactions between a LiCoO2 electrode and a liquid ethylene carbonate (EC) electrolyte. For configurations during the FPMD simulation, we also performed first-principles Co K-edge x-ray absorption near-edge structure (XANES) simulations, which can properly reproduce the bulk and surface spectra of LiCoO2. We observed strong absorption of an EC molecule on the LiCoO2 {110} surface, involving ring opening of the molecule, bond formation between oxygen atoms in the molecule and surface Co ions, and emission of one surface Li ion, while all the surface Co ions remain Co3 +. The surface Co ions having the bond with an oxygen atom in the molecule showed remarkable changes in simulated K-edge spectra which are similar to those of the in situ observation under electrolyte soaking [D. Takamatsu et al., Angew. Chem., Int. Ed. 51, 11597 (2012), 10.1002/anie.201203910]. Thus, the local environmental changes of surface Co ions due to the reactions with an EC molecule can explain the experimental spectrum changes.

Quantitative ion beam analysis of M-C-O systems: application to an oxidized uranium carbide sample

NASA Astrophysics Data System (ADS)

Martin, G.; Raveu, G.; Garcia, P.; Carlot, G.; Khodja, H.; Vickridge, I.; Barthe, M. F.; Sauvage, T.

2014-04-01

A large variety of materials contain both carbon and oxygen atoms, in particular oxidized carbides, carbon alloys (as ZrC, UC, steels, etc.), and oxycarbide compounds (SiCO glasses, TiCO, etc.). Here a new ion beam analysis methodology is described which enables quantification of elemental composition and oxygen concentration profile over a few microns. It is based on two procedures. The first, relative to the experimental configuration relies on a specific detection setup which is original in that it enables the separation of the carbon and oxygen NRA signals. The second concerns the data analysis procedure i.e. the method for deriving the elemental composition from the particle energy spectrum. It is a generic algorithm and is here successfully applied to characterize an oxidized uranium carbide sample, developed as a potential fuel for generation IV nuclear reactors. Furthermore, a micro-beam was used to simultaneously determine the local elemental composition and oxygen concentration profiles over the first microns below the sample surface. This method is adapted to the determination of the composition of M?C?O? compounds with a sensitivity on elemental atomic concentrations around 1000 ppm.

Domain pinning near a single-grain boundary in tetragonal and rhombohedral lead zirconate titanate films

DOE PAGES

Marincel, Dan M.; Zhang, H. R.; Briston, J.; ...

2015-04-27

The interaction of grain boundaries with ferroelectric domain walls strongly influences the extrinsic contribution to piezoelectric activity in Pb(Zr,Ti)O 3 (PZT), ubiquitous in modern transducers and actuators. However, the fundamental understanding of these phenomena has been limited by complex mechanisms originating from the interplay of atomic-level domain wall pinning, collective domain wall dynamics, and emergent mesoscopic behavior. This contribution utilizes engineered grain boundaries created by depositing epitaxial PZT films with various Zr:Ti ratio onto 24º SrTiO 3 tilt bicrystals. The nonlinear piezoelectric response and surface domain structure across the boundary are investigated using piezoresponse force microscopy whilst cross section domainmore » structure is studied using transmission electron microscopy. The grain boundary reduces domain wall motion over a width of 800±70 nm for PZT 45:55 and 450±30 nm for PZT 52:48. Phase field modeling provides an understanding of the elastic and electric fields associated with the grain boundary and local domain configurations. In conclusion, this study demonstrates that complex mesoscopic behaviors can be explored to complement atomic-level pictures of the material system.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Berrondo, M.

We calculate the equilibrium configurations of a system of deuterium atoms absorbed in palladium. The interaction potential energy is taken as a sum of pair functionals including non-additive effects, which are crucial for this case. We conclude from our calculations that the most probable configuration for the deuterium in the {beta}-phase of PdD involves at least a partial occupation of the tetrahedral sites of the fcc palladium unit cell.

Theoretical study of Ag doping-induced vacancies defects in armchair graphene

NASA Astrophysics Data System (ADS)

Benchallal, L.; Haffad, S.; Lamiri, L.; Boubenider, F.; Zitoune, H.; Kahouadji, B.; Samah, M.

2018-06-01

We have performed a density functional theory (DFT) study of the absorption of silver atoms (Ag,Ag2 and Ag3) in graphene using SIESTA code, in the generalized gradient approximation (GGA). The absorption energy, geometry, magnetic moments and charge transfer of Ag clusters-graphene system are calculated. The minimum energy configuration demonstrates that all structures remain planar and silver atoms fit into this plane. The charge transfer between the silver clusters and carbon atoms constituting the graphene surface is an indicative of a strong bond. The structure doped with a single silver atom has a magnetic moment and the two other are nonmagnetic.

cgDNA: a software package for the prediction of sequence-dependent coarse-grain free energies of B-form DNA.

PubMed

Petkevičiūtė, D; Pasi, M; Gonzalez, O; Maddocks, J H

2014-11-10

cgDNA is a package for the prediction of sequence-dependent configuration-space free energies for B-form DNA at the coarse-grain level of rigid bases. For a fragment of any given length and sequence, cgDNA calculates the configuration of the associated free energy minimizer, i.e. the relative positions and orientations of each base, along with a stiffness matrix, which together govern differences in free energies. The model predicts non-local (i.e. beyond base-pair step) sequence dependence of the free energy minimizer. Configurations can be input or output in either the Curves+ definition of the usual helical DNA structural variables, or as a PDB file of coordinates of base atoms. We illustrate the cgDNA package by comparing predictions of free energy minimizers from (a) the cgDNA model, (b) time-averaged atomistic molecular dynamics (or MD) simulations, and (c) NMR or X-ray experimental observation, for (i) the Dickerson-Drew dodecamer and (ii) three oligomers containing A-tracts. The cgDNA predictions are rather close to those of the MD simulations, but many orders of magnitude faster to compute. Both the cgDNA and MD predictions are in reasonable agreement with the available experimental data. Our conclusion is that cgDNA can serve as a highly efficient tool for studying structural variations in B-form DNA over a wide range of sequences. © The Author(s) 2014. Published by Oxford University Press on behalf of Nucleic Acids Research.

Tunable electronic properties of graphene through controlling bonding configurations of doped nitrogen atoms.

PubMed

Zhang, Jia; Zhao, Chao; Liu, Na; Zhang, Huanxi; Liu, Jingjing; Fu, Yong Qing; Guo, Bin; Wang, Zhenlong; Lei, Shengbin; Hu, PingAn

2016-06-21

Single-layer and mono-component doped graphene is a crucial platform for a better understanding of the relationship between its intrinsic electronic properties and atomic bonding configurations. Large-scale doped graphene films dominated with graphitic nitrogen (GG) or pyrrolic nitrogen (PG) were synthesized on Cu foils via a free radical reaction at growth temperatures of 230-300 °C and 400-600 °C, respectively. The bonding configurations of N atoms in the graphene lattices were controlled through reaction temperature, and characterized using Raman spectroscopy, X-ray photoelectron spectroscopy and scanning tunneling microscope. The GG exhibited a strong n-type doping behavior, whereas the PG showed a weak n-type doping behavior. Electron mobilities of the GG and PG were in the range of 80.1-340 cm(2) V(-1)·s(-1) and 59.3-160.6 cm(2) V(-1)·s(-1), respectively. The enhanced doping effect caused by graphitic nitrogen in the GG produced an asymmetry electron-hole transport characteristic, indicating that the long-range scattering (ionized impurities) plays an important role in determining the carrier transport behavior. Analysis of temperature dependent conductance showed that the carrier transport mechanism in the GG was thermal excitation, whereas that in the PG, was a combination of thermal excitation and variable range hopping.

Tunable electronic properties of graphene through controlling bonding configurations of doped nitrogen atoms

PubMed Central

Zhang, Jia; Zhao, Chao; Liu, Na; Zhang, Huanxi; Liu, Jingjing; Fu, Yong Qing; Guo, Bin; Wang, Zhenlong; Lei, Shengbin; Hu, PingAn

2016-01-01

Single–layer and mono–component doped graphene is a crucial platform for a better understanding of the relationship between its intrinsic electronic properties and atomic bonding configurations. Large–scale doped graphene films dominated with graphitic nitrogen (GG) or pyrrolic nitrogen (PG) were synthesized on Cu foils via a free radical reaction at growth temperatures of 230–300 °C and 400–600 °C, respectively. The bonding configurations of N atoms in the graphene lattices were controlled through reaction temperature, and characterized using Raman spectroscopy, X–ray photoelectron spectroscopy and scanning tunneling microscope. The GG exhibited a strong n–type doping behavior, whereas the PG showed a weak n–type doping behavior. Electron mobilities of the GG and PG were in the range of 80.1–340 cm2 V−1·s−1 and 59.3–160.6 cm2 V−1·s−1, respectively. The enhanced doping effect caused by graphitic nitrogen in the GG produced an asymmetry electron–hole transport characteristic, indicating that the long–range scattering (ionized impurities) plays an important role in determining the carrier transport behavior. Analysis of temperature dependent conductance showed that the carrier transport mechanism in the GG was thermal excitation, whereas that in the PG, was a combination of thermal excitation and variable range hopping. PMID:27325386

Cluster model studies of anion and molecular specificities via electrospray ionization photoelectron spectroscopy

DOE PAGES

Wang, Xue -Bin

2017-01-06

Ion specificity, a widely observed macroscopic phenomenon in condensed phases and at interfaces, is essentially a fundamental chemical physical issue. We have been investigating such effects using cluster models in an “atom-by-atom” and “molecule-by-molecule” fashion not possible with condensed-phase methods. We use electrospray ionization (ESI) to generate molecular and ionic clusters to simulate key molecular entities involved in local binding regions, and characterize them employing negative ion photoelectron spectroscopy (NIPES). Inter- and intramolecular interactions and binding configurations are directly obtained as functions of cluster size and composition, providing insightful molecular-level description and characterization over the local active sites that playmore » crucial roles in determining solution chemistry and condensed phase phenomena. Finally, the topics covered in this article are relevant to a wide scope of research fields ranging from ion specific effects in electrolyte solutions, ion selectivity/recognition in normal functioning of life, to molecular specificity in aerosol particle formation, as well as in rational material design and synthesis.« less

Atomic Structure and Properties of Extended Defects in Silicon

DOE Office of Scientific and Technical Information (OSTI.GOV)

Buczko, R.; Chisholm, M.F.; Kaplan, T.

1998-10-15

The Z-contrast technique represents a new approach to high-resolution electron microscopy allowing for the first time incoherent imaging of materials on the atomic scale. The key advantages of the technique, an intrinsically higher resolution limit and directly interpretable, compositionally sensitive imaging, allow a new level of insight into the atomic configurations of extended defects in silicon. This experimental technique has been combined with theoretical calculations (a combination of first principles, tight binding, and classical methods) to extend this level of insight by obtaining the energetic and electronic structure of the defects.

Atomic and electronic structure of the silicon and silicon-metal Si{sub 20}, Si{sub 20}{sup -}, NaSi{sub 20}, KSi{sub 20} nanoparticles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Borshch, N. A., E-mail: ssd18@phys.vsu.ru; Pereslavtseva, N. S.; Kurganskii, S. I.

The results of atomic-structure optimization and calculation of the electronic structure of the Si{sub 20}, Si{sub 20}{sup -}, NaSi{sub 20}, and KSi{sub 20} clusters are reported. The PM3 and AM1 semiempirical methods were used in the calculations. It is shown that the Na and K atoms stabilize the fullerene-like silicon structure. The effect of configuration of the clusters on their electronic structure is analyzed.

Singlet vs. triplet interelectronic repulsion in confined atoms

NASA Astrophysics Data System (ADS)

Sarsa, A.; Buendía, E.; Gálvez, F. J.; Katriel, J.

2018-06-01

Hund's multiplicity rule invariably holds for the ground configurations of few-electron atoms as well as those of multi-electron quantum dots. However, the ordering of the corresponding interelectronic repulsions exhibits a reversal in the former but not in the latter system, upon varying the system parameters. Here, we investigate the transition between these two types of behaviour by studying few-electron atoms confined in spherical cavities. "Counter-intuitive" ordering of the interelectronic repulsions is confirmed when the nuclear charge is low enough and the cavity radius is large enough.

Simplified configuration for the combustor of an oil burner using a low pressure, high flow air-atomizing nozzle

DOEpatents

Butcher, Thomas A.; Celebi, Yusuf; Fisher, Leonard

2000-09-15

The invention relates to clean burning of fuel oil with air. More specifically, to a fuel burning combustion head using a low-pressure, high air flow atomizing nozzle so that there will be a complete combustion of oil resulting in a minimum emission of pollutants. The improved fuel burner uses a low pressure air atomizing nozzle that does not result in the use of additional compressors or the introduction of pressurized gases downstream, nor does it require a complex design. Inventors:

Squeezing via two-photon transitions

NASA Astrophysics Data System (ADS)

Savage, C. M.; Walls, D. F.

1986-05-01

The squeezing spectrum for a cavity field mode interacting with an ensemble of three-level 'Lambda-configuration' atoms by an effective two-photon transition is calculated. The advantage of the three-level Lambda system as a squeezing medium, that is, optical nonlinearity without atomic saturation, has recently been pointed out by Reid, Walls, and Dalton. Perfect squeezing is predicted at the turning points for dispersive optical bistability and good squeezing for a range of other cases. Three-level ladder atoms interacting by an effective two-photon transition are also shown to give perfect squeezing in the dispersive limit.

Atomic configurations at InAs partial dislocation cores associated with Z-shape faulted dipoles.

PubMed

Li, Luying; Gan, Zhaofeng; McCartney, Martha R; Liang, Hanshuang; Yu, Hongbin; Gao, Yihua; Wang, Jianbo; Smith, David J

2013-11-15

The atomic arrangements of two types of InAs dislocation cores associated by a Z-shape faulted dipole are observed directly by aberration-corrected high-angle annular-dark-field imaging. Single unpaired columns of different atoms in a matrix of dumbbells are clearly resolved, with observable variations of bonding lengths due to excess Coulomb force from bare ions at the dislocation core. The corresponding geometric phase analysis provides confirmation that the dislocation cores serve as origins of strain field inversion while stacking faults maintain the existing strain status.

Hydrogen atom abstraction from aldehydes - OH + H2CO and O + H2CO

NASA Technical Reports Server (NTRS)

Dupuis, M.; Lester, W. A., Jr.

1984-01-01

The essential features of the potential energy surfaces governing hydrogen abstraction from formaldehyde by oxygen atom and hydroxyl radical have been characterized with ab inito multiconfiguration Hartree-Fock (MCHF) and configuration interaction (CI) wave functions. The results are consistent with a very small activation energy for the OH + H2CO reaction, and an activation energy of a few kcal/mol for the O + H2CO reaction. In the transition state structure of both systems, the attacking oxygen atom is nearly collinear with the attacked CH bond.

An electromechanical Ising Hamiltonian

PubMed Central

Mahboob, Imran; Okamoto, Hajime; Yamaguchi, Hiroshi

2016-01-01

Solving intractable mathematical problems in simulators composed of atoms, ions, photons, or electrons has recently emerged as a subject of intense interest. We extend this concept to phonons that are localized in spectrally pure resonances in an electromechanical system that enables their interactions to be exquisitely fashioned via electrical means. We harness this platform to emulate the Ising Hamiltonian whose spin 1/2 particles are replicated by the phase bistable vibrations from the parametric resonances of multiple modes. The coupling between the mechanical spins is created by generating two-mode squeezed states, which impart correlations between modes that can imitate a random, ferromagnetic state or an antiferromagnetic state on demand. These results suggest that an electromechanical simulator could be built for the Ising Hamiltonian in a nontrivial configuration, namely, for a large number of spins with multiple degrees of coupling. PMID:28861469

An electromechanical Ising Hamiltonian.

PubMed

Mahboob, Imran; Okamoto, Hajime; Yamaguchi, Hiroshi

2016-06-01

Solving intractable mathematical problems in simulators composed of atoms, ions, photons, or electrons has recently emerged as a subject of intense interest. We extend this concept to phonons that are localized in spectrally pure resonances in an electromechanical system that enables their interactions to be exquisitely fashioned via electrical means. We harness this platform to emulate the Ising Hamiltonian whose spin 1/2 particles are replicated by the phase bistable vibrations from the parametric resonances of multiple modes. The coupling between the mechanical spins is created by generating two-mode squeezed states, which impart correlations between modes that can imitate a random, ferromagnetic state or an antiferromagnetic state on demand. These results suggest that an electromechanical simulator could be built for the Ising Hamiltonian in a nontrivial configuration, namely, for a large number of spins with multiple degrees of coupling.

Heat-Pipe Bismuth Laser; Examination of Laser Action at 4722A in Bismuth Vapor

DTIC Science & Technology

1976-11-01

11, 15(1975). of Type 6p 3 -6p 2 7s in the Bismuth Atomic Spectrum in Intermediate Coupling," Acta Physica Polonica A47, 231(1975). 19. A.N. Nesmeyanov...Calculated Transit n Probabilities and Lifetimes for the First Excited Configuration np (n+l)s in the Neutral As, Sb and Bi Atoms, " Physica Scripta

Structural, electronic and vibrational properties of small GaxNy (x+y = 2 5) nanoclusters: a B3LYP-DFT study

NASA Astrophysics Data System (ADS)

Yadav, P. S.; Yadav, R. K.; Agrawal, B. K.

2007-02-01

An ab initio study of the stability, structural and electronic properties has been made for 49 gallium nitride nanoclusters, GaxNy (x+y = 2-5). Among the various configurations corresponding to a fixed x+y = n value, the configuration possessing the maximum value of binding energy (BE) is named as the most stable structure. The vibrational and optical properties have been investigated only for the most stable structures. A B3LYP-DFT/6-311G(3df) method has been employed to optimize the geometries of the nanoclusters fully. The binding energies (BEs), highest-occupied and lowest-unoccupied molecular orbital (HOMO-LUMO) gaps and the bond lengths have been obtained for all the clusters. We have considered the zero-point energy (ZPE) corrections ignored by the earlier workers. The adiabatic and vertical ionization potentials (IPs) and electron affinities (EAs), charge on atoms, dipole moments, vibrational frequencies, infrared intensities (IR Int.), relative infrared intensities (Rel. IR Int.) and Raman scattering activities have been investigated for the most stable structures. The configurations containing the N atoms in majority are seen to be the most stable structures. The strong N-N bond has an important role in stabilizing the clusters. For clusters containing one Ga atom and all the others as N atoms, the BE increases monotonically with the number of the N atoms. The HOMO-LUMO gap and IP fluctuate with the cluster size n, having larger values for the clusters containing odd number of N atoms. On the other hand, the EA decreases with the cluster size up to n = 3, and shows slow fluctuations thereafter for the larger clusters. In general, the adiabatic IP (EA) is smaller (greater) than the vertical IP (EA) because of the lower energies of the most stable ground state of the cationic (anionic) clusters. The optical absorption spectrum or electron energy loss spectrum (EELS) is unique for every cluster, and may be used to characterize a specific cluster. All the predicted physical quantities are in good agreement with the experimental data wherever available. The growth of these most stable structures should be possible in experiments.

Configuring pnicogen rings in skutterudites for low phonon conductivity

NASA Astrophysics Data System (ADS)

Uher, Ctirad

2013-03-01

During the past dozen or so years, skutterudites have attracted much interest as prospective thermoelectric materials for power-generation applications in the temperature range 500K - 850K. Primary interest was focused on filled forms of skutterudites where loosely-bonded filler species resonantly scatter normal phonon modes of the structure thus reducing the lattice thermal conductivity. Using this approach with multiple fillers and incorporating various forms of nanoinclusions, impressive figures of merit ZT = 1.5-1.7 have been reported with n-type filled skutterudites. Since the dominant heat-carrying modes in skutterudites are associated with vibrations of the pnicogen rings, disruptions of the ring structure by substitutional alloying should be a similarly effective approach of lowering the lattice thermal conductivity. In this talk I discuss our recent work exploring alloying configurations of pnicogen rings that yield particularly low values of the thermal conductivity. We found that compensated double-substitution (replacing two Sb atoms with one atom each from the column IV and column VI elements) is a very effective approach. Our ab initio calculations, in combination with a cluster expansion, have allowed us to identify stable alloy configurations on the Sb rings. Subsequent molecular and lattice dynamics simulations on low energy configurations established the range of atomic displacement parameters and values of the thermal conductivity. Theoretical results turned out to be in good agreement with our experimental thermal conductivity values. Combining both approaches of compensated double-substitution and filling of structural cages should be an effective way of further improving the thermoelectric figure of merit of skutterudites. Work supported by the Center for Solar and Thermal Energy Conversion, and Enegy Frontier Research Center funded by the Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0000957

Ab Initio Study of Aluminium Impurity and Interstitial-Substitutional Complexes in Ge Using a Hybrid Functional (HSE)

NASA Astrophysics Data System (ADS)

Igumbor, E.; Mapasha, R. E.; Meyer, W. E.

2017-07-01

The results of an ab initio modelling of aluminium substitutional impurity ({\\hbox {Al}}_Ge), aluminium interstitial in Ge [{\\hbox {I}}_Al for the tetrahedral (T) and hexagonal (H) configurations] and aluminium interstitial-substitutional pairs in Ge ({\\hbox {I}}_Al{\\hbox {Al}}_Ge) are presented. For all calculations, the hybrid functional of Heyd, Scuseria, and Ernzerhof in the framework of density functional theory was used. Defects formation energies, charge state transition levels and minimum energy configurations of the {\\hbox {Al}}_Ge, {\\hbox {I}}_Al and {\\hbox {I}}_Al{\\hbox {Al}}_Ge were obtained for -2, -1, 0, +1 and +2 charge states. The calculated formation energy shows that for the neutral charge state, the {\\hbox {I}}_Al is energetically more favourable in the T than the H configuration. The {\\hbox {I}}_Al{\\hbox {Al}}_Ge forms with formation energies of -2.37 eV and -2.32 eV, when the interstitial atom is at the T and H sites, respectively. The {\\hbox {I}}_Al{\\hbox {Al}}_Ge is energetically more favourable when the interstitial atom is at the T site with a binding energy of 0.8 eV. The {\\hbox {I}}_Al in the T configuration, induced a deep donor (+2/+1) level at EV+0.23 eV and the {\\hbox {Al}}_Ge induced a single acceptor level (0/-1) at EV+0.14 eV in the band gap of Ge. The {\\hbox {I}}_Al{\\hbox {Al}}_Ge induced double-donor levels are at E_V+0.06 and E_V+0.12 eV, when the interstitial atom is at the T and H sites, respectively. The {\\hbox {I}}_Al and {\\hbox {I}}_Al{\\hbox {Al}}_Ge exhibit properties of charge state-controlled metastability.

Locality of correlation in density functional theory.

PubMed

Burke, Kieron; Cancio, Antonio; Gould, Tim; Pittalis, Stefano

2016-08-07

The Hohenberg-Kohn density functional was long ago shown to reduce to the Thomas-Fermi (TF) approximation in the non-relativistic semiclassical (or large-Z) limit for all matter, i.e., the kinetic energy becomes local. Exchange also becomes local in this limit. Numerical data on the correlation energy of atoms support the conjecture that this is also true for correlation, but much less relevant to atoms. We illustrate how expansions around a large particle number are equivalent to local density approximations and their strong relevance to density functional approximations. Analyzing highly accurate atomic correlation energies, we show that EC → -AC ZlnZ + BCZ as Z → ∞, where Z is the atomic number, AC is known, and we estimate BC to be about 37 mhartree. The local density approximation yields AC exactly, but a very incorrect value for BC, showing that the local approximation is less relevant for the correlation alone. This limit is a benchmark for the non-empirical construction of density functional approximations. We conjecture that, beyond atoms, the leading correction to the local density approximation in the large-Z limit generally takes this form, but with BC a functional of the TF density for the system. The implications for the construction of approximate density functionals are discussed.

Localization of atomic excitation beyond the diffraction limit using electromagnetically induced transparency

NASA Astrophysics Data System (ADS)

Miles, J. A.; Das, Diptaranjan; Simmons, Z. J.; Yavuz, D. D.

2015-09-01

We experimentally demonstrate the localization of excitation between hyperfine ground states of 87Rb atoms to as small as λ /13 -wide spatial regions. We use ultracold atoms trapped in a dipole trap and utilize electromagnetically induced transparency (EIT) for the atomic excitation. The localization is achieved by combining a spatially varying coupling laser (standing wave) with the intensity dependence of EIT. The excitation is fast (150 ns laser pulses) and the dark-state fidelity can be made higher than 94% throughout the standing wave. Because the width of the localized regions is much smaller than the wavelength of the driving light, traditional optical imaging techniques cannot resolve the localized features. Therefore, to measure the excitation profile, we use an autocorrelation-like method where we perform two EIT sequences separated by a time delay, during which we move the standing wave.

Probing the effect of electron channelling on atomic resolution energy dispersive X-ray quantification.

PubMed

MacArthur, Katherine E; Brown, Hamish G; Findlay, Scott D; Allen, Leslie J

2017-11-01

Advances in microscope stability, aberration correction and detector design now make it readily possible to achieve atomic resolution energy dispersive X-ray mapping for dose resilient samples. These maps show impressive atomic-scale qualitative detail as to where the elements reside within a given sample. Unfortunately, while electron channelling is exploited to provide atomic resolution data, this very process makes the images rather more complex to interpret quantitatively than if no electron channelling occurred. Here we propose small sample tilt as a means for suppressing channelling and improving quantification of composition, whilst maintaining atomic-scale resolution. Only by knowing composition and thickness of the sample is it possible to determine the atomic configuration within each column. The effects of neighbouring atomic columns with differing composition and of residual channelling on our ability to extract exact column-by-column composition are also discussed. Copyright © 2017 Elsevier B.V. All rights reserved.

0.75 atoms improve the clock signal of 10,000 atoms

NASA Astrophysics Data System (ADS)

Kruse, I.; Lange, K.; Peise, J.; Lücke, B.; Pezzè, L.; Arlt, J.; Ertmer, W.; Lisdat, C.; Santos, L.; Smerzi, A.; Klempt, C.

2017-02-01

Since the pioneering work of Ramsey, atom interferometers are employed for precision metrology, in particular to measure time and to realize the second. In a classical interferometer, an ensemble of atoms is prepared in one of the two input states, whereas the second one is left empty. In this case, the vacuum noise restricts the precision of the interferometer to the standard quantum limit (SQL). Here, we propose and experimentally demonstrate a novel clock configuration that surpasses the SQL by squeezing the vacuum in the empty input state. We create a squeezed vacuum state containing an average of 0.75 atoms to improve the clock sensitivity of 10,000 atoms by 2.05 dB. The SQL poses a significant limitation for today's microwave fountain clocks, which serve as the main time reference. We evaluate the major technical limitations and challenges for devising a next generation of fountain clocks based on atomic squeezed vacuum.

Compact atom interferometer using single laser

NASA Astrophysics Data System (ADS)

Chiow, Sheng-wey; Yu, Nan

2018-06-01

A typical atom interferometer requires vastly different laser frequencies at different stages of operation, e.g., near resonant light for laser cooling and far detuned light for atom optics, such that multiple lasers are typically employed. The number of laser units constrains the achievable minimum size and power in practical devices for resource critical environments such as space. We demonstrate a compact atom interferometer accelerometer operated by a single diode laser. This is achieved by dynamically changing the laser output frequency in GHz range while maintaining spectroscopic reference to an atomic transition via a sideband generated by phase modulation. At the same time, a beam path sharing configuration is also demonstrated for a compact sensor head design, in which atom interferometer beams share the same path as that of the cooling beam. This beam path sharing also significantly simplifies three-axis atomic accelerometry in microgravity using single sensor head.

Thermogravimetric analysis of the interaction of ferromagnetic metal atom and multiwalled carbon nanotubes.

PubMed

Rawat, Naveen; Gudyaka, Russel; Kumar, Mohit; Joshi, Bharat; Santhanam, Kalathur S V

2008-04-01

This paper describes the thermal oxidative behavior of atomized iron or atomized cobalt in the presence of multiwalled carbon nanotubes (MWCNT). The thermogravimetric analysis shows the atomized iron thermal oxidation starts at about 500 degrees C that is absent when the atomized iron is sintered with multiwalled carbon naonotubes. The thermal oxidation of iron in the sintered samples requires the collapse of the multiwalled carbon nanotubes. A similar behavior is observed with atomized cobalt when its oxidation requires the collapse of the nanotubes. This thermal oxidative shift is interpreted as due to the atomized iron or atomized cobalt atom experiencing extensive overlap and confinement effect with multiwalled carbon nanotubes causing a spin transfer. This confinement effect is suggested to produce a transformation of iron from the outermost electronic distribution of 3d64s2 to an effective configuration of 3d84s0 and for cobalt 3d74s2 to 3d94s0 producing spintronics effect.

Repetitive Interrogation of 2-Level Quantum Systems

NASA Technical Reports Server (NTRS)

Prestage, John D.; Chung, Sang K.

2010-01-01

Trapped ion clocks derive information from a reference atomic transition by repetitive interrogations of the same quantum system, either a single ion or ionized gas of many millions of ions. Atomic beam frequency standards, by contrast, measure reference atomic transitions in a continuously replenished "flow through" configuration where initial ensemble atomic coherence is zero. We will describe some issues and problems that can arise when atomic state selection and preparation of the quantum atomic system is not completed, that is, optical pumping has not fully relaxed the coherence and also not fully transferred atoms to the initial state. We present a simple two-level density matrix analysis showing how frequency shifts during the state-selection process can cause frequency shifts of the measured clock transition. Such considerations are very important when a low intensity lamp light source is used for state selection, where there is relatively weak relaxation and re-pumping of ions to an initial state and much weaker 'environmental' relaxation of the atomic coherence set-up in the atomic sample.

Atomically resolved structure of ligand-protected Au{sub 9} clusters on TiO{sub 2} nanosheets using aberration-corrected STEM

DOE Office of Scientific and Technical Information (OSTI.GOV)

Al Qahtani, Hassan S.; Andersson, Gunther G., E-mail: gunther.andersson@flinders.edu.au, E-mail: nakayama.tomonobu@nims.go.jp; Kimoto, Koji

2016-03-21

Triphenylphosphine ligand-protected Au{sub 9} clusters deposited onto titania nanosheets show three different atomic configurations as observed by scanning transmission electron microscopy. The configurations observed are a 3-dimensional structure, corresponding to the previously proposed Au{sub 9} core of the clusters, and two pseudo-2-dimensional (pseudo-2D) structures, newly found by this work. With the help of density functional theory (DFT) calculations, the observed pseudo-2D structures are attributed to the low energy, de-ligated structures formed through interaction with the substrate. The combination of scanning transmission electron microscopy with DFT calculations thus allows identifying whether or not the deposited Au{sub 9} clusters have been de-ligatedmore » in the deposition process.« less

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

PubMed

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

2015-05-28

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

Local structure and polarization resistance of Ce doped SrMnO{sub 3} using extended x-ray fine structure analysis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ryu, Jiseung; Lee, Heesoo, E-mail: heesoo@pusan.ac.kr

2014-09-15

Changes to the local structure of Sr and Mn atoms in Sr{sub 1−x}Ce{sub x}MnO{sub 3} (SCM) according to increasing Ce content and the effect of the structural change on the polarization resistance of SCM were investigated. The reduction of manganese was confirmed by the absorption edge shift of the Mn K-edge toward lower energies. The noise of oscillation in extended X-ray absorption fine structure k{sup 3}χ data at Mn K-edge reveals the distortion of the local structure of Mn atoms, and the peak that indicates the bonding length of Mn-O, Sr/Ce, and -Mn decreased with the addition of Ce contentmore » in Fourier transformations of the Mn K-edge. The distortion of the local structure at Mn atoms was affected by the reduced manganese ions having larger ionic radii than Mn{sup 4+}. Meanwhile, few distortions of local atomic structures of Sr atoms occurred, and the average nearest neighboring distances of Sr-O and Sr-Mn are ∼2.13 Å and ∼2.95 Å, respectively. The average bonding lengths of the Ce-O and Ce-Mn increased because the ionic radius of substituted Ce ion with 12 coordination number is smaller than that of Sr ion, which leads the reduction of Mn ions and the distortion of local structure at the substituted A-site. Therefore, we reasoned that the distortion of the local atomic structure at Mn atoms in MnO{sub 6} and Ce atoms in A-site is one of the causes for interrupting oxygen ion transfers as a geometric factor, which results in an increase in the polarization resistance of SCM within the Ce composition range from 10 mol. % to 30 mol. %.« less

Study of diffusion and local structure of sodium-silicate liquid: the molecular dynamic simulation

NASA Astrophysics Data System (ADS)

Hung, Pham Khac; Noritake, Fumiya; San, Luyen Thi; Van, To Ba; Vinh, Le The

2017-10-01

A systematic analysis on sodium-silicate melt with various silica contents was carried out. The simulation revealed two diffusion mechanisms occurred in the melt: the bond-breaking and hopping between sites. The local structure was analyzed through T-simplexes. It was revealed that T-clusters have a non-spherical shape and represent the diffusion channel, in which Na atoms are dominant, but no any O atoms are located. The SiO2-poor melt acquires a long channel. In contrast, the SiO2-rich melt consists of unconnected short channels. The simulation also revealed the immobile and mobile regions which differ in local structure and constituent composition. We propose a new CL-function to characterizing the spatial distribution of different atom component. The spatial distribution of mobile and immobile atoms is found quite different. In particular, the immobile atoms are concentrated in high-density regions possessing very large density of immobile atoms. The spatial distribution of mobile atoms in contrast is more homogeneous.

Laser Induced Breakdown Spectroscopy Based on Single Beam Splitting and Geometric Configuration for Effective Signal Enhancement

PubMed Central

Yang, Guang; Lin, Qingyu; Ding, Yu; Tian, Di; Duan, Yixiang

2015-01-01

A new laser induced breakdown spectroscopy (LIBS) based on single-beam-splitting (SBS) and proper optical geometric configuration has been initially explored in this work for effective signal enhancement. In order to improve the interaction efficiency of laser energy with the ablated material, a laser beam operated in pulse mode was divided into two streams to ablate/excite the target sample in different directions instead of the conventional one beam excitation in single pulse LIBS (SP-LIBS). In spatial configuration, the laser beam geometry plays an important role in the emission signal enhancement. Thus, an adjustable geometric configuration with variable incident angle between the two splitted laser beams was constructed for achieving maximum signal enhancement. With the optimized angles of 60° and 70° for Al and Cu atomic emission lines at 396.15 nm and 324.75 nm respectively, about 5.6- and 4.8-folds signal enhancements were achieved for aluminum alloy and copper alloy samples compared to SP-LIBS. Furthermore, the temporal analysis, in which the intensity of atomic lines in SP-LIBS decayed at least ten times faster than the SBS-LIBS, proved that the energy coupling efficiency of SBS-LIBS was significantly higher than that of SP-LIBS. PMID:25557721

Matrix Synthesis of Graphene on a Diamond Surface and Its Simulation

NASA Astrophysics Data System (ADS)

Alekseev, N. I.

2018-07-01

A quantum-chemical simulation is performed for the transformation of the upper sublayer of carbon atoms in the lattice of single-crystal diamond into a flat graphene lattice under the influence of the atoms of a molten copper film on the diamond surface. It is established that the stable system configuration corresponds to the thermally activated motion of carbon atoms in the lower sublayer of the interface diamond layer to the position of graphene, i.e., at the same level as the atoms of the upper sublayer. The energy gain in comparison to the noninteracting subsystems of the copper and diamond atoms is approximately 0.7 eV per atom of the lower sublayer. The maximum size of the resulting graphene film is estimated and a possible mechanism for its rupture is considered.

Polymorphous band structure model of gapping in the antiferromagnetic and paramagnetic phases of the Mott insulators MnO, FeO, CoO, and NiO

NASA Astrophysics Data System (ADS)

Trimarchi, Giancarlo; Wang, Zhi; Zunger, Alex

2018-01-01

The existence of band gaps in both the antiferromagnetic (AFM) and paramagnetic (PM) phases of the classic NaCl-structure Mott insulators MnO, FeO, CoO, and NiO is traditionally viewed and taught as a manifestation of strong correlation whereby insulation results from electrons moving across the lattice forming states with doubly occupied d orbitals on certain atomic sites and empty d orbitals on other sites. Within such theories, the gap of the AFM and PM phases of these oxides emerges even in the absence of spatial symmetry breaking. The need for such a correlated picture is partially based on the known failure of the commonly used band models for the PM phase that assume for such a spin disordered state the macroscopically averaged NaCl structure, where all transition metal (TM) sites are symmetry-equivalent (a monomorphous description), producing a gapless PM state with zero magnetic moments, in sharp conflict with experiment. Here, we seek to understand the minimum theoretical description needed to capture the leading descriptors of ground state Mott insulation in the classic, 3 d monoxide Mott systems—gapping and moment formation in the AFM and PM phase. As noted by previous authors, the spin-ordered AFM phase in these materials already shows in band theory a significant band gap when one doubles the NaCl unit cell by permitting different potentials for transition-metal atoms with different spins. For the spin-disordered PM phase, we allow analogously larger NaCl-type supercells where each TM site can have different spin direction and local bonding environments (i.e., disordered), yet the total spin is zero. Such a polymorphous description has the flexibility to acquire symmetry-breaking energy-lowering patterns that can lift the degeneracy of the d orbitals and develop large on-site magnetic moments without violating the global, averaged NaCl symmetry. Electrons are exchanged between spin-up and spin-down bands to create closed-shell insulating configurations that lend themselves to a single determinental description. It turns out that such a polymorphous description of the structure within the single-determinant, mean-field, Bloch periodic band structure approach (based on DFT +U ) allows large on-site magnetic moments to develop spontaneously, leading to significant (1-3 eV) band gaps and large local moments in the AFM and PM phases of the classic NaCl-structure Mott insulators MnO, FeO, CoO, and NiO in agreement with experiment. We adapt to the spin disordered polymorphous configurations the "special quasirandom structure" (SQS) construct known from the theory of disordered substitutional alloys whereby supercell approximants which represent the best random configuration average (not individual snapshots) for finite (64, 216 atoms, or larger) supercells of a given lattice symmetry are constructed. We conclude that the basic features of these paradigmatic Mott insulators can be approximated by the physics included in energy-lowering symmetry broken DFT.

Evaluating the Free Energies of Solvation and Electronic Structures of Lithium-Ion Battery Electrolytes.

PubMed

Shakourian-Fard, Mehdi; Kamath, Ganesh; Sankaranarayanan, Subramanian K R S

2016-09-19

Adaptive biasing force molecular dynamics simulations and density functional theory calculations were performed to understand the interaction of Li(+) with pure carbonates and ethylene carbonate (EC)-based binary mixtures. The most favorable Li carbonate cluster configurations obtained from molecular dynamics simulations were subjected to detailed structural and thermochemistry calculations on the basis of the M06-2X/6-311++G(d,p) level of theory. We report the ranking of these electrolytes on the basis of the free energies of Li-ion solvation in carbonates and EC-based mixtures. A strong local tetrahedral order involving four carbonates around the Li(+) was seen in the first solvation shell. Thermochemistry calculations revealed that the enthalpy of solvation and the Gibbs free energy of solvation of the Li(+) ion with carbonates are negative and suggested the ion-carbonate complexation process to be exothermic and spontaneous. Natural bond orbital analysis indicated that Li(+) interacts with the lone pairs of electrons on the carbonyl oxygen atom in the primary solvation sphere. These interactions lead to an increase in the carbonyl (C=O) bond lengths, as evidenced by a redshift in the vibrational frequencies [ν(C=O)] and a decrease in the electron density values at the C=O bond critical points in the primary solvation sphere. Quantum theory of atoms in molecules, localized molecular orbital energy decomposition analysis (LMO-EDA), and noncovalent interaction plots revealed the electrostatic nature of the Li(+) ion interactions with the carbonyl oxygen atoms in these complexes. On the basis of LMO-EDA, the strongest attractive interaction in these complexes was found to be the electrostatic interaction followed by polarization, dispersion, and exchange interactions. Overall, our calculations predicted EC and a binary mixture of EC/dimethyl carbonate to be appropriate electrolytes for Li-ion batteries, which complies with experiments and other theoretical results. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Machine learning assisted first-principles calculation of multicomponent solid solutions: estimation of interface energy in Ni-based superalloys

NASA Astrophysics Data System (ADS)

Chandran, Mahesh; Lee, S. C.; Shim, Jae-Hyeok

2018-02-01

A disordered configuration of atoms in a multicomponent solid solution presents a computational challenge for first-principles calculations using density functional theory (DFT). The challenge is in identifying the few probable (low energy) configurations from a large configurational space before DFT calculation can be performed. The search for these probable configurations is possible if the configurational energy E({\\boldsymbol{σ }}) can be calculated accurately and rapidly (with a negligibly small computational cost). In this paper, we demonstrate such a possibility by constructing a machine learning (ML) model for E({\\boldsymbol{σ }}) trained with DFT-calculated energies. The feature vector for the ML model is formed by concatenating histograms of pair and triplet (only equilateral triangle) correlation functions, {g}(2)(r) and {g}(3)(r,r,r), respectively. These functions are a quantitative ‘fingerprint’ of the spatial arrangement of atoms, familiar in the field of amorphous materials and liquids. The ML model is used to generate an accurate distribution P(E({\\boldsymbol{σ }})) by rapidly spanning a large number of configurations. The P(E) contains full configurational information of the solid solution and can be selectively sampled to choose a few configurations for targeted DFT calculations. This new framework is employed to estimate (100) interface energy ({σ }{{IE}}) between γ and γ \\prime at 700 °C in Alloy 617, a Ni-based superalloy, with composition reduced to five components. The estimated {σ }{{IE}} ≈ 25.95 mJ m-2 is in good agreement with the value inferred by the precipitation model fit to experimental data. The proposed new ML-based ab initio framework can be applied to calculate the parameters and properties of alloys with any number of components, thus widening the reach of first-principles calculation to realistic compositions of industrially relevant materials and alloys.

Local random configuration-tree theory for string repetition and facilitated dynamics of glass

NASA Astrophysics Data System (ADS)

Lam, Chi-Hang

2018-02-01

We derive a microscopic theory of glassy dynamics based on the transport of voids by micro-string motions, each of which involves particles arranged in a line hopping simultaneously displacing one another. Disorder is modeled by a random energy landscape quenched in the configuration space of distinguishable particles, but transient in the physical space as expected for glassy fluids. We study the evolution of local regions with m coupled voids. At a low temperature, energetically accessible local particle configurations can be organized into a random tree with nodes and edges denoting configurations and micro-string propagations respectively. Such trees defined in the configuration space naturally describe systems defined in two- or three-dimensional physical space. A micro-string propagation initiated by a void can facilitate similar motions by other voids via perturbing the random energy landscape, realizing path interactions between voids or equivalently string interactions. We obtain explicit expressions of the particle diffusion coefficient and a particle return probability. Under our approximation, as temperature decreases, random trees of energetically accessible configurations exhibit a sequence of percolation transitions in the configuration space, with local regions containing fewer coupled voids entering the non-percolating immobile phase first. Dynamics is dominated by coupled voids of an optimal group size, which increases as temperature decreases. Comparison with a distinguishable-particle lattice model (DPLM) of glass shows very good quantitative agreements using only two adjustable parameters related to typical energy fluctuations and the interaction range of the micro-strings.

Similar local order in disordered fluorite and aperiodic pyrochlore structures

DOE PAGES

Shamblin, Jacob; Tracy, Cameron; Palomares, Raul; ...

2017-10-01

A major challenge to understanding the response of materials to extreme environments (e.g., nuclear fuels/waste forms and fusion materials) is to unravel the processes by which a material can incorporate atomic-scale disorder, and at the same time, remain crystalline. While it has long been known that all condensed matter, even liquids and glasses, possess short-range order, the relation between fully-ordered, disordered, and aperiodic structures over multiple length scales is not well understood. For example, when defects are introduced (via pressure or irradiation) into materials adopting the pyrochlore structure, these complex oxides either disorder over specific crystallographic sites, remaining crystalline, ormore » become aperiodic. Here we present neutron total scattering results characterizing the irradiation response of two pyrochlores, one that is known to disorder (Er2Sn2O7) and the other to amorphize (Dy2Sn2O7) under ion irradiation. The results demonstrate that in both cases, the local pyrochlore structure is transformed into similar short range configurations that are best fit by the orthorhombic weberite structure, even though the two compositions have distinctly different structures, aperiodic vs. disordered-crystalline, at longer length scales. Thus, a material's resistance to amorphization may not depend primarily on local defect formation energies, but rather on the structure's compatibility with meso-scale modulations of the local order in a way that maintains long-range periodicity.« less

Shear response of grain boundaries with metastable structures by molecular dynamics simulations

NASA Astrophysics Data System (ADS)

Zhang, Liang; Lu, Cheng; Shibuta, Yasushi

2018-04-01

Grain boundaries (GBs) can play a role as the favored locations to annihilate point defects, such as interstitial atoms and vacancies. It is thus highly probable that different boundary structures can be simultaneously present in equilibrium with each other in the same GB, and thus the GB achieves a metastable state. However, the structural transition and deformation mechanism of such GBs are currently not well understood. In this work, molecular dynamics simulations were carried out to study the multiple structures of a Σ5(310)/[001] GB in bicrystal Al and to investigate the effect of structural multiplicity on the mechanical and kinetic properties of such a GB. Different GB structures were obtained by changing the starting atomic configuration of the bicrystal model, and the GB structures had significantly different atomic density. For the Σ5(310) GB with metastable structures, GB sliding was the dominant mechanism at a low temperature (T = 10 K) under shear stress. The sliding mechanism resulted from the uncoordinated transformation of the inhomogeneous structural units. The nucleation of voids was observed during GB sliding at the low temperature, and the voids subsequently evolved to a nanocrack at the boundary plane. Increasing the temperature can induce the structural transition of local GB structures and can change their overall kinetic properties. GB migration with occasional GB sliding dominated the deformation mechanism at elevated temperatures (T = 300 and 600 K), and the migration process of the metastable GB structures is closely related to the thermally assisted diffusion mechanism.

Mixing of MnPc electronic states at the MnPc/Au(110) interface

NASA Astrophysics Data System (ADS)

Gargiani, Pierluigi; Lisi, Simone; Avvisati, Giulia; Mondelli, Pierluigi; Fatale, Sara; Betti, Maria Grazia

2017-10-01

Manganese-phthalocyanines form assembled chains with a variety of ordered super-structures, flat lying along the Au(110) reconstructed channels. The chains first give rise to a ×5 symmetry reconstruction, while further deposition of MnPc leads to a ×7 periodicity at the completion of the first single layer. A net polarization with the formation of an interface dipole is mainly due to the molecular π-states located on the macrocycles pyrrole rings, while the central metal ion induces a reduction in the polarization, whose amount is related to the Mn-Au interaction. The adsorption-induced interface polarization is compared to other 3d-metal phthalocyanines, to unravel the role of the central metal atom configuration in the interaction process of the d-states. The MnPc adsorption on Au(110) induces the re-hybridization of the electronic states localized on the central metal atom, promoting a charge redistribution of the molecular orbitals of the MnPc molecules. The molecule-substrate interaction is controlled by a symmetry-determined mixing between the electronic states, involving also the molecular empty orbitals with d character hybridized with the nitrogen atoms of the pyrrole ring, as deduced by photoemission and X-ray absorption spectroscopy exploiting light polarization. The symmetry-determined mixing between the electronic states of the Mn metal center and of the Au substrate induces a density of states close to the Fermi level for the ×5 phase.

Molecular dynamics simulations of hydrogen diffusion in aluminum

DOE PAGES

Zhou, X. W.; El Gabaly, F.; Stavila, V.; ...

2016-03-23

In this study, hydrogen diffusion impacts the performance of solid-state hydrogen storage materials and contributes to the embrittlement of structural materials under hydrogen-containing environments. In atomistic simulations, the diffusion energy barriers are usually calculated using molecular statics simulations where a nudged elastic band method is used to constrain a path connecting the two end points of an atomic jump. This approach requires prior knowledge of the “end points”. For alloy and defective systems, the number of possible atomic jumps with respect to local atomic configurations is tremendous. Even when these jumps can be exhaustively studied, it is still unclear howmore » they can be combined to give an overall diffusion behavior seen in experiments. Here we describe the use of molecular dynamics simulations to determine the overall diffusion energy barrier from the Arrhenius equation. This method does not require information about atomic jumps, and it has additional advantages, such as the ability to incorporate finite temperature effects and to determine the pre-exponential factor. As a test case for a generic method, we focus on hydrogen diffusion in bulk aluminum. We find that the challenge of this method is the statistical variation of the results. However, highly converged energy barriers can be achieved by an appropriate set of temperatures, output time intervals (for tracking hydrogen positions), and a long total simulation time. Our results help elucidate the inconsistencies of the experimental diffusion data published in the literature. The robust approach developed here may also open up future molecular dynamics simulations to rapidly study diffusion properties of complex material systems in multidimensional spaces involving composition and defects.« less

An Estimation of Hybrid Quantum Mechanical Molecular Mechanical Polarization Energies for Small Molecules Using Polarizable Force-Field Approaches

DOE PAGES

Huang, Jing; Mei, Ye; König, Gerhard; ...

2017-01-24

Here in this work, we report two polarizable molecular mechanics (polMM) force field models for estimating the polarization energy in hybrid quantum mechanical molecular mechanical (QM/MM) calculations. These two models, named the potential of atomic charges (PAC) and potential of atomic dipoles (PAD), are formulated from the ab initio quantum mechanical (QM) response kernels for the prediction of the QM density response to an external molecular mechanical (MM) environment (as described by external point charges). The PAC model is similar to fluctuating charge (FQ) models because the energy depends on external electrostatic potential values at QM atomic sites; the PADmore » energy depends on external electrostatic field values at QM atomic sites, resembling induced dipole (ID) models. To demonstrate their uses, we apply the PAC and PAD models to 12 small molecules, which are solvated by TIP3P water. The PAC model reproduces the QM/MM polarization energy with a R 2 value of 0.71 for aniline (in 10,000 TIP3P water configurations) and 0.87 or higher for other eleven solute molecules, while the PAD model has a much better performance with R 2 values of 0.98 or higher. The PAC model reproduces reference QM/MM hydration free energies for 12 solute molecules with a RMSD of 0.59 kcal/mol. The PAD model is even more accurate, with a much smaller RMSD of 0.12 kcal/mol, with respect to the reference. Lastly, this suggests that polarization effects, including both local charge distortion and intramolecular charge transfer, can be well captured by induced dipole type models with proper parametrization.« less

An Estimation of Hybrid Quantum Mechanical Molecular Mechanical Polarization Energies for Small Molecules Using Polarizable Force-Field Approaches.

PubMed

Huang, Jing; Mei, Ye; König, Gerhard; Simmonett, Andrew C; Pickard, Frank C; Wu, Qin; Wang, Lee-Ping; MacKerell, Alexander D; Brooks, Bernard R; Shao, Yihan

2017-02-14

In this work, we report two polarizable molecular mechanics (polMM) force field models for estimating the polarization energy in hybrid quantum mechanical molecular mechanical (QM/MM) calculations. These two models, named the potential of atomic charges (PAC) and potential of atomic dipoles (PAD), are formulated from the ab initio quantum mechanical (QM) response kernels for the prediction of the QM density response to an external molecular mechanical (MM) environment (as described by external point charges). The PAC model is similar to fluctuating charge (FQ) models because the energy depends on external electrostatic potential values at QM atomic sites; the PAD energy depends on external electrostatic field values at QM atomic sites, resembling induced dipole (ID) models. To demonstrate their uses, we apply the PAC and PAD models to 12 small molecules, which are solvated by TIP3P water. The PAC model reproduces the QM/MM polarization energy with a R 2 value of 0.71 for aniline (in 10,000 TIP3P water configurations) and 0.87 or higher for other 11 solute molecules, while the PAD model has a much better performance with R 2 values of 0.98 or higher. The PAC model reproduces reference QM/MM hydration free energies for 12 solute molecules with a RMSD of 0.59 kcal/mol. The PAD model is even more accurate, with a much smaller RMSD of 0.12 kcal/mol, with respect to the reference. This suggests that polarization effects, including both local charge distortion and intramolecular charge transfer, can be well captured by induced dipole type models with proper parametrization.

An Estimation of Hybrid Quantum Mechanical Molecular Mechanical Polarization Energies for Small Molecules Using Polarizable Force-Field Approaches

DOE Office of Scientific and Technical Information (OSTI.GOV)

Huang, Jing; Mei, Ye; König, Gerhard

Here in this work, we report two polarizable molecular mechanics (polMM) force field models for estimating the polarization energy in hybrid quantum mechanical molecular mechanical (QM/MM) calculations. These two models, named the potential of atomic charges (PAC) and potential of atomic dipoles (PAD), are formulated from the ab initio quantum mechanical (QM) response kernels for the prediction of the QM density response to an external molecular mechanical (MM) environment (as described by external point charges). The PAC model is similar to fluctuating charge (FQ) models because the energy depends on external electrostatic potential values at QM atomic sites; the PADmore » energy depends on external electrostatic field values at QM atomic sites, resembling induced dipole (ID) models. To demonstrate their uses, we apply the PAC and PAD models to 12 small molecules, which are solvated by TIP3P water. The PAC model reproduces the QM/MM polarization energy with a R 2 value of 0.71 for aniline (in 10,000 TIP3P water configurations) and 0.87 or higher for other eleven solute molecules, while the PAD model has a much better performance with R 2 values of 0.98 or higher. The PAC model reproduces reference QM/MM hydration free energies for 12 solute molecules with a RMSD of 0.59 kcal/mol. The PAD model is even more accurate, with a much smaller RMSD of 0.12 kcal/mol, with respect to the reference. Lastly, this suggests that polarization effects, including both local charge distortion and intramolecular charge transfer, can be well captured by induced dipole type models with proper parametrization.« less

Collisional-radiative modeling of tungsten at temperatures of 1200–2400 eV

DOE PAGES

Colgan, James; Fontes, Christopher; Zhang, Honglin; ...

2015-04-30

We discuss new collisional-radiative modeling calculations of tungsten at moderate temperatures of 1200 to 2400 eV. Such plasma conditions are relevant to ongoing experimental work at ASDEX Upgrade and are expected to be relevant for ITER. Our calculations are made using the Los Alamos National Laboratory (LANL) collisional-radiative modeling ATOMIC code. These calculations formed part of a submission to the recent NLTE-8 workshop that was held in November 2013. This series of workshops provides a forum for detailed comparison of plasma and spectral quantities from NLTE collisional-radiative modeling codes. We focus on the LANL ATOMIC calculations for tungsten that weremore » submitted to the NLTE-8 workshop and discuss different models that were constructed to predict the tungsten emission. In particular, we discuss comparisons between semi-relativistic configuration-average and fully relativistic configuration-average calculations. As a result, we also present semi-relativistic calculations that include fine-structure detail, and discuss the difficult problem of ensuring completeness with respect to the number of configurations included in a CR calculation.« less

Standing and sitting adlayers in atomic layer deposition of ZnO

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gao, Zhengning; Banerjee, Parag, E-mail: parag.banerjee@wustl.edu; Wu, Fei

The extent of reactivity of diethyl zinc (DEZ) with a hydroxylated surface during atomic layer deposition (ALD) of ZnO using DEZ and water is measured. Two adlayer configurations of DEZ are possible. The “standing” adlayer releases one ethyl group from DEZ. The “sitting” adlayer releases both ethyl groups, thus forming a Zn bridge between two O anions. Density functional theory calculations suggest the sitting configuration is more stable than the standing configuration by 790 meV. In situ quadrupole mass spectroscopy of by-product ethane generated in ALD half cycles indicate that ∼1.56 OH sites react with a DEZ molecule resulting in 71.6%more » of sitting sites. A simple simulation of a “ball-and-stick” DEZ molecule randomly collapsing on a neighboring site remarkably captures this adlayer behavior. It is concluded that DEZ fraction sitting is a competitive process of a standing DEZ molecule collapsing onto an available neighboring hydroxyl site, as sites vie for occupancy via adsorption and surface diffusion.« less

Array Receivers and Sound Sources for Three Dimensional Shallow Water Acoustic Field Experiments

DTIC Science & Technology

2016-12-06

upgrade included improving the SHRU clocks by utilizing chip- scale atomic clocks (CSAC), enlarging battery packs to extend the operation duration, and...instrument upgrade included improving the SHRU clocks by utilizing chip-scale atomic clocks (CSAC), enlarging battery packs to extend the operation...Changing the deployment configuration to use dual pressure housings to augment the alkaline primary battery payload to achieve the one-year duration

Crystal structure of 1,2,3,5-di-O-methyl­ene-α-d-xylo­furan­ose

PubMed Central

Tiritiris, Ioannis; Tussetschläger, Stefan; Kantlehner, Willi

2015-01-01

The title compound, C7H10O5, was synthesized by reaction of d-xylose with paraformaldehyde. In the crystal, the central part of the mol­ecule consists of a five-membered C4O ring with an envelope conformation, with the methine C atom adjacent to the O atom being the flap. The protected O atoms of both cyclic acetal groups are oriented so that the four chiral C atoms of the furan­ose part show an R configuration. C—H⋯O hydrogen bonds are present between adjacent mol­ecules, generating a three-dimensional network. PMID:26594582

Two-species five-beam magneto-optical trap for erbium and dysprosium

NASA Astrophysics Data System (ADS)

Ilzhöfer, P.; Durastante, G.; Patscheider, A.; Trautmann, A.; Mark, M. J.; Ferlaino, F.

2018-02-01

We report on the first realization of a two-species magneto-optical trap (MOT) for the highly magnetic erbium and dysprosium atoms. The MOT operates on an intercombination line for the respective species. Owing to the narrow-line character of such a cooling transition and the action of gravity, we demonstrate a trap geometry employing only five beams in the orthogonal configuration. We observe that the mixture is cooled and trapped very efficiently, with up to 5 ×108 Er atoms and 109 Dy atoms at temperatures of about 10 μ K . Our results offer an ideal starting condition for the creation of a dipolar quantum mixture of highly magnetic atoms.

First-principles studies of a photovoltaic material based on silicon heavily codoped with sulfur and nitrogen

NASA Astrophysics Data System (ADS)

Dong, Xiao; Wang, Yongyong; Song, Xiaohui; Yang, Feng

2018-03-01

In silicon co-hyperdoped with nitrogen and sulfur, dopant atoms tend to form dimers in the near-equilibrium process. The dimer that contains substitutional N and S atoms has the lowest formation energy and can form an impurity band that overlaps with the conduction band (CB). When separating the two atoms far apart from each other, the impurity band is clearly isolated from the CB and becomes an intermediate band (IB). The sub-band-gap absorption decreases with the decrease in the substitutional atom distance. The sub-band-gap absorption of the material is the combined effect of the configurations with different N-S distances.

Nanoscale soldering of axially positioned single-walled carbon nanotubes: a molecular dynamics simulation study.

PubMed

Cui, Jianlei; Yang, Lijun; Zhou, Liang; Wang, Yang

2014-02-12

The miniaturization of electronics devices into the nanometer scale is indispensable for next-generation semi-conductor technology. Carbon nanotubes (CNTs) are considered to be the promising candidates for future interconnection wires. To study the carbon nanotubes interconnection during nanosoldering, the melting process of nanosolder and nanosoldering process between single-walled carbon nanotubes are simulated with molecular dynamics method. As the simulation results, the melting point of 2 nm silver solder is about 605 K because of high surface energy, which is below the melting temperature of Ag bulk material. In the nanosoldering process simulations, Ag atoms may be dragged into the nanotubes to form different connection configuration, which has no apparent relationship with chirality of SWNTs. The length of core filling nanowires structure has the relationship with the diameter, and it does not become longer with the increasing diameter of SWNT. Subsequently, the dominant mechanism of was analyzed. In addition, as the heating temperature and time, respectively, increases, more Ag atoms can enter the SWNTs with longer length of Ag nanowires. And because of the strong metal bonds, less Ag atoms can remain with the tight atomic structures in the gap between SWNT and SWNT. The preferred interconnection configurations can be achieved between SWNT and SWNT in this paper.

Specific Non-Local Interactions Are Not Necessary for Recovering Native Protein Dynamics

PubMed Central

Dasgupta, Bhaskar; Kasahara, Kota; Kamiya, Narutoshi; Nakamura, Haruki; Kinjo, Akira R.

2014-01-01

The elastic network model (ENM) is a widely used method to study native protein dynamics by normal mode analysis (NMA). In ENM we need information about all pairwise distances, and the distance between contacting atoms is restrained to the native value. Therefore ENM requires O(N2) information to realize its dynamics for a protein consisting of N amino acid residues. To see if (or to what extent) such a large amount of specific structural information is required to realize native protein dynamics, here we introduce a novel model based on only O(N) restraints. This model, named the ‘contact number diffusion’ model (CND), includes specific distance restraints for only local (along the amino acid sequence) atom pairs, and semi-specific non-local restraints imposed on each atom, rather than atom pairs. The semi-specific non-local restraints are defined in terms of the non-local contact numbers of atoms. The CND model exhibits the dynamic characteristics comparable to ENM and more correlated with the explicit-solvent molecular dynamics simulation than ENM. Moreover, unrealistic surface fluctuations often observed in ENM were suppressed in CND. On the other hand, in some ligand-bound structures CND showed larger fluctuations of buried protein atoms interacting with the ligand compared to ENM. In addition, fluctuations from CND and ENM show comparable correlations with the experimental B-factor. Although there are some indications of the importance of some specific non-local interactions, the semi-specific non-local interactions are mostly sufficient for reproducing the native protein dynamics. PMID:24625758

Equilibrium structure of δ-Bi(2)O(3) from first principles.

PubMed

Music, Denis; Konstantinidis, Stephanos; Schneider, Jochen M

2009-04-29

Using ab initio calculations, we have systematically studied the structure of δ-Bi(2)O(3) (fluorite prototype, 25% oxygen vacancies) probing [Formula: see text] and combined [Formula: see text] and [Formula: see text] oxygen vacancy ordering, random distribution of oxygen vacancies with two different statistical descriptions as well as local relaxations. We observe that the combined [Formula: see text] and [Formula: see text] oxygen vacancy ordering is the most stable configuration. Radial distribution functions for these configurations can be classified as discrete (ordered configurations) and continuous (random configurations). This classification can be understood on the basis of local structural relaxations. Up to 28.6% local relaxation of the oxygen sublattice is present in the random configurations, giving rise to continuous distribution functions. The phase stability obtained may be explained with the bonding analysis. Electron lone-pair charges in the predominantly ionic Bi-O matrix may stabilize the combined [Formula: see text] and [Formula: see text] oxygen vacancy ordering.

Non-Hermitian optics in atomic systems

NASA Astrophysics Data System (ADS)

Zhang, Zhaoyang; Ma, Danmeng; Sheng, Jiteng; Zhang, Yiqi; Zhang, Yanpeng; Xiao, Min

2018-04-01

A wide class of non-Hermitian Hamiltonians can possess entirely real eigenvalues when they have parity-time (PT) symmetric potentials. Recently, this family of non-Hermitian systems has attracted considerable attention in diverse areas of physics due to their extraordinary properties, especially in optical systems based on solid-state materials, such as coupled gain-loss waveguides and microcavities. Considering the desired refractive index can be effectively manipulated through atomic coherence, it is important to realize such non-Hermitian optical potentials and further investigate their distinct properties in atomic systems. In this paper, we review the recent theoretical and experimental progress of non-Hermitian optics with coherently prepared multi-level atomic configurations. The realizations of (anti-) PT symmetry with different schemes have extensively demonstrated the special optical properties of non-Hermitian optical systems with atomic coherence.

Electronic and optical properties of hydrogenated silicon carbide nanosheets: A DFT study

NASA Astrophysics Data System (ADS)

Delavari, Najmeh; Jafari, Mahmoud

2018-07-01

Density-functional theory has been applied to investigate the effect of hydrogen adsorption on silicon carbide (SiC) nanosheets, considering six, different configurations for adsorption process. The chair-like configuration is found to be the most stable because of the adsorption of hydrogen atoms by silicon and carbon atoms on the opposite sides. The pure and hydrogenated SiC monolayers are also found to be sp2- and sp3-hybridized, respectively. The binding energy of the hydrogen atoms in the chair-like structure is calculated about -3.845 eV, implying the system to be much more stable than the same study based on graphene, though with nearly the same electronic properties, strongly proposing the SiC monolayer to be a promising material for next generation hydrogen storage. Optical properties presented in terms of the real and the imaginary parts of the dielectric function also demonstrate a decrease in the dielectric constant and the static refractive index due to hydrogen adsorption with the Plasmon frequency of the chair-like, hydrogenated monolayer, occurring at higher energies compared to that of the pure one.

Density functional study for crystalline structures and electronic properties of Si1- x Sn x binary alloys

NASA Astrophysics Data System (ADS)

Nagae, Yuki; Kurosawa, Masashi; Shibayama, Shigehisa; Araidai, Masaaki; Sakashita, Mitsuo; Nakatsuka, Osamu; Shiraishi, Kenji; Zaima, Shigeaki

2016-08-01

We have carried out density functional theory (DFT) calculation for Si1- x Sn x alloy and investigated the effect of the displacement of Si and Sn atoms with strain relaxation on the lattice constant and E- k dispersion. We calculated the formation probabilities for all atomic configurations of Si1- x Sn x according to the Boltzmann distribution. The average lattice constant and E- k dispersion were weighted by the formation probability of each configuration of Si1- x Sn x . We estimated the displacement of Si and Sn atoms from the initial tetrahedral site in the Si1- x Sn x unit cell considering structural relaxation under hydrostatic pressure, and we found that the breaking of the degenerated electronic levels of the valence band edge could be caused by the breaking of the tetrahedral symmetry. We also calculated the E- k dispersion of the Si1- x Sn x alloy by the DFT+U method and found that a Sn content above 50% would be required for the indirect-direct transition.

Reinforced dynamics for enhanced sampling in large atomic and molecular systems

NASA Astrophysics Data System (ADS)

Zhang, Linfeng; Wang, Han; E, Weinan

2018-03-01

A new approach for efficiently exploring the configuration space and computing the free energy of large atomic and molecular systems is proposed, motivated by an analogy with reinforcement learning. There are two major components in this new approach. Like metadynamics, it allows for an efficient exploration of the configuration space by adding an adaptively computed biasing potential to the original dynamics. Like deep reinforcement learning, this biasing potential is trained on the fly using deep neural networks, with data collected judiciously from the exploration and an uncertainty indicator from the neural network model playing the role of the reward function. Parameterization using neural networks makes it feasible to handle cases with a large set of collective variables. This has the potential advantage that selecting precisely the right set of collective variables has now become less critical for capturing the structural transformations of the system. The method is illustrated by studying the full-atom explicit solvent models of alanine dipeptide and tripeptide, as well as the system of a polyalanine-10 molecule with 20 collective variables.

Broadband photon-photon interactions mediated by cold atoms in a photonic crystal fiber

PubMed Central

Litinskaya, Marina; Tignone, Edoardo; Pupillo, Guido

2016-01-01

We demonstrate theoretically that photon-photon attraction can be engineered in the continuum of scattering states for pairs of photons propagating in a hollow-core photonic crystal fiber filled with cold atoms. The atoms are regularly spaced in an optical lattice configuration and the photons are resonantly tuned to an internal atomic transition. We show that the hard-core repulsion resulting from saturation of the atomic transitions induces bunching in the photonic component of the collective atom-photon modes (polaritons). Bunching is obtained in a frequency range as large as tens of GHz, and can be controlled by the inter-atomic separation. We provide a fully analytical explanation for this phenomenon by proving that correlations result from a mismatch of the quantization volumes for atomic excitations and photons in the continuum. Even stronger correlations can be observed for in-gap two-polariton bound states. Our theoretical results use parameters relevant for current experiments and suggest a simple and feasible way to induce interactions between photons. PMID:27170160

Localization and force analysis at the single virus particle level using atomic force microscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Chih-Hao; Horng, Jim-Tong; Chang, Jeng-Shian

2012-01-06

Highlights: Black-Right-Pointing-Pointer Localization of single virus particle. Black-Right-Pointing-Pointer Force measurements. Black-Right-Pointing-Pointer Force mapping. -- Abstract: Atomic force microscopy (AFM) is a vital instrument in nanobiotechnology. In this study, we developed a method that enables AFM to simultaneously measure specific unbinding force and map the viral glycoprotein at the single virus particle level. The average diameter of virus particles from AFM images and the specificity between the viral surface antigen and antibody probe were integrated to design a three-stage method that sets the measuring area to a single virus particle before obtaining the force measurements, where the influenza virus was usedmore » as the object of measurements. Based on the purposed method and performed analysis, several findings can be derived from the results. The mean unbinding force of a single virus particle can be quantified, and no significant difference exists in this value among virus particles. Furthermore, the repeatability of the proposed method is demonstrated. The force mapping images reveal that the distributions of surface viral antigens recognized by antibody probe were dispersed on the whole surface of individual virus particles under the proposed method and experimental criteria; meanwhile, the binding probabilities are similar among particles. This approach can be easily applied to most AFM systems without specific components or configurations. These results help understand the force-based analysis at the single virus particle level, and therefore, can reinforce the capability of AFM to investigate a specific type of viral surface protein and its distributions.« less

A Configurational-Bias-Monte-Carlo Back-Mapping Algorithm for Efficient and Rapid Conversion of Coarse-Grained Water Structures Into Atomistic Models.

PubMed

Loeffler, Troy David; Chan, Henry; Narayanan, Badri; Cherukara, Mathew J; Gray, Stephen K; Sankaranarayanan, Subramanian K R S

2018-06-20

Coarse-grained molecular dynamics (MD) simulations represent a powerful approach to simulate longer time scale and larger length scale phenomena than those accessible to all-atom models. The gain in efficiency, however, comes at the cost of atomistic details. The reverse transformation, also known as back-mapping, of coarse grained beads into their atomistic constituents represents a major challenge. Most existing approaches are limited to specific molecules or specific force-fields and often rely on running a long time atomistic MD of the back-mapped configuration to arrive at an optimal solution. Such approaches are problematic when dealing with systems with high diffusion barriers. Here, we introduce a new extension of the configurational-bias-Monte-Carlo (CBMC) algorithm, which we term the crystalline-configurational-bias-Monte-Carlo (C-CBMC) algortihm, that allows rapid and efficient conversion of a coarse-grained model back into its atomistic representation. Although the method is generic, we use a coarse-grained water model as a representative example and demonstrate the back-mapping or reverse transformation for model systems ranging from the ice-liquid water interface to amorphous and crystalline ice configurations. A series of simulations using the TIP4P/Ice model are performed to compare the new CBMC method to several other standard Monte Carlo and Molecular Dynamics based back-mapping techniques. In all the cases, the C-CBMC algorithm is able to find optimal hydrogen bonded configuration many thousand evaluations/steps sooner than the other methods compared within this paper. For crystalline ice structures such as a hexagonal, cubic, and cubic-hexagonal stacking disorder structures, the C-CBMC was able to find structures that were between 0.05 and 0.1 eV/water molecule lower in energy than the ground state energies predicted by the other methods. Detailed analysis of the atomistic structures show a significantly better global hydrogen positioning when contrasted with the existing simpler back-mapping methods. Our results demonstrate the efficiency and efficacy of our new back-mapping approach, especially for crystalline systems where simple force-field based relaxations have a tendency to get trapped in local minima.

Locality of correlation in density functional theory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Burke, Kieron; Cancio, Antonio; Gould, Tim

The Hohenberg-Kohn density functional was long ago shown to reduce to the Thomas-Fermi (TF) approximation in the non-relativistic semiclassical (or large-Z) limit for all matter, i.e., the kinetic energy becomes local. Exchange also becomes local in this limit. Numerical data on the correlation energy of atoms support the conjecture that this is also true for correlation, but much less relevant to atoms. We illustrate how expansions around a large particle number are equivalent to local density approximations and their strong relevance to density functional approximations. Analyzing highly accurate atomic correlation energies, we show that E{sub C} → −A{sub C} ZlnZ +more » B{sub C}Z as Z → ∞, where Z is the atomic number, A{sub C} is known, and we estimate B{sub C} to be about 37 mhartree. The local density approximation yields A{sub C} exactly, but a very incorrect value for B{sub C}, showing that the local approximation is less relevant for the correlation alone. This limit is a benchmark for the non-empirical construction of density functional approximations. We conjecture that, beyond atoms, the leading correction to the local density approximation in the large-Z limit generally takes this form, but with B{sub C} a functional of the TF density for the system. The implications for the construction of approximate density functionals are discussed.« less

Average structure and M2 site configurations in C2/c clinopyroxenes along the Di-En join

NASA Astrophysics Data System (ADS)

Tribaudino, M.; Benna, P.; Bruno, E.

1989-12-01

In order to clarify the structural configurations observed in Diss in the Ca-rich region of the Di-En join (in which TEM observations show neither exsolution microstructures nor evidence of spinodal decomposition) single crystals large enough for X-ray diffraction analyses, with composition (Ca0.66Mg0.34)MgSi2O6, have been equilibrated close to the solvus at T=1350° C for 317 h, and quenched at room temperature. The refinement in C2/c space group shows that in the M2 site Ca and Mg are fully ‘ordered’ in two split positions (M2occ: 0.66 Ca; M2'occ: 0.34 Mg). Since the average structure shows a relevant elongation of anisotropic thermal ellipsoids of the O2 and O3 oxygen atoms, the refinement has been carried out according to a split model for O2 and O3 atoms: Ca appears 8-coordinated (as in diopside) and Mg shows a sixfold coordination similar to that of high-pigeonite. This coordination for Mg is significantly different from the fourfold coordination (Zn-like in Zn-cpx) proposed previously and it is a more probable coordination for Mg from a crystalchemical point of view. The same results were obtained refining a Di80En20 cpx, equilibrated at T=1230° C, according to the same O-split model. The data support the coexistence of a Di-like configuration for Ca and of a highPig-like configuration for Mg away from the solvus also. At T very near to T solidus the different configurations, observed at room temperature in the quenched samples, should converge and Ca and Mg should retain a single disordered configuration in the M2 site.

Quantum phases of a three-level matter-radiation interaction model using SU(3) coherent states with different cooperation numbers

NASA Astrophysics Data System (ADS)

Quezada, L. F.; Nahmad-Achar, E.

2018-06-01

We use coherent states as trial states for a variational approach to study a system of a finite number of three-level atoms interacting in a dipolar approximation with a one-mode electromagnetic field. The atoms are treated as semidistinguishable using different cooperation numbers and representations of SU(3). We focus our analysis on the quantum phases of the system as well as the behavior of the most relevant observables near the phase transitions. The results are computed for all three possible configurations (Ξ , Λ , and V ) of the three-level atoms.

Alloy-assisted deposition of three-dimensional arrays of atomic gold catalyst for crystal growth studies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fang, Yin; Jiang, Yuanwen; Cherukara, Mathew J.

Large-scale assembly of individual atoms over smooth surfaces is difficult to achieve. A configuration of an atom reservoir, in which individual atoms can be readily extracted, may successfully address this challenge. In this work, we demonstrate that a liquid gold-silicon alloy established in classical vapor-liquid-solid growth can deposit ordered and three-dimensional rings of isolated gold atoms over silicon nanowire sidewalls. Here, we perform ab initio molecular dynamics simulation and unveil a surprising single atomic gold-catalyzed chemical etching of silicon. Experimental verification of this catalytic process in silicon nanowires yields dopant-dependent, massive and ordered 3D grooves with spacing down to similarmore » to 5 nm. Finally, we use these grooves as self-labeled and ex situ markers to resolve several complex silicon growths, including the formation of nodes, kinks, scale-like interfaces, and curved backbones.« less

Improvement of an Atomic Clock using Squeezed Vacuum

NASA Astrophysics Data System (ADS)

Kruse, I.; Lange, K.; Peise, J.; Lücke, B.; Pezzè, L.; Arlt, J.; Ertmer, W.; Lisdat, C.; Santos, L.; Smerzi, A.; Klempt, C.

2016-09-01

Since the pioneering work of Ramsey, atom interferometers are employed for precision metrology, in particular to measure time and to realize the second. In a classical interferometer, an ensemble of atoms is prepared in one of the two input states, whereas the second one is left empty. In this case, the vacuum noise restricts the precision of the interferometer to the standard quantum limit (SQL). Here, we propose and experimentally demonstrate a novel clock configuration that surpasses the SQL by squeezing the vacuum in the empty input state. We create a squeezed vacuum state containing an average of 0.75 atoms to improve the clock sensitivity of 10000 atoms by 2.05-0.37 +0 .34 dB . The SQL poses a significant limitation for today's microwave fountain clocks, which serve as the main time reference. We evaluate the major technical limitations and challenges for devising a next generation of fountain clocks based on atomic squeezed vacuum.

Thermoelectricity in atom-sized junctions at room temperatures

PubMed Central

Tsutsui, Makusu; Morikawa, Takanori; Arima, Akihide; Taniguchi, Masateru

2013-01-01

Atomic and molecular junctions are an emerging class of thermoelectric materials that exploit quantum confinement effects to obtain an enhanced figure of merit. An important feature in such nanoscale systems is that the electron and heat transport become highly sensitive to the atomic configurations. Here we report the characterization of geometry-sensitive thermoelectricity in atom-sized junctions at room temperatures. We measured the electrical conductance and thermoelectric power of gold nanocontacts simultaneously down to the single atom size. We found junction conductance dependent thermoelectric voltage oscillations with period 2e2/h. We also observed quantum suppression of thermovoltage fluctuations in fully-transparent contacts. These quantum confinement effects appeared only statistically due to the geometry-sensitive nature of thermoelectricity in the atom-sized junctions. The present method can be applied to various nanomaterials including single-molecules or nanoparticles and thus may be used as a useful platform for developing low-dimensional thermoelectric building blocks. PMID:24270238

Alloy-assisted deposition of three-dimensional arrays of atomic gold catalyst for crystal growth studies

DOE PAGES

Fang, Yin; Jiang, Yuanwen; Cherukara, Mathew J.; ...

2017-12-08

Large-scale assembly of individual atoms over smooth surfaces is difficult to achieve. A configuration of an atom reservoir, in which individual atoms can be readily extracted, may successfully address this challenge. In this work, we demonstrate that a liquid gold-silicon alloy established in classical vapor-liquid-solid growth can deposit ordered and three-dimensional rings of isolated gold atoms over silicon nanowire sidewalls. Here, we perform ab initio molecular dynamics simulation and unveil a surprising single atomic gold-catalyzed chemical etching of silicon. Experimental verification of this catalytic process in silicon nanowires yields dopant-dependent, massive and ordered 3D grooves with spacing down to similarmore » to 5 nm. Finally, we use these grooves as self-labeled and ex situ markers to resolve several complex silicon growths, including the formation of nodes, kinks, scale-like interfaces, and curved backbones.« less

Wavelengths and energy levels for the Zn I isoelectronic sequence Sn{sup 20+} through U{sup 62+}

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brown, C.M.; Seely, J.F.; Kania, D.R.

Calculated and experimentally determined transition energies are presented for the Zn I isoelectronic sequence for the elements with atomic numbers Z = 50-92. The excitation energies were calculated for the 84 levels belonging to the 10 configurations of the type 4l4l{prime} by using the Hebrew University Lawrence Livermore Atomic Code (HULLAC). The analysis of the energy level structure along the isoelectronic sequence accounted for 20 avoided level crossings. The differences between the calculated and experimental transition energies were determined for 16 transitions, and the excitation energies of the levels belonging to the 4s4p, 4p{sup 2}, 4s4d, and 4s4f configurations weremore » derived from the semiempirically corrected transition energies. 16 refs., 3 figs., 1 tab.« less

Energy levels and radiative rates for Ne-like ions from Cu to Ga

NASA Astrophysics Data System (ADS)

Singh, Narendra; Aggarwal, Sunny

2017-11-01

Energy levels, lifetimes and wave function compositions are computed for 127 fine structural levels in Ne-like ions (Z=29{-}31). Configuration interaction has been included among 51 configurations (generating 1016 levels) and multiconfigurational Dirac-Fock method is used to generate the wave functions. Similar calculations have also been performed using the fully relativistic flexible atomic code (FAC). Transition wavelength, oscillator strength, transition probabilities and line strength are reported for electric dipole (E1), electric quadrupole (E2), magnetic dipole (M1) and magnetic quadrupole (M2) transitions from the ground level. We compared our calculated results with the available data in the literature. The calculated results are found to be in close agreement with the previous results. Further, we predict some new atomic data which may be important for plasma diagnostics.

Band engineering in twisted molybdenum disulfide bilayers

NASA Astrophysics Data System (ADS)

Zhao, Yipeng; Liao, Chengwei; Ouyang, Gang

2018-05-01

In order to explore the theoretical relationship between interlayer spacing, interaction and band offset at the atomic level in vertically stacked two-dimensional (2D) van der Waals (vdW) structures, we propose an analytical model to address the evolution of interlayer vdW coupling with random stacking configurations in MoS2 bilayers based on the atomic-bond-relaxation correlation mechanism. We found that interlayer spacing changes substantially with respect to the orientations, and the bandgap increases from 1.53 eV (AB stacking) to 1.68 eV (AA stacking). Our results reveal that the evolution of interlayer vdW coupling originates from the interlayer interaction, leading to interlayer separations and electronic properties changing with stacking configurations. Our predictions constitute a demonstration of twist engineering the band shift in the emergent class of 2D crystals, transition-metal dichalcogenides.

Atomic resolution holography.

PubMed

Hayashi, Kouichi

2014-11-01

Atomic resolution holography, such as X-ray fluorescence holography (XFH)[1] and photoelectron holography (PH), has the attention of researcher as an informative local structure analysis, because it provides three dimensional atomic images around specific elements within a range of a few nanometers. It can determine atomic arrangements around a specific element without any prior knowledge of structures. It is considered that the atomic resolution holographic is a third method of structural analysis at the atomic level after X-ray diffraction (XRD) and X-ray absorption fine structure (XAFS). As known by many researchers, XRD and XAFS are established methods that are widespread use in various fields. XRD and XAFS provide information on long-range translational periodicities and very local environments, respectively, whereas the atomic resolution holography gives 3D information on the local order and can visualize surrounding atoms with a large range of coordination shells. We call this feature "3D medium-range local structure observation".In addition to this feature, the atomic resolution holography is very sensitive to the displacement of atoms from their ideal positions, and one can obtain quantitative information about local lattice distortions by analyzing reconstructed atomic images[2] When dopants with different atomic radii from the matrix elements are present, the lattices around the dopants are distorted. However, using the conventional methods of structural analysis, one cannot determine the extent to which the local lattice distortions are preserved from the dopants. XFH is a good tool for solving this problem.Figure 1 shows a recent achievement on a relaxor ferroelectric of Pb(Mg1/3Nb2/3)O3 (PMN) using XFH. The structural studies of relaxor ferroelectrics have been carried out by X-ray or neutron diffractions, which suggested rhombohedral distortions of their lattices. However, their true pictures have not been obtained, yet. The Nb Kα holograms showed four separate Pb images, as shown in Fig.1. Using these images, we could obtain acute and obtuse rhombohedral structures of the crystal unit cells. Moreover, the Pb-Pb correlated images reconstructed from Pb Lα holograms showed a local structure of body center-like 2a0 ×2a0 × 2a0 superlattice, proving a rigid 3D network structural model combining the two kinds of rhombohedrons. This superstructure are believed to play an important role in the relaxor behaviour of PMN at atomic level[3].jmicro;63/suppl_1/i13/DFU047F1F1DFU047F1Fig. 1.3D images of the nearest Pb and O atoms around Nb in Pb(Mg1/3Nb2/3)O3. The cube represents 1/8 of the unit cell. © The Author 2014. Published by Oxford University Press on behalf of The Japanese Society of Microscopy. All rights reserved. For permissions, please e-mail: journals.permissions@oup.com.

Spatially restricted electrical activation of retinal ganglion cells in the rabbit retina by hexapolar electrode return configuration

NASA Astrophysics Data System (ADS)

Habib, Amgad G.; Cameron, Morven A.; Suaning, Gregg J.; Lovell, Nigel H.; Morley, John W.

2013-06-01

Objective. Visual prostheses currently in development aim to restore some form of vision to patients suffering from diseases such as age-related macular degeneration and retinitis pigmentosa. Most rely on electrically stimulating inner retinal cells via electrodes implanted on or near the retina, resulting in percepts of light termed ‘phosphenes’. Activation of spatially distinct populations of cells in the retina is key for pattern vision to be produced. To achieve this, the electrical stimulation must be localized, activating cells only in the direct vicinity of the stimulating electrode(s). With this goal in mind, a hexagonal return (hexapolar) configuration has been proposed as an alternative to the traditional monopolar or bipolar return configurations for electrically stimulating the retina. This study investigated the efficacy of the hexapolar configuration in localizing the activation of retinal ganglion cells (RGCs), compared to a monopolar configuration. Approach. Patch-clamp electrophysiology was used to measure the activation thresholds of RGCs in whole-mount rabbit retina to monopolar and hexapolar electrical stimulation, applied subretinally. Main results. Hexapolar activation thresholds for RGCs located outside the hex guard were found to be significantly (>2 fold) higher than those located inside the area of tissue bounded by the hex guard. The hexapolar configuration localized the activation of RGCs more effectively than its monopolar counterpart. Furthermore, no difference in hexapolar thresholds or localization was observed when using cathodic-first versus anodic-first stimulation. Significance. The hexapolar configuration may provide an improved method for electrically stimulating spatially distinct populations of cells in retinal tissue.

Doping of Semiconducting Atomic Chains

NASA Technical Reports Server (NTRS)

Toshishige, Yamada; Kutler, Paul (Technical Monitor)

1997-01-01

Due to the rapid progress in atom manipulation technology, atomic chain electronics would not be a dream, where foreign atoms are placed on a substrate to form a chain, and its electronic properties are designed by controlling the lattice constant d. It has been shown theoretically that a Si atomic chain is metallic regardless of d and that a Mg atomic chain is semiconducting or insulating with a band gap modified with d. For electronic applications, it is essential to establish a method to dope a semiconducting chain, which is to control the Fermi energy position without altering the original band structure. If we replace some of the chain atoms with dopant atoms randomly, the electrons will see random potential along the chain and will be localized strongly in space (Anderson localization). However, if we replace periodically, although the electrons can spread over the chain, there will generally appear new bands and band gaps reflecting the new periodicity of dopant atoms. This will change the original band structure significantly. In order to overcome this dilemma, we may place a dopant atom beside the chain at every N lattice periods (N > 1). Because of the periodic arrangement of dopant atoms, we can avoid the unwanted Anderson localization. Moreover, since the dopant atoms do not constitute the chain, the overlap interaction between them is minimized, and the band structure modification can be made smallest. Some tight-binding results will be discussed to demonstrate the present idea.

Correlation of atomic packing with the boson peak in amorphous alloys

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yang, W. M.; Key Laboratory of Magnetic Materials and Devices, Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo 315201; School of Materials Science and Engineering, Southeast University, Nanjing 211189

2014-09-28

Boson peaks (BP) have been observed from phonon specific heats in 10 studied amorphous alloys. Two Einstein-type vibration modes were proposed in this work and all data can be fitted well. By measuring and analyzing local atomic structures of studied amorphous alloys and 56 reported amorphous alloys, it is found that (a) the BP originates from local harmonic vibration modes associated with the lengths of short-range order (SRO) and medium-range order (MRO) in amorphous alloys, and (b) the atomic packing in amorphous alloys follows a universal scaling law, i.e., the ratios of SRO and MRO lengths to solvent atomic diametermore » are 3 and 7, respectively, which exact match with length ratios of BP vibration frequencies to Debye frequency for the studied amorphous alloys. This finding provides a new perspective for atomic packing in amorphous materials, and has significant implications for quantitative description of the local atomic orders and understanding the structure-property relationship.« less

Twisted MoSe 2 bilayers with variable local stacking and interlayer coupling revealed by low-frequency Raman spectroscopy

DOE PAGES

Puretzky, Alexander A.; Liang, Liangbo; Li, Xufan; ...

2016-01-14

Unique twisted bilayers of MoSe 2 with multiple stacking orientations and interlayer couplings in the narrow range of twist angles, 60 ± 3°, are revealed by low-frequency Raman spectroscopy and theoretical analysis. The slight deviation from 60 allows the concomitant presence of patches featuring all three high-symmetry stacking configurations (2H or AA', AB', A'B) in one unique bilayer system. In this case, the periodic arrangement of the patches and their size strongly depend on the twist angle. Ab initio modeling predicts significant changes in frequencies and intensities of low-frequency modes versus stacking and twist angle. Experimentally, the variable stacking andmore » coupling across the interface is revealed by the appearance of two breathing modes corresponding to the mixture of the high-symmetry stacking configurations and unaligned regions of monolayers. Only one breathing mode is observed outside the narrow range of twist angles. This indicates a stacking transition to unaligned monolayers with mismatched atom registry without the in-plane restoring force required to generate a shear mode. As a result, the variable interlayer coupling and spacing in transition metal dichalcogenide bilayers revealed in this study may provide a new platform for optoelectronic applications of these materials.« less

Twisted MoSe 2 bilayers with variable local stacking and interlayer coupling revealed by low-frequency Raman spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Puretzky, Alexander A.; Liang, Liangbo; Li, Xufan

Unique twisted bilayers of MoSe 2 with multiple stacking orientations and interlayer couplings in the narrow range of twist angles, 60 ± 3°, are revealed by low-frequency Raman spectroscopy and theoretical analysis. The slight deviation from 60 allows the concomitant presence of patches featuring all three high-symmetry stacking configurations (2H or AA', AB', A'B) in one unique bilayer system. In this case, the periodic arrangement of the patches and their size strongly depend on the twist angle. Ab initio modeling predicts significant changes in frequencies and intensities of low-frequency modes versus stacking and twist angle. Experimentally, the variable stacking andmore » coupling across the interface is revealed by the appearance of two breathing modes corresponding to the mixture of the high-symmetry stacking configurations and unaligned regions of monolayers. Only one breathing mode is observed outside the narrow range of twist angles. This indicates a stacking transition to unaligned monolayers with mismatched atom registry without the in-plane restoring force required to generate a shear mode. As a result, the variable interlayer coupling and spacing in transition metal dichalcogenide bilayers revealed in this study may provide a new platform for optoelectronic applications of these materials.« less

Aspects of image recognition in Vivid Technologies' dual-energy x-ray system for explosives detection

NASA Astrophysics Data System (ADS)

Eilbert, Richard F.; Krug, Kristoph D.

1993-04-01

The Vivid Rapid Explosives Detection Systems is a true dual energy x-ray machine employing precision x-ray data acquisition in combination with unique algorithms and massive computation capability. Data from the system's 960 detectors is digitally stored and processed by powerful supermicro-computers organized as an expandable array of parallel processors. The algorithms operate on the dual energy attenuation image data to recognize and define objects in the milieu of the baggage contents. Each object is then systematically examined for a match to a specific effective atomic number, density, and mass threshold. Material properties are determined by comparing the relative attenuations of the 75 kVp and 150 kVp beams and electronically separating the object from its local background. Other heuristic algorithms search for specific configurations and provide additional information. The machine automatically detects explosive materials and identifies bomb components in luggage with high specificity and throughput, X-ray dose is comparable to that of current airport x-ray machines. The machine is also configured to find heroin, cocaine, and US currency by selecting appropriate settings on-site. Since January 1992, production units have been operationally deployed at U.S. and European airports for improved screening of checked baggage.

Local Chemical Ordering and Negative Thermal Expansion in PtNi Alloy Nanoparticles.

PubMed

Li, Qiang; Zhu, He; Zheng, Lirong; Fan, Longlong; Wang, Na; Rong, Yangchun; Ren, Yang; Chen, Jun; Deng, Jinxia; Xing, Xianran

2017-12-13

An atomic insight into the local chemical ordering and lattice strain is particular interesting to recent emerging bimetallic nanocatalysts such as PtNi alloys. Here, we reported the atomic distribution, chemical environment, and lattice thermal evolution in full-scale structural description of PtNi alloy nanoparticles (NPs). The different segregation of elements in the well-faceted PtNi nanoparticles is convinced by extended X-ray absorption fine structure (EXAFS). Atomic pair distribution function (PDF) study evidences the coexistence of the face-centered cubic and tetragonal ordering parts in the local environment of PtNi nanoparticles. Further reverse Monte Carlo (RMC) simulation with PDF data obviously exposed the segregation as Ni and Pt in the centers of {111} and {001} facets, respectively. Layer-by-layer statistical analysis up to 6 nm for the local atomic pairs revealed the distribution of local tetragonal ordering on the surface. This local coordination environment facilitates the distribution of heteroatomic Pt-Ni pairs, which plays an important role in the negative thermal expansion of Pt 41 Ni 59 NPs. The present study on PtNi alloy NPs from local short-range coordination to long-range average lattice provides a new perspective on tailoring physical properties in nanomaterials.

Myrtenal, a controversial molecule for the proper application of the CIP Sequence Rule for multiple bonds.

PubMed

Zepeda, L Gerardo; Burgueño-Tapia, Eleuterio; Joseph-Nathan, Pedro

2011-04-01

This communication highlights the need of building hierarchical digraphs for the unequivocal assignment of stereochemical descriptors of (-)-myrtenal, a naturally-occurring oxygenated monoterpene whose absolute configuration (AC) is sometimes misrepresented in its structural formulae. Differentiation between duplicated atoms and phantom atoms for the proper application of the sequence rules is shown to be an essential step to get a proper construction of hierarchical digraphs.

Defect-Induced Hedgehog Polarization States in Multiferroics

NASA Astrophysics Data System (ADS)

Li, Linze; Cheng, Xiaoxing; Jokisaari, Jacob R.; Gao, Peng; Britson, Jason; Adamo, Carolina; Heikes, Colin; Schlom, Darrell G.; Chen, Long-Qing; Pan, Xiaoqing

2018-03-01

Continuous developments in nanotechnology require new approaches to materials synthesis that can produce novel functional structures. Here, we show that nanoscale defects, such as nonstoichiometric nanoregions (NSNRs), can act as nano-building blocks for creating complex electrical polarization structures in the prototypical multiferroic BiFeO3 . An array of charged NSNRs are produced in BiFeO3 thin films by tuning the substrate temperature during film growth. Atomic-scale scanning transmission electron microscopy imaging reveals exotic polarization rotation patterns around these NSNRs. These polarization patterns resemble hedgehog or vortex topologies and can cause local changes in lattice symmetries leading to mixed-phase structures resembling the morphotropic phase boundary with high piezoelectricity. Phase-field simulations indicate that the observed polarization configurations are mainly induced by charged states at the NSNRs. Engineering defects thus may provide a new route for developing ferroelectric- or multiferroic-based nanodevices.

Quantum-chemical insights from deep tensor neural networks

PubMed Central

Schütt, Kristof T.; Arbabzadah, Farhad; Chmiela, Stefan; Müller, Klaus R.; Tkatchenko, Alexandre

2017-01-01

Learning from data has led to paradigm shifts in a multitude of disciplines, including web, text and image search, speech recognition, as well as bioinformatics. Can machine learning enable similar breakthroughs in understanding quantum many-body systems? Here we develop an efficient deep learning approach that enables spatially and chemically resolved insights into quantum-mechanical observables of molecular systems. We unify concepts from many-body Hamiltonians with purpose-designed deep tensor neural networks, which leads to size-extensive and uniformly accurate (1 kcal mol−1) predictions in compositional and configurational chemical space for molecules of intermediate size. As an example of chemical relevance, the model reveals a classification of aromatic rings with respect to their stability. Further applications of our model for predicting atomic energies and local chemical potentials in molecules, reliable isomer energies, and molecules with peculiar electronic structure demonstrate the potential of machine learning for revealing insights into complex quantum-chemical systems. PMID:28067221

Quantum-chemical insights from deep tensor neural networks.

PubMed

Schütt, Kristof T; Arbabzadah, Farhad; Chmiela, Stefan; Müller, Klaus R; Tkatchenko, Alexandre

2017-01-09

Learning from data has led to paradigm shifts in a multitude of disciplines, including web, text and image search, speech recognition, as well as bioinformatics. Can machine learning enable similar breakthroughs in understanding quantum many-body systems? Here we develop an efficient deep learning approach that enables spatially and chemically resolved insights into quantum-mechanical observables of molecular systems. We unify concepts from many-body Hamiltonians with purpose-designed deep tensor neural networks, which leads to size-extensive and uniformly accurate (1 kcal mol -1 ) predictions in compositional and configurational chemical space for molecules of intermediate size. As an example of chemical relevance, the model reveals a classification of aromatic rings with respect to their stability. Further applications of our model for predicting atomic energies and local chemical potentials in molecules, reliable isomer energies, and molecules with peculiar electronic structure demonstrate the potential of machine learning for revealing insights into complex quantum-chemical systems.

Defect-Induced Hedgehog Polarization States in Multiferroics.

PubMed

Li, Linze; Cheng, Xiaoxing; Jokisaari, Jacob R; Gao, Peng; Britson, Jason; Adamo, Carolina; Heikes, Colin; Schlom, Darrell G; Chen, Long-Qing; Pan, Xiaoqing

2018-03-30

Continuous developments in nanotechnology require new approaches to materials synthesis that can produce novel functional structures. Here, we show that nanoscale defects, such as nonstoichiometric nanoregions (NSNRs), can act as nano-building blocks for creating complex electrical polarization structures in the prototypical multiferroic BiFeO_{3}. An array of charged NSNRs are produced in BiFeO_{3} thin films by tuning the substrate temperature during film growth. Atomic-scale scanning transmission electron microscopy imaging reveals exotic polarization rotation patterns around these NSNRs. These polarization patterns resemble hedgehog or vortex topologies and can cause local changes in lattice symmetries leading to mixed-phase structures resembling the morphotropic phase boundary with high piezoelectricity. Phase-field simulations indicate that the observed polarization configurations are mainly induced by charged states at the NSNRs. Engineering defects thus may provide a new route for developing ferroelectric- or multiferroic-based nanodevices.

Exciton characteristics in graphene epoxide.

PubMed

Zhu, Xi; Su, Haibin

2014-02-25

Exciton characteristics in graphene epoxide (GE) are investigated by density functional theory with quasi-particle corrections and many-body interactions. The nature of the exciton is influenced by epoxide content and detailed geometric configurations. Two kinds of excitons are identified in GE: Frenkel-like exciton originated from the sp(2) carbon cluster and charge-transfer exciton formed by localized states involving both oxygen and carbon atoms. The unusual blue shift associated with the Frenkel-like exciton leaking is highlighted. One scaling relationship is proposed to address the power-law dependence of Frenkel-like exciton binding strength on its size. The charge-transfer exciton appears in GE samples with the high oxygen coverage. Particularly, the exciton in GE structures exhibits long lifetime by analyzing both radiative and nonradiative decay processes. This study sheds light on the potential applications of GE-based structures with attractive high quantum yield in light emission and optoelectronic technology.

Frustration by design

DOE PAGES

Gilbert, Ian; Nisoli, Cristiano; Schiffer, Peter

2016-07-01

Geometrical frustration is a condition that occurs when a material’s lattice geometry precludes minimizing the energy of all the interactions among pairs of neighbors simultaneously. Moreover, the simplest example is three antiferromagnetically coupled Ising spins, pointing up or down, on the corners of an equilateral triangle: It is also impossible to arrange the spins so that each pair is antiparallel. In more complex magnetic lattices, the frustrated state can arise from the combination of lattice geometry and the strength and sign of the interactions among the magnetic dipole moments.1 (See the article by Roderich Moessner and Art Ramirez, Physics Today,more » February 2006, page 24.) A wide variety of exotic and collective phenomena sometimes arises from the competing interactions. One prime example is spin liquids, materials in which the local atomic moments fluctuate down to the lowest accessible temperatures and never settle into a static ground-state configuration.« less

Quantum-chemical insights from deep tensor neural networks

NASA Astrophysics Data System (ADS)

Schütt, Kristof T.; Arbabzadah, Farhad; Chmiela, Stefan; Müller, Klaus R.; Tkatchenko, Alexandre

2017-01-01

Learning from data has led to paradigm shifts in a multitude of disciplines, including web, text and image search, speech recognition, as well as bioinformatics. Can machine learning enable similar breakthroughs in understanding quantum many-body systems? Here we develop an efficient deep learning approach that enables spatially and chemically resolved insights into quantum-mechanical observables of molecular systems. We unify concepts from many-body Hamiltonians with purpose-designed deep tensor neural networks, which leads to size-extensive and uniformly accurate (1 kcal mol-1) predictions in compositional and configurational chemical space for molecules of intermediate size. As an example of chemical relevance, the model reveals a classification of aromatic rings with respect to their stability. Further applications of our model for predicting atomic energies and local chemical potentials in molecules, reliable isomer energies, and molecules with peculiar electronic structure demonstrate the potential of machine learning for revealing insights into complex quantum-chemical systems.

Reconciling Structural and Thermodynamic Predictions Using All-Atom and Coarse-Grain Force Fields: The Case of Charged Oligo-Arginine Translocation into DMPC Bilayers

PubMed Central

2015-01-01

Using the translocation of short, charged cationic oligo-arginine peptides (mono-, di-, and triarginine) from bulk aqueous solution into model DMPC bilayers, we explore the question of the similarity of thermodynamic and structural predictions obtained from molecular dynamics simulations using all-atom and Martini coarse-grain force fields. Specifically, we estimate potentials of mean force associated with translocation using standard all-atom (CHARMM36 lipid) and polarizable and nonpolarizable Martini force fields, as well as a series of modified Martini-based parameter sets. We find that we are able to reproduce qualitative features of potentials of mean force of single amino acid side chain analogues into model bilayers. In particular, modifications of peptide–water and peptide–membrane interactions allow prediction of free energy minima at the bilayer–water interface as obtained with all-atom force fields. In the case of oligo-arginine peptides, the modified parameter sets predict interfacial free energy minima as well as free energy barriers in almost quantitative agreement with all-atom force field based simulations. Interfacial free energy minima predicted by a modified coarse-grained parameter set are −2.51, −4.28, and −5.42 for mono-, di-, and triarginine; corresponding values from all-atom simulations are −0.83, −3.33, and −3.29, respectively, all in units of kcal/mol. We found that a stronger interaction between oligo-arginine and the membrane components and a weaker interaction between oligo-arginine and water are crucial for producing such minima in PMFs using the polarizable CG model. The difference between bulk aqueous and bilayer center states predicted by the modified coarse-grain force field are 11.71, 14.14, and 16.53 kcal/mol, and those by the all-atom model are 6.94, 8.64, and 12.80 kcal/mol; those are of almost the same order of magnitude. Our simulations also demonstrate a remarkable similarity in the structural aspects of the ensemble of configurations generated using the all-atom and coarse-grain force fields. Both resolutions show that oligo-arginine peptides adopt preferential orientations as they translocate into the bilayer. The guiding theme centers on charged groups maintaining coordination with polar and charged bilayer components as well as local water. We also observe similar behaviors related with membrane deformations. PMID:25290376

Reconciling structural and thermodynamic predictions using all-atom and coarse-grain force fields: the case of charged oligo-arginine translocation into DMPC bilayers.

PubMed

Hu, Yuan; Sinha, Sudipta Kumar; Patel, Sandeep

2014-10-16

Using the translocation of short, charged cationic oligo-arginine peptides (mono-, di-, and triarginine) from bulk aqueous solution into model DMPC bilayers, we explore the question of the similarity of thermodynamic and structural predictions obtained from molecular dynamics simulations using all-atom and Martini coarse-grain force fields. Specifically, we estimate potentials of mean force associated with translocation using standard all-atom (CHARMM36 lipid) and polarizable and nonpolarizable Martini force fields, as well as a series of modified Martini-based parameter sets. We find that we are able to reproduce qualitative features of potentials of mean force of single amino acid side chain analogues into model bilayers. In particular, modifications of peptide-water and peptide-membrane interactions allow prediction of free energy minima at the bilayer-water interface as obtained with all-atom force fields. In the case of oligo-arginine peptides, the modified parameter sets predict interfacial free energy minima as well as free energy barriers in almost quantitative agreement with all-atom force field based simulations. Interfacial free energy minima predicted by a modified coarse-grained parameter set are -2.51, -4.28, and -5.42 for mono-, di-, and triarginine; corresponding values from all-atom simulations are -0.83, -3.33, and -3.29, respectively, all in units of kcal/mol. We found that a stronger interaction between oligo-arginine and the membrane components and a weaker interaction between oligo-arginine and water are crucial for producing such minima in PMFs using the polarizable CG model. The difference between bulk aqueous and bilayer center states predicted by the modified coarse-grain force field are 11.71, 14.14, and 16.53 kcal/mol, and those by the all-atom model are 6.94, 8.64, and 12.80 kcal/mol; those are of almost the same order of magnitude. Our simulations also demonstrate a remarkable similarity in the structural aspects of the ensemble of configurations generated using the all-atom and coarse-grain force fields. Both resolutions show that oligo-arginine peptides adopt preferential orientations as they translocate into the bilayer. The guiding theme centers on charged groups maintaining coordination with polar and charged bilayer components as well as local water. We also observe similar behaviors related with membrane deformations.

Approaching the theoretical limit in periodic local MP2 calculations with atomic-orbital basis sets: the case of LiH.

PubMed

Usvyat, Denis; Civalleri, Bartolomeo; Maschio, Lorenzo; Dovesi, Roberto; Pisani, Cesare; Schütz, Martin

2011-06-07

The atomic orbital basis set limit is approached in periodic correlated calculations for solid LiH. The valence correlation energy is evaluated at the level of the local periodic second order Møller-Plesset perturbation theory (MP2), using basis sets of progressively increasing size, and also employing "bond"-centered basis functions in addition to the standard atom-centered ones. Extended basis sets, which contain linear dependencies, are processed only at the MP2 stage via a dual basis set scheme. The local approximation (domain) error has been consistently eliminated by expanding the orbital excitation domains. As a final result, it is demonstrated that the complete basis set limit can be reached for both HF and local MP2 periodic calculations, and a general scheme is outlined for the definition of high-quality atomic-orbital basis sets for solids. © 2011 American Institute of Physics

Local-feature analysis for automated coarse-graining of bulk-polymer molecular dynamics simulations.

PubMed

Xue, Y; Ludovice, P J; Grover, M A

2012-12-01

A method for automated coarse-graining of bulk polymers is presented, using the data-mining tool of local feature analysis. Most existing methods for polymer coarse-graining define superatoms based on their covalent bonding topology along the polymer backbone, but here superatoms are defined based only on their correlated motions, as observed in molecular dynamics simulations. Correlated atomic motions are identified in the simulation data using local feature analysis, between atoms in the same or in different polymer chains. Groups of highly correlated atoms constitute the superatoms in the coarse-graining scheme, and the positions of their seed coordinates are then projected forward in time. Based on only the seed positions, local feature analysis enables the full reconstruction of all atomic positions. This reconstruction suggests an iterative scheme to reduce the computation of the simulations to initialize another short molecular dynamic simulation, identify new superatoms, and again project forward in time.