A Simple Demonstration of Atomic and Molecular Orbitals Using Circular Magnets

ERIC Educational Resources Information Center

Chakraborty, Maharudra; Mukhopadhyay, Subrata; Das, Ranendu Sekhar

2014-01-01

A quite simple and inexpensive technique is described here to represent the approximate shapes of atomic orbitals and the molecular orbitals formed by them following the principles of the linear combination of atomic orbitals (LCAO) method. Molecular orbitals of a few simple molecules can also be pictorially represented. Instructors can employ the…

Photoexcitation of atoms by Laguerre-Gaussian beams

NASA Astrophysics Data System (ADS)

Peshkov, A. A.; Seipt, D.; Surzhykov, A.; Fritzsche, S.

2017-08-01

In a recent experiment, Schmiegelow et al. [Nat. Commun. 7, 12998 (2016), 10.1038/ncomms12998] investigated the magnetic sublevel population of Ca+ ions in a Laguerre-Gaussian light beam if the target atoms were just centered along the beam axis. They demonstrated in this experiment that the sublevel population of the excited atoms is uniquely defined by the projection of the orbital angular momentum of the incident light. However, little attention has been paid so far to the question of how the magnetic sublevels are populated when atoms are displaced from the beam axis by some impact parameter b . Here, we analyze this sublevel population for different atomic impact parameters in first-order perturbation theory and by making use of the density-matrix formalism. Detailed calculations are performed especially for the 4 s 1/2 2S →3 d 5/2 2 transition in Ca+ ions and for the vector potential of a Laguerre-Gaussian beam in Coulomb gauge. It is shown that the magnetic sublevel population of the excited 5/2 2D level varies significantly with the impact parameter and is sensitive to the polarization, the radial index, as well as the orbital angular momentum of the incident light beam.

Atomic orbitals in molecules: general electronegativity and improvement of Mulliken population analysis.

PubMed

Lu, Haigang; Dai, Dadi; Yang, Pin; Li, Lemin

2006-01-21

An approach of atomic orbitals in molecules (AOIM) has been developed to study the atomic properties in molecules, in which the molecular orbitals are expressed in terms of the optimized minimal atomic orbitals. The atomic electronegativities are calculated using Pauling's electronegativity of free atom and are employed to find the electronegativity equilibrium in molecules and to describe the amphoteric properties of the transition metals from the groups 4 to 10. AOIM can also improve the numerical stability and accuracy of the original Mulliken population analysis.

Operation of the computer model for direct atomic oxygen exposure of Earth satellites

NASA Technical Reports Server (NTRS)

Bourassa, R. J.; Gruenbaum, P. E.; Gillis, J. R.; Hargraves, C. R.

1995-01-01

One of the primary causes of material degradation in low Earth orbit (LEO) is exposure to atomic oxygen. When atomic oxygen molecules collide with an orbiting spacecraft, the relative velocity is 7 to 8 km/sec and the collision energy is 4 to 5 eV per atom. Under these conditions, atomic oxygen may initiate a number of chemical and physical reactions with exposed materials. These reactions contribute to material degradation, surface erosion, and contamination. Interpretation of these effects on materials and the design of space hardware to withstand on-orbit conditions requires quantitative knowledge of the atomic oxygen exposure environment. Atomic oxygen flux is a function of orbit altitude, the orientation of the orbit plan to the Sun, solar and geomagnetic activity, and the angle between exposed surfaces and the spacecraft heading. We have developed a computer model to predict the atomic oxygen exposure of spacecraft in low Earth orbit. The application of this computer model is discussed.

Polarized atomic orbitals for self-consistent field electronic structure calculations

NASA Astrophysics Data System (ADS)

Lee, Michael S.; Head-Gordon, Martin

1997-12-01

We present a new self-consistent field approach which, given a large "secondary" basis set of atomic orbitals, variationally optimizes molecular orbitals in terms of a small "primary" basis set of distorted atomic orbitals, which are simultaneously optimized. If the primary basis is taken as a minimal basis, the resulting functions are termed polarized atomic orbitals (PAO's) because they are valence (or core) atomic orbitals which have distorted or polarized in an optimal way for their molecular environment. The PAO's derive their flexibility from the fact that they are formed from atom-centered linear-combinations of the larger set of secondary atomic orbitals. The variational conditions satisfied by PAO's are defined, and an iterative method for performing a PAO-SCF calculation is introduced. We compare the PAO-SCF approach against full SCF calculations for the energies, dipoles, and molecular geometries of various molecules. The PAO's are potentially useful for studying large systems that are currently intractable with larger than minimal basis sets, as well as offering potential interpretative benefits relative to calculations in extended basis sets.

Linear-scaling explicitly correlated treatment of solids: periodic local MP2-F12 method.

PubMed

Usvyat, Denis

2013-11-21

Theory and implementation of the periodic local MP2-F12 method in the 3*A fixed-amplitude ansatz is presented. The method is formulated in the direct space, employing local representation for the occupied, virtual, and auxiliary orbitals in the form of Wannier functions (WFs), projected atomic orbitals (PAOs), and atom-centered Gaussian-type orbitals, respectively. Local approximations are introduced, restricting the list of the explicitly correlated pairs, as well as occupied, virtual, and auxiliary spaces in the strong orthogonality projector to the pair-specific domains on the basis of spatial proximity of respective orbitals. The 4-index two-electron integrals appearing in the formalism are approximated via the direct-space density fitting technique. In this procedure, the fitting orbital spaces are also restricted to local fit-domains surrounding the fitted densities. The formulation of the method and its implementation exploits the translational symmetry and the site-group symmetries of the WFs. Test calculations are performed on LiH crystal. The results show that the periodic LMP2-F12 method substantially accelerates basis set convergence of the total correlation energy, and even more so the correlation energy differences. The resulting energies are quite insensitive to the resolution-of-the-identity domain sizes and the quality of the auxiliary basis sets. The convergence with the orbital domain size is somewhat slower, but still acceptable. Moreover, inclusion of slightly more diffuse functions, than those usually used in the periodic calculations, improves the convergence of the LMP2-F12 correlation energy with respect to both the size of the PAO-domains and the quality of the orbital basis set. At the same time, the essentially diffuse atomic orbitals from standard molecular basis sets, commonly utilized in molecular MP2-F12 calculations, but problematic in the periodic context, are not necessary for LMP2-F12 treatment of crystals.

The Chocolate Shop and Atomic Orbitals: A New Atomic Model Created by High School Students to Teach Elementary Students

ERIC Educational Resources Information Center

Liguori, Lucia

2014-01-01

Atomic orbital theory is a difficult subject for many high school and beginning undergraduate students, as it includes mathematical concepts not yet covered in the school curriculum. Moreover, it requires certain ability for abstraction and imagination. A new atomic orbital model "the chocolate shop" created "by" students…

Strain effect on the adsorption, diffusion, and molecular dissociation of hydrogen on Mg (0001) surface

NASA Astrophysics Data System (ADS)

Lei, Huaping; Wang, Caizhuang; Yao, Yongxin; Wang, Yangang; Hupalo, Myron; McDougall, Dan; Tringides, Michael; Ho, Kaiming

2013-12-01

The adsorption, diffusion, and molecular dissociation of hydrogen on the biaxially strained Mg (0001) surface have been systematically investigated by the first principle calculations based on density functional theory. When the strain changes from the compressive to tensile state, the adsorption energy of H atom linearly increases while its diffusion barrier linearly decreases oppositely. The dissociation barrier of H2 molecule linearly reduces in the tensile strain region. Through the chemical bonding analysis including the charge density difference, the projected density of states and the Mulliken population, the mechanism of the strain effect on the adsorption of H atom and the dissociation of H2 molecule has been elucidated by an s-p charge transfer model. With the reduction of the orbital overlap between the surface Mg atoms upon the lattice expansion, the charge transfers from p to s states of Mg atoms, which enhances the hybridization of H s and Mg s orbitals. Therefore, the bonding interaction of H with Mg surface is strengthened and then the atomic diffusion and molecular dissociation barriers of hydrogen decrease accordingly. Our works will be helpful to understand and to estimate the influence of the lattice deformation on the performance of Mg-containing hydrogen storage materials.

Effect of phosphorus on the electronic and optical properties of naphthoxaphospholes: theoretical investigation

NASA Astrophysics Data System (ADS)

Moon, Jiwon; Kim, Minbi; Lim, Jeong Sik; Kim, Joonghan

2018-06-01

Density functional theory (DFT) and time-dependent DFT calculations were performed to elucidate the electronic and optical properties of 2-R-naphthol[2,3-d]oxaphospholes (R-NOPs). On the basis of the calculated results, the poor π overlap between the 3pz orbital of P atom and the 2pz orbitals of other atoms and increasing polarity of P atom result in a reduced energy gap between the highest occupied molecular orbital and the lowest unoccupied molecular orbital. When these two effects are considered simultaneously, the absorption energies obtained for the S1 state can be below 3.00 eV according to replace the P atom of oxaphosphole ring by As atom (increasing the poor π overlap) and change the functional groups (increasing polarity). The origin of these two effects is the inherent size of the 3p orbital of P atom. The role of P atom in the control of the electronic and optical properties of R-NOPs is clearly elucidated.

Visualizing Three-Dimensional Hybrid Atomic Orbitals Using Winplot: An Application for Student Self Instruction

ERIC Educational Resources Information Center

Saputra, Andrian; Canaval, Lorentz R.; Sunyono; Fadiawati, Noor; Diawati, Chansyanah; Setyorini, M.; Kadaritna, Nina; Kadaryanto, Budi

2015-01-01

Quick and real-time plotting equations using the Winplot software can be employed to create accurate hybrid atomic orbitals without complicated scripting. Performing this task on their own, students can more easily understand and remember hybrid atomic orbitals, in terms of shape and orientation.

Analytic energy derivatives for the calculation of the first-order molecular properties using the domain-based local pair-natural orbital coupled-cluster theory

NASA Astrophysics Data System (ADS)

Datta, Dipayan; Kossmann, Simone; Neese, Frank

2016-09-01

The domain-based local pair-natural orbital coupled-cluster (DLPNO-CC) theory has recently emerged as an efficient and powerful quantum-chemical method for the calculation of energies of molecules comprised of several hundred atoms. It has been demonstrated that the DLPNO-CC approach attains the accuracy of a standard canonical coupled-cluster calculation to about 99.9% of the basis set correlation energy while realizing linear scaling of the computational cost with respect to system size. This is achieved by combining (a) localized occupied orbitals, (b) large virtual orbital correlation domains spanned by the projected atomic orbitals (PAOs), and (c) compaction of the virtual space through a truncated pair natural orbital (PNO) basis. In this paper, we report on the implementation of an analytic scheme for the calculation of the first derivatives of the DLPNO-CC energy for basis set independent perturbations within the singles and doubles approximation (DLPNO-CCSD) for closed-shell molecules. Perturbation-independent one-particle density matrices have been implemented in order to account for the response of the CC wave function to the external perturbation. Orbital-relaxation effects due to external perturbation are not taken into account in the current implementation. We investigate in detail the dependence of the computed first-order electrical properties (e.g., dipole moment) on the three major truncation parameters used in a DLPNO-CC calculation, namely, the natural orbital occupation number cutoff used for the construction of the PNOs, the weak electron-pair cutoff, and the domain size cutoff. No additional truncation parameter has been introduced for property calculation. We present benchmark calculations on dipole moments for a set of 10 molecules consisting of 20-40 atoms. We demonstrate that 98%-99% accuracy relative to the canonical CCSD results can be consistently achieved in these calculations. However, this comes with the price of tightening the threshold for the natural orbital occupation number cutoff by an order of magnitude compared to the DLPNO-CCSD energy calculations.

Modulation of spatial spin polarization at organic spinterface by side groups

NASA Astrophysics Data System (ADS)

Qiu, Shuai; Zhang, Zhao; Miao, Yuan-yuan; Zhang, Guang-ping; Ren, Jun-feng; Wang, Chuan-kui; Hu, Gui-chao

2018-01-01

Spin polarization at benzene/Ni organic/ferromagnetic interface is investigated by applying different substituting side groups. Based on first-principle calculations, it is demonstrated that the spin polarization of the states may be tuned in magnitude and sign by the side groups, which depends on the type of side groups as well as their position in the aromatic ring. Especially, a spatial spin polarization modulation is realized at the surface with the utilization of electron donating group sbnd NH2 or electron accepting group sbnd NO2. The analysis of projected density of states onto the pz orbital of carbon atoms indicates that the side group reduces the structural symmetry of the molecule and changes the pz orbital of carbon atom at different position, which further modifies the pz-d orbital hybridization as well as the spin transfer between the molecule and the ferromagnet. This work indicates a feasible way to modulate the spatial spin polarization at organic spinterface by side groups, which deserves to be measured by spin-polarized scanning tunneling microscopy.

Is It Time to Retire the Hybrid Atomic Orbital?

ERIC Educational Resources Information Center

Grushow, Alexander

2011-01-01

A rationale for the removal of the hybrid atomic orbital from the chemistry curriculum is examined. Although the hybrid atomic orbital model does not accurately predict spectroscopic energies, many chemical educators continue to use and teach the model despite the confusion it can cause for students. Three arguments for retaining the model in the…

Testing relativity with orbiting clocks

NASA Astrophysics Data System (ADS)

Nissen, J. A.; Lipa, J. A.; Wang, S.; Avaloff, D.; Stricker, D. A.

2011-02-01

We describe the background and status of a superconducting microwave clock suitable for relativity experiments in earth orbit. The project has the capability of performing improved tests of Lorentz invariance via a Michelson-Morley type experiment, and setting new limits on nine parameters in the Standard Model Extension. If flown with a high stability atomic clock, a Kennedy-Thorndike experiment along with additional tests in general relativity could be performed.In orbit, unwanted cavity frequency variations are expected to be caused mainly by acceleration effects due to residual drag and vibration, temperature variations, and fluctuations in the energy stored in the cavity. A cavity support system has been designed to reduce acceleration effects and a high resolution thermometer has been implemented to improve temperature control.

Orbital dependent functionals: An atom projector augmented wave method implementation

NASA Astrophysics Data System (ADS)

Xu, Xiao

This thesis explores the formulation and numerical implementation of orbital dependent exchange-correlation functionals within electronic structure calculations. These orbital-dependent exchange-correlation functionals have recently received renewed attention as a means to improve the physical representation of electron interactions within electronic structure calculations. In particular, electron self-interaction terms can be avoided. In this thesis, an orbital-dependent functional is considered in the context of Hartree-Fock (HF) theory as well as the Optimized Effective Potential (OEP) method and the approximate OEP method developed by Krieger, Li, and Iafrate, known as the KLI approximation. In this thesis, the Fock exchange term is used as a simple well-defined example of an orbital-dependent functional. The Projected Augmented Wave (PAW) method developed by P. E. Blochl has proven to be accurate and efficient for electronic structure calculations for local and semi-local functions because of its accurate evaluation of interaction integrals by controlling multiple moments. We have extended the PAW method to treat orbital-dependent functionals in Hartree-Fock theory and the Optimized Effective Potential method, particularly in the KLI approximation. In the course of study we develop a frozen-core orbital approximation that accurately treats the core electron contributions for above three methods. The main part of the thesis focuses on the treatment of spherical atoms. We have investigated the behavior of PAW-Hartree Fock and PAW-KLI basis, projector, and pseudopotential functions for several elements throughout the periodic table. We have also extended the formalism to the treatment of solids in a plane wave basis and implemented PWPAW-KLI code, which will appear in future publications.

Spin-orbit interaction of light on the surface of atomically thin crystals

NASA Astrophysics Data System (ADS)

Zhou, Junxiao; Chen, Shizhen; Zhang, Wenshuai; Luo, Hailu; Wen, Shuangchun

2017-09-01

Two-dimensional (2D) atomic crystals have extraordinary electronic and photonic properties and hold great promise in the applications of photonic and optoelectronics. Here, we review some of our works about the spin-orbit interaction of light on the surface of 2D atomic crystals. First, we propose a general model to describe the spin-orbit interaction of light of the 2D free standing atomic crystal, and find that it is not necessary to involve the effective refractive index to describe the spin-orbit interaction. By developing the quantum weak measurements, we detect the spin-orbit interaction of light in 2D atomic crystals, which can act as a simple method for defining the layer numbers of graphene. Moreover, we find the transverse spin-dependent splitting in the photonic spin Hall effect exhibits a quantized behavior. Furthermore, the spin-orbit interaction of light for the case of air-topological insulator interface can be routed by adjusting the strength of the axion coupling. These basic finding may enhance the comprehension of the spin-orbit interaction, and find the important application in optoelectronic.

Intrinsic Resolution of Molecular Electronic Wave Functions and Energies in Terms of Quasi-atoms and Their Interactions.

PubMed

West, Aaron C; Schmidt, Michael W; Gordon, Mark S; Ruedenberg, Klaus

2017-02-09

A general intrinsic energy resolution has been formulated for strongly correlated wave functions in the full molecular valence space and its subspaces. The information regarding the quasi-atomic organization of the molecular electronic structure is extracted from the molecular wave function without introducing any additional postulated model state wave functions. To this end, the molecular wave function is expressed in terms of quasi-atomic molecular orbitals, which maximize the overlap between subspaces of the molecular orbital space and the free-atom orbital spaces. As a result, the molecular wave function becomes the superposition of a wave function representing the juxtaposed nonbonded quasi-atoms and a wave function describing the interatomic electron migrations that create bonds through electron sharing. The juxtaposed nonbonded quasi-atoms are shown to consist of entangled quasi-atomic states from different atoms. The binding energy is resolved as a sum of contributions that are due to quasi-atom formation, quasiclassical electrostatic interactions, and interatomic interferences caused by electron sharing. The contributions are further resolved according to orbital interactions. The various transformations that generate the analysis are determined by criteria that are independent of the working orbital basis used for calculating the molecular wave function. The theoretical formulation of the resolution is quantitatively validated by an application to the C 2 molecule.

How localized is ``local?'' Efficiency vs. accuracy of O(N) domain decomposition in local orbital based all-electron electronic structure theory

NASA Astrophysics Data System (ADS)

Havu, Vile; Blum, Volker; Scheffler, Matthias

2007-03-01

Numeric atom-centered local orbitals (NAO) are efficient basis sets for all-electron electronic structure theory. The locality of NAO's can be exploited to render (in principle) all operations of the self-consistency cycle O(N). This is straightforward for 3D integrals using domain decomposition into spatially close subsets of integration points, enabling critical computational savings that are effective from ˜tens of atoms (no significant overhead for smaller systems) and make large systems (100s of atoms) computationally feasible. Using a new all-electron NAO-based code,^1 we investigate the quantitative impact of exploiting this locality on two distinct classes of systems: Large light-element molecules [Alanine-based polypeptide chains (Ala)n], and compact transition metal clusters. Strict NAO locality is achieved by imposing a cutoff potential with an onset radius rc, and exploited by appropriately shaped integration domains (subsets of integration points). Conventional tight rc<= 3å have no measurable accuracy impact in (Ala)n, but introduce inaccuracies of 20-30 meV/atom in Cun. The domain shape impacts the computational effort by only 10-20 % for reasonable rc. ^1 V. Blum, R. Gehrke, P. Havu, V. Havu, M. Scheffler, The FHI Ab Initio Molecular Simulations (aims) Project, Fritz-Haber-Institut, Berlin (2006).

Using Atomic Orbitals and Kinesthetic Learning to Authentically Derive Molecular Stretching Vibrations

ERIC Educational Resources Information Center

Bridgeman, Adam J.; Schmidt, Timothy W.; Young, Nigel A.

2013-01-01

The stretching modes of ML[subscript "x"] complexes have the same symmetry as the atomic orbitals on M that are used to form its s bonds. In the exercise suggested here, the atomic orbitals are used to derive the form of the stretching modes without the need for formal group theory. The analogy allows students to help understand many…

Simulation of the low earth orbital atomic oxygen interaction with materials by means of an oxygen ion beam

NASA Technical Reports Server (NTRS)

Banks, Bruce A.; Rutledge, Sharon K.; Paulsen, Phillip E.; Steuber, Thomas J.

1989-01-01

Atomic oxygen is the predominant species in low-Earth orbit between the altitudes of 180 and 650 km. These highly reactive atoms are a result of photodissociation of diatomic oxygen molecules from solar photons having a wavelength less than or equal to 2430A. Spacecraft in low-Earth orbit collide with atomic oxygen in the 3P ground state at impact energies of approximately 4.2 to 4.5 eV. As a consequence, organic materials previously used for high altitude geosynchronous spacecraft are severely oxidized in the low-Earth orbital environment. The evaluation of materials durability to atomic oxygen requires ground simulation of this environment to cost effectively screen materials for durability. Directed broad beam oxygen sources are necessary to evaluate potential spacecraft materials performance before and after exposure to the simulated low-Earth orbital environment. This paper presents a description of a low energy, broad oxygen ion beam source used to simulate the low-Earth orbital atomic oxygen environment. The results of materials interaction with this beam and comparison with actual in-space tests of the same meterials will be discussed. Resulting surface morphologies appear to closely replicate those observed in space tests.

The calculated magnetic, electronic and thermodynamic properties of Ce{sub 3}Co{sub 29}Si{sub 4}B{sub 10} compound

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

Huo, Jin-Rong; Wang, Xiao-Xu; Cloud Computing Department, Beijing Computing Center, Beijing 100084

2016-05-15

The magnetic moment, lattice parameter and atom fraction coordinates for Ce{sub 3}Co{sub 29}Si{sub 4}B{sub 10} are calculated by the first-principles GGA+U method, and the results indicate that the calculated and experimental values are basically accordant when U=2.6 eV. We study the interaction effect and orbital hybridization between Co and Ce atoms. The projected density of states at U=2.6 eV which provided by Co-2c, Ce-2b and Ce-4d sites are contrasted with else U values. Meanwhile the electron density of states for different sites and the distance between various atoms are exhibited. In addition, the thermodynamic properties of Ce{sub 3}Co{sub 29}Si{sub 4}B{submore » 10} are evaluated by using a series of interatomic pair potentials. - Graphical abstract: Change of the total magnetic moment for Ce{sub 3}Co{sub 29}Si{sub 4}B{sub 10} along with the value of U. There is a sharply decline of the curve at U=2.6 eV and, at the moment, the total magnetic moment of the compound have a good agreement with the experimental data. - Highlights: • We research of quaternary rare earth and transition metal compounds. • We perform the calculation of magnetic moment and electronic structure by GGA+U method. • The orbital hybridization between Co and Ce atoms is displayed and analyzed. • Show the plot of projected density of states for different sites more clearly. • Calculate the thermodynamic property of rare-earth transition metal compound.« less

Self-consistent self-interaction corrected density functional theory calculations for atoms using Fermi-Löwdin orbitals: Optimized Fermi-orbital descriptors for Li-Kr

NASA Astrophysics Data System (ADS)

Kao, Der-you; Withanage, Kushantha; Hahn, Torsten; Batool, Javaria; Kortus, Jens; Jackson, Koblar

2017-10-01

In the Fermi-Löwdin orbital method for implementing self-interaction corrections (FLO-SIC) in density functional theory (DFT), the local orbitals used to make the corrections are generated in a unitary-invariant scheme via the choice of the Fermi orbital descriptors (FODs). These are M positions in 3-d space (for an M-electron system) that can be loosely thought of as classical electron positions. The orbitals that minimize the DFT energy including the SIC are obtained by finding optimal positions for the FODs. In this paper, we present optimized FODs for the atoms from Li-Kr obtained using an unbiased search method and self-consistent FLO-SIC calculations. The FOD arrangements display a clear shell structure that reflects the principal quantum numbers of the orbitals. We describe trends in the FOD arrangements as a function of atomic number. FLO-SIC total energies for the atoms are presented and are shown to be in close agreement with the results of previous SIC calculations that imposed explicit constraints to determine the optimal local orbitals, suggesting that FLO-SIC yields the same solutions for atoms as these computationally demanding earlier methods, without invoking the constraints.

Photonic Interrogation and Control of Nano Processes

NASA Technical Reports Server (NTRS)

Jassemnejad, Baha

2003-01-01

My research activities for the summer of 2003 consisted of two projects: One project was concerned with determining a method for predicting the static and dynamic assembly properties of nano-structures using laser tweezers. The other project was to investigate the generation of Laguerre-Gaussian modes using a spatial light modulator incorporated into an optical tweezers system. Concerning the first project, I initially pursued the approach suggested by my NASA colleague Dr. Art Decker. This approach involved mimicking the model of the structure of atomic nucleus for the assembly of 1 to 100 atoms using allowed quadruple transitions induced by orbital angular momentums of a Laguerre- Gaussian (Doughnut) laser mode. After realizing the inaptness of the nuclear model with the nanostructure model as far as the binding forces and transitions were concerned, I focused on using quantum dot modei. This model was not attuned also for the host lattice influences the electronic structure of the quantum dot. Thus one other option that I decided to pursue was the approach of molecular quantum mechanics. In this approach the nanostructure is treated as a large (10-100 nm) molecule constructed from single element or multi-elements. Subsequent to consultation with Dr. Fred Morales, a chemical engineer at NASA GRC, and Dr. David Ball, a computational chemist at Cleveland State University, I acquired a molecular-quantum computation software, Hyperchem 7.0. This software allows simulation of different molecular structures as far as their static and dynamic behaviors are concerned. The time that I spent on this project was about eight weeks. Once this suitable approach was identified, I realized the need to collaborate with a computational quantum chemist to pursue searching for stable nanostructures in the range of 10-100 nm that we can be assembled using laser tweezers. The second project was about generating laser tweezers that possess orbital angular momentum. As shown, we were able to generate laser tweezers modes of different orbital angular momentum using a spatial light modulator incorporated into a laser tweezers system. The motivation for investigating these types of modes stems from being able to spin particles at high speeds and also to orient two particles in separate traps and then join them together. Also, there has been recent intense interest on fundamental physics research on orbital angular momentum of light. The fact that circularly polarized light may have associated with it angular momentum that relates to the spin of individual photons (spin 0 for the plane polarized light, spin +1 for the right-circularly polarized light and spin -1 for the left-circularly polarized light) was first demonstrated by Beth in 1936. Orbital angular momentum is, however, distinct from spin in that the spin angular momentum of light is intrinsically linked to the behavior of the electric field in the light whereas orbital angular momentum is a consequence of inclined wavefronts. In 1992 L. Allen, et al showed that the Laguerre-Gaussian (LG) modes could possess well-defined orbital angular momentum that can exceed 1 planck's constant, i.e. l plancks constant per photon, where l is the azimuthal index of the mode.

Intrinsic Resolution of Molecular Electronic Wave Functions and Energies in Terms of Quasi-atoms and Their Interactions

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

West, Aaron C.; Schmidt, Michael W.; Gordon, Mark S.

A general intrinsic energy resolution has been formulated for strongly correlated wave functions in the full molecular valence space and its subspaces. The information regarding the quasi-atomic organization of the molecular electronic structure is extracted from the molecular wave function without introducing any additional postulated model state wave functions. To this end, the molecular wave function is expressed in terms of quasi-atomic molecular orbitals, which maximize the overlap between subspaces of the molecular orbital space and the free-atom orbital spaces. As a result, the molecular wave function becomes the superposition of a wave function representing the non-bonded juxtaposed quasi-atoms andmore » a wave function describing the interatomic electron migrations that create bonds through electron sharing. The juxtaposed nonbonded quasi-atoms are shown to consist of entangled quasi-atomic states from different atoms. The binding energy is resolved as a sum of contributions that are due to quasi-atom formation, quasiclassical electrostatic interactions and interatomic interferences caused by electron sharing. The contributions are further resolved according to orbital interactions. The various transformations that generate the analysis are determined by criteria that are independent of the working orbital basis used for calculating the molecular wave function. Lastly, the theoretical formulation of the resolution is quantitatively validated by an application to the C 2 molecule.« less

Intrinsic Resolution of Molecular Electronic Wave Functions and Energies in Terms of Quasi-atoms and Their Interactions

DOE PAGES

West, Aaron C.; Schmidt, Michael W.; Gordon, Mark S.; ...

2017-01-30

A general intrinsic energy resolution has been formulated for strongly correlated wave functions in the full molecular valence space and its subspaces. The information regarding the quasi-atomic organization of the molecular electronic structure is extracted from the molecular wave function without introducing any additional postulated model state wave functions. To this end, the molecular wave function is expressed in terms of quasi-atomic molecular orbitals, which maximize the overlap between subspaces of the molecular orbital space and the free-atom orbital spaces. As a result, the molecular wave function becomes the superposition of a wave function representing the non-bonded juxtaposed quasi-atoms andmore » a wave function describing the interatomic electron migrations that create bonds through electron sharing. The juxtaposed nonbonded quasi-atoms are shown to consist of entangled quasi-atomic states from different atoms. The binding energy is resolved as a sum of contributions that are due to quasi-atom formation, quasiclassical electrostatic interactions and interatomic interferences caused by electron sharing. The contributions are further resolved according to orbital interactions. The various transformations that generate the analysis are determined by criteria that are independent of the working orbital basis used for calculating the molecular wave function. Lastly, the theoretical formulation of the resolution is quantitatively validated by an application to the C 2 molecule.« less

Momentum-resolved radio-frequency spectroscopy of a spin-orbit-coupled atomic Fermi gas near a Feshbach resonance in harmonic traps

NASA Astrophysics Data System (ADS)

Peng, Shi-Guo; Liu, Xia-Ji; Hu, Hui; Jiang, Kaijun

2012-12-01

We theoretically investigate the momentum-resolved radio-frequency spectroscopy of a harmonically trapped atomic Fermi gas near a Feshbach resonance in the presence of equal Rashba and Dresselhaus spin-orbit coupling. The system is qualitatively modeled as an ideal gas mixture of atoms and molecules, in which the properties of molecules, such as the wave function, binding energy, and effective mass, are determined from the two-particle solution of two interacting atoms. We calculate separately the radio-frequency response from atoms and molecules at finite temperatures by using the standard Fermi golden rule and take into account the effect of harmonic traps within local density approximation. The total radio-frequency spectroscopy is discussed as functions of temperature and spin-orbit coupling strength. Our results give a qualitative picture of radio-frequency spectroscopy of a resonantly interacting spin-orbit-coupled Fermi gas and can be directly tested in atomic Fermi gases of 40K atoms at Shanxi University and 6Li atoms at the Massachusetts Institute of Technology.

Hydrodynamics of Normal Atomic Gases with Spin-orbit Coupling

PubMed Central

Hou, Yan-Hua; Yu, Zhenhua

2015-01-01

Successful realization of spin-orbit coupling in atomic gases by the NIST scheme opens the prospect of studying the effects of spin-orbit coupling on many-body physics in an unprecedentedly controllable way. Here we derive the linearized hydrodynamic equations for the normal atomic gases of the spin-orbit coupling by the NIST scheme with zero detuning. We show that the hydrodynamics of the system crucially depends on the momentum susceptibilities which can be modified by the spin-orbit coupling. We reveal the effects of the spin-orbit coupling on the sound velocities and the dipole mode frequency of the gases by applying our formalism to the ideal Fermi gas. We also discuss the generalization of our results to other situations. PMID:26483090

Hydrodynamics of Normal Atomic Gases with Spin-orbit Coupling.

PubMed

Hou, Yan-Hua; Yu, Zhenhua

2015-10-20

Successful realization of spin-orbit coupling in atomic gases by the NIST scheme opens the prospect of studying the effects of spin-orbit coupling on many-body physics in an unprecedentedly controllable way. Here we derive the linearized hydrodynamic equations for the normal atomic gases of the spin-orbit coupling by the NIST scheme with zero detuning. We show that the hydrodynamics of the system crucially depends on the momentum susceptibilities which can be modified by the spin-orbit coupling. We reveal the effects of the spin-orbit coupling on the sound velocities and the dipole mode frequency of the gases by applying our formalism to the ideal Fermi gas. We also discuss the generalization of our results to other situations.

Laser sculpting of atomic sp, sp(2) , and sp(3) hybrid orbitals.

PubMed

Liu, Chunmei; Manz, Jörn; Yang, Yonggang

2015-01-12

Atomic sp, sp(2) , and sp(3) hybrid orbitals were introduced by Linus Pauling to explain the nature of the chemical bond. Quantum dynamics simulations show that they can be sculpted by means of a selective series of coherent laser pulses, starting from the 1s orbital of the hydrogen atom. Laser hybridization generates atoms with state-selective electric dipoles, opening up new possibilities for the study of chemical reaction dynamics and heterogeneous catalysis. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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.

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.

General contraction of Gaussian basis sets. II - Atomic natural orbitals and the calculation of atomic and molecular properties

NASA Technical Reports Server (NTRS)

Almlof, Jan; Taylor, Peter R.

1990-01-01

A recently proposed scheme for using natural orbitals from atomic configuration interaction wave functions as a basis set for linear combination of atomic orbitals (LCAO) calculations is extended for the calculation of molecular properties. For one-electron properties like multipole moments, which are determined largely by the outermost regions of the molecular wave function, it is necessary to increase the flexibility of the basis in these regions. This is most easily done by uncontracting the outermost Gaussian primitives, and/or by adding diffuse primitives. A similar approach can be employed for the calculation of polarizabilities. Properties which are not dominated by the long-range part of the wave function, such as spectroscopic constants or electric field gradients at the nucleus, can generally be treated satisfactorily with the original atomic natural orbital sets.

Creating fractional quantum Hall states with atomic clusters using light-assisted insertion of angular momentum

NASA Astrophysics Data System (ADS)

Zhang, Junyi; Beugnon, Jerome; Nascimbene, Sylvain

We describe a protocol to prepare clusters of ultracold bosonic atoms in strongly interacting states reminiscent of fractional quantum Hall states. Our scheme consists in injecting a controlled amount of angular momentum to an atomic gas using Raman transitions carrying orbital angular momentum. By injecting one unit of angular momentum per atom, one realizes a single-vortex state, which is well described by mean-field theory for large enough particle numbers. We also present schemes to realize fractional quantum Hall states, namely, the bosonic Laughlin and Moore-Read states. We investigate the requirements for adiabatic nucleation of such topological states, in particular comparing linear Landau-Zener ramps and arbitrary ramps obtained from optimized control methods. We also show that this protocol requires excellent control over the isotropic character of the trapping potential. ERC-Synergy Grant UQUAM, ANR-10-IDEX-0001-02, DIM NanoK Atocirc project.

Computing Rydberg Electron Transport Rates Using Periodic Orbits

NASA Astrophysics Data System (ADS)

Sattari, Sulimon; Mitchel, Kevin

2017-04-01

Electron transport rates in chaotic atomic systems are computable from classical periodic orbits. This technique allows for replacing a Monte Carlo simulation launching millions of orbits with a sum over tens or hundreds of properly chosen periodic orbits using a formula called the spectral determiant. A firm grasp of the structure of the periodic orbits is required to obtain accurate transport rates. We apply a technique called homotopic lobe dynamics (HLD) to understand the structure of periodic orbits to compute the ionization rate in a classically chaotic atomic system, namely the hydrogen atom in strong parallel electric and magnetic fields. HLD uses information encoded in the intersections of stable and unstable manifolds of a few orbits to compute relevant periodic orbits in the system. All unstable periodic orbits are computed up to a given period, and the ionization rate computed from periodic orbits converges exponentially to the true value as a function of the period used. Using periodic orbit continuation, the ionization rate is computed over a range of electron energy and magnetic field values. The future goal of this work is to semiclassically compute quantum resonances using periodic orbits.

In-space technology development: Atomic oxygen and orbital debris effects

NASA Technical Reports Server (NTRS)

Visentine, James T.; Potter, Andrew E., Jr.

1989-01-01

Earlier Shuttle flight experiments have shown atomic oxygen within the orbital environment can interact with many materials to produce surface recession and mass loss and combine catalytically with other constituents to generate visible and infrared glows. In addition to these effects, examinations of returned satellite hardware have shown many spacecraft materials are also susceptible to damage from high velocity impacts with orbital space debris. These effects are of particular concern for large, multi-mission spacecraft, such as Space Station and SDI operational satellites, that will operate in low-Earth orbit (LEO) during the late 1990's. Not only must these spacecraft include materials and exterior coatings that are resistant to atomic oxygen surface interactions, but these materials must also provide adequate protection against erosion and pitting that could result from numerous impacts with small particles (less than 100 microns) of orbital space debris. An overview of these concerns is presented, and activities now underway to develop materials and coatings are outlined that will provide adequate atomic protection for future spacecraft. The report also discusses atomic oxygen and orbital debris flight experiments now under development to expand our limited data base, correlate ground-based measurments with flight results, and develop an orbital debris collision warning system for use by future spacecraft.

Lattice structures and electronic properties of CIGS/CdS interface: First-principles calculations

NASA Astrophysics Data System (ADS)

Tang, Fu-Ling; Liu, Ran; Xue, Hong-Tao; Lu, Wen-Jiang; Feng, Yu-Dong; Rui, Zhi-Yuan; Huang, Min

2014-07-01

Using first-principles calculations within density functional theory, we study the atomic structures and electronic properties of the perfect and defective (2VCu+InCu) CuInGaSe2/CdS interfaces theoretically, especially the interface states. We find that the local lattice structure of (2VCu+InCu) interface is somewhat disorganized. By analyzing the local density of states projected on several atomic layers of the two interfaces models, we find that for the (2VCu+InCu) interface the interface states near the Fermi level in CuInGaSe2 and CdS band gap regions are mainly composed of interfacial Se-4p, Cu-3d and S-3p orbitals, while for the perfect interface there are no clear interface states in the CuInGaSe2 region but only some interface states which are mainly composed of S-3p orbitals in the valance band of CdS region.

Magnetic anisotropy of heteronuclear dimers in the gas phase and supported on graphene: relativistic density-functional calculations.

PubMed

Błoński, Piotr; Hafner, Jürgen

2014-04-09

The structural and magnetic properties of mixed PtCo, PtFe, and IrCo dimers in the gas phase and supported on a free-standing graphene layer have been calculated using density-functional theory, both in the scalar-relativistic limit and self-consistently including spin-orbit coupling. The influence of the strong magnetic moments of the 3d atoms on the spin and orbital moments of the 5d atoms, and the influence of the strong spin-orbit coupling contributed by the 5d atom on the orbital moments of the 3d atoms have been studied in detail. The magnetic anisotropy energy is found to depend very sensitively on the nature of the eigenstates in the vicinity of the Fermi level, as determined by band filling, exchange splitting and spin-orbit coupling. The large magnetic anisotropy energy of free PtCo and IrCo dimers relative to the easy direction parallel to the dimer axis is coupled to a strong anisotropy of the orbital magnetic moments of the Co atom for both dimers, and also on the Ir atom in IrCo. In contrast the PtFe dimer shows a weak perpendicular anisotropy and only small spin and orbital anisotropies of opposite sign on the two atoms. For dimers supported on graphene, the strong binding within the dimer and the stronger interaction of the 3d atom with the substrate stabilizes an upright geometry. Spin and orbital moments on the 3d atom are strongly quenched, but due to the weaker binding within the dimer the properties of the 5d atom are more free-atom-like with increased spin and orbital moments. The changes in the magnetic moment are reflected in the structure of the electronic eigenstates near the Fermi level, for all three dimers the easy magnetic direction is now parallel to the dimer axis and perpendicular to the graphene layer. The already very large magnetic anisotropy energy (MAE) of IrCo is further enhanced by the interaction with the support, the MAE of PtFe changes sign, and that of the PtCo dimer is reduced. These changes are discussed in relation to the relativistic electronic structure of free and supported dimers and it is demonstrated that the existence of a partially occupied quasi-degenerate state at the Fermi level favors the formation of a large magnetic anisotropy.

Simple and efficient LCAO basis sets for the diffuse states in carbon nanostructures.

PubMed

Papior, Nick R; Calogero, Gaetano; Brandbyge, Mads

2018-06-27

We present a simple way to describe the lowest unoccupied diffuse states in carbon nanostructures in density functional theory calculations using a minimal LCAO (linear combination of atomic orbitals) basis set. By comparing plane wave basis calculations, we show how these states can be captured by adding long-range orbitals to the standard LCAO basis sets for the extreme cases of planar sp 2 (graphene) and curved carbon (C 60 ). In particular, using Bessel functions with a long range as additional basis functions retain a minimal basis size. This provides a smaller and simpler atom-centered basis set compared to the standard pseudo-atomic orbitals (PAOs) with multiple polarization orbitals or by adding non-atom-centered states to the basis.

Energy level diagrams for black hole orbits

NASA Astrophysics Data System (ADS)

Levin, Janna

2009-12-01

A spinning black hole with a much smaller black hole companion forms a fundamental gravitational system, like a colossal classical analog to an atom. In an appealing if imperfect analogy with atomic physics, this gravitational atom can be understood through a discrete spectrum of periodic orbits. Exploiting a correspondence between the set of periodic orbits and the set of rational numbers, we are able to construct periodic tables of orbits and energy level diagrams of the accessible states around black holes. We also present a closed-form expression for the rational q, thereby quantifying zoom-whirl behavior in terms of spin, energy and angular momentum. The black hole atom is not just a theoretical construct, but corresponds to extant astrophysical systems detectable by future gravitational wave observatories.

Simple and efficient LCAO basis sets for the diffuse states in carbon nanostructures

NASA Astrophysics Data System (ADS)

Papior, Nick R.; Calogero, Gaetano; Brandbyge, Mads

2018-06-01

We present a simple way to describe the lowest unoccupied diffuse states in carbon nanostructures in density functional theory calculations using a minimal LCAO (linear combination of atomic orbitals) basis set. By comparing plane wave basis calculations, we show how these states can be captured by adding long-range orbitals to the standard LCAO basis sets for the extreme cases of planar sp 2 (graphene) and curved carbon (C60). In particular, using Bessel functions with a long range as additional basis functions retain a minimal basis size. This provides a smaller and simpler atom-centered basis set compared to the standard pseudo-atomic orbitals (PAOs) with multiple polarization orbitals or by adding non-atom-centered states to the basis.

Hund’s rule in superatoms with transition metal impurities

PubMed Central

Medel, Victor M.; Reveles, Jose Ulises; Khanna, Shiv N.; Chauhan, Vikas; Sen, Prasenjit; Castleman, A. Welford

2011-01-01

The quantum states in metal clusters bunch into supershells with associated orbitals having shapes resembling those in atoms, giving rise to the concept that selected clusters could mimic the characteristics of atoms and be classified as superatoms. Unlike atoms, the superatom orbitals span over multiple atoms and the filling of orbitals does not usually exhibit Hund’s rule seen in atoms. Here, we demonstrate the possibility of enhancing exchange splitting in superatom shells via a composite cluster of a central transition metal and surrounding nearly free electron metal atoms. The transition metal d states hybridize with superatom D states and result in enhanced splitting between the majority and minority sets where the moment and the splitting can be controlled by the nature of the central atom. We demonstrate these findings through studies on TMMgn clusters where TM is a 3d atom. The clusters exhibit Hund’s filling, opening the pathway to superatoms with magnetic shells. PMID:21646542

Hund's rule in superatoms with transition metal impurities.

PubMed

Medel, Victor M; Reveles, Jose Ulises; Khanna, Shiv N; Chauhan, Vikas; Sen, Prasenjit; Castleman, A Welford

2011-06-21

The quantum states in metal clusters bunch into supershells with associated orbitals having shapes resembling those in atoms, giving rise to the concept that selected clusters could mimic the characteristics of atoms and be classified as superatoms. Unlike atoms, the superatom orbitals span over multiple atoms and the filling of orbitals does not usually exhibit Hund's rule seen in atoms. Here, we demonstrate the possibility of enhancing exchange splitting in superatom shells via a composite cluster of a central transition metal and surrounding nearly free electron metal atoms. The transition metal d states hybridize with superatom D states and result in enhanced splitting between the majority and minority sets where the moment and the splitting can be controlled by the nature of the central atom. We demonstrate these findings through studies on TMMg(n) clusters where TM is a 3d atom. The clusters exhibit Hund's filling, opening the pathway to superatoms with magnetic shells.

Spin-splitting calculation for zincblende semiconductors using an atomic bond-orbital model.

PubMed

Kao, Hsiu-Fen; Lo, Ikai; Chiang, Jih-Chen; Chen, Chun-Nan; Wang, Wan-Tsang; Hsu, Yu-Chi; Ren, Chung-Yuan; Lee, Meng-En; Wu, Chieh-Lung; Gau, Ming-Hong

2012-10-17

We develop a 16-band atomic bond-orbital model (16ABOM) to compute the spin splitting induced by bulk inversion asymmetry in zincblende materials. This model is derived from the linear combination of atomic-orbital (LCAO) scheme such that the characteristics of the real atomic orbitals can be preserved to calculate the spin splitting. The Hamiltonian of 16ABOM is based on a similarity transformation performed on the nearest-neighbor LCAO Hamiltonian with a second-order Taylor expansion k at the Γ point. The spin-splitting energies in bulk zincblende semiconductors, GaAs and InSb, are calculated, and the results agree with the LCAO and first-principles calculations. However, we find that the spin-orbit coupling between bonding and antibonding p-like states, evaluated by the 16ABOM, dominates the spin splitting of the lowest conduction bands in the zincblende materials.

Hyperspherical Symmetry of Hydrogenic Orbitals and Recoupling Coefficients among Alternative Bases

NASA Astrophysics Data System (ADS)

Aquilanti, Vincenzo; Cavalli, Simonetta; Coletti, Cecilia

1998-04-01

Fock's representation of momentum space hydrogenic orbitals in terms of harmonics on the hypersphere S3 of a four-dimensional space is extended to classify alternative bases. These orbitals are of interest for Sturmian expansions of use in atomic and molecular structure calculations and for the description of atoms in fields. Because of the correspondence between the S3 manifold and the SU\\(2\\) group, new sum rules are established which are of relevance for the connection, not only among hydrogen atom orbitals in different bases, but also among the usual vector coupling coefficients and rotation matrix elements.

General contraction of Gaussian basis sets. Part 2: Atomic natural orbitals and the calculation of atomic and molecular properties

NASA Technical Reports Server (NTRS)

Almloef, Jan; Taylor, Peter R.

1989-01-01

A recently proposed scheme for using natural orbitals from atomic configuration interaction (CI) wave functions as a basis set for linear combination of atomic orbitals (LCAO) calculations is extended for the calculation of molecular properties. For one-electron properties like multipole moments, which are determined largely by the outermost regions of the molecular wave function, it is necessary to increase the flexibility of the basis in these regions. This is most easily done by uncontracting the outmost Gaussian primitives, and/or by adding diffuse primitives. A similar approach can be employed for the calculation of polarizabilities. Properties which are not dominated by the long-range part of the wave function, such as spectroscopic constants or electric field gradients at the nucleus, can generally be treated satisfactorily with the original atomic natural orbital (ANO) sets.

A theoretical NMR study of selected benzazoles: Comparison of GIPAW and GIAO-PCM (DMSO) calculations.

PubMed

Marín-Luna, Marta; Alkorta, Ibon; Elguero, José

2018-03-01

This paper compares the absolute shieldings obtained by gauge-including-projected-augmented-wave (GIPAW) to those obtained by gauge-invariant atomic orbital/Becke, 3-parameter, Lee-Yang-Parr (GIAO/B3LYP)/6-311++G(d,p)-polarizable continuum model (PCM, dimethyl sulfoxide) for nine benzazoles (benzimidazoles, indazoles, and benzotriazoles) recorded in the solid-state. Three nuclei were explored, 13 C, 15 N, and 19 F, and the gauge-including-projected-augmented-wave approach only proved better for 15 N MAS NMR. Copyright © 2017 John Wiley & Sons, Ltd.

Roothaan's approach to solve the Hartree-Fock equations for atoms confined by soft walls: Basis set with correct asymptotic behavior.

PubMed

Rodriguez-Bautista, Mariano; Díaz-García, Cecilia; Navarrete-López, Alejandra M; Vargas, Rubicelia; Garza, Jorge

2015-07-21

In this report, we use a new basis set for Hartree-Fock calculations related to many-electron atoms confined by soft walls. One- and two-electron integrals were programmed in a code based in parallel programming techniques. The results obtained with this proposal for hydrogen and helium atoms were contrasted with other proposals to study just one and two electron confined atoms, where we have reproduced or improved the results previously reported. Usually, an atom enclosed by hard walls has been used as a model to study confinement effects on orbital energies, the main conclusion reached by this model is that orbital energies always go up when the confinement radius is reduced. However, such an observation is not necessarily valid for atoms confined by penetrable walls. The main reason behind this result is that for atoms with large polarizability, like beryllium or potassium, external orbitals are delocalized when the confinement is imposed and consequently, the internal orbitals behave as if they were in an ionized atom. Naturally, the shell structure of these atoms is modified drastically when they are confined. The delocalization was an argument proposed for atoms confined by hard walls, but it was never verified. In this work, the confinement imposed by soft walls allows to analyze the delocalization concept in many-electron atoms.

Roothaan’s approach to solve the Hartree-Fock equations for atoms confined by soft walls: Basis set with correct asymptotic behavior

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

Rodriguez-Bautista, Mariano; Díaz-García, Cecilia; Navarrete-López, Alejandra M.

2015-07-21

In this report, we use a new basis set for Hartree-Fock calculations related to many-electron atoms confined by soft walls. One- and two-electron integrals were programmed in a code based in parallel programming techniques. The results obtained with this proposal for hydrogen and helium atoms were contrasted with other proposals to study just one and two electron confined atoms, where we have reproduced or improved the results previously reported. Usually, an atom enclosed by hard walls has been used as a model to study confinement effects on orbital energies, the main conclusion reached by this model is that orbital energiesmore » always go up when the confinement radius is reduced. However, such an observation is not necessarily valid for atoms confined by penetrable walls. The main reason behind this result is that for atoms with large polarizability, like beryllium or potassium, external orbitals are delocalized when the confinement is imposed and consequently, the internal orbitals behave as if they were in an ionized atom. Naturally, the shell structure of these atoms is modified drastically when they are confined. The delocalization was an argument proposed for atoms confined by hard walls, but it was never verified. In this work, the confinement imposed by soft walls allows to analyze the delocalization concept in many-electron atoms.« less

The adsorption of Run (n = 1-4) on γ-Al2O3 Surface: A DFT study

NASA Astrophysics Data System (ADS)

Liu, Zhe; Guo, Yafei; Chen, Yu; Shen, Rong

2018-05-01

The density functional theory (DFT) was adopted to study the adsorption and growth of Run (n = 1-4) clusters on γ-Al2O3 surface, which is of great significances for the design of many important catalysts, especially for carbon dioxide methanation. It is found that both the Rusbnd Ru bond length and adsorption energy Eads of Ru clusters with the surface increase with the Run clusters increasing. The growth ability of the supported Run cluster is weaker than the gas phase Run clusters through comparing their respective growth process, which ascribes to the stabilization of γ-Al2O3 support. An interesting discovery is that the basin structure was supposed to be the most favorable adsorption geometry for Run clusters. Additionally, the distances between Ru atoms in the adsorbed clusters are longer than that in their isolated counterparts. Bader charge analysis was conducted for the most stable configurations of Run (n = 1-4) clusters on γ-Al2O3 surface as well. And the results suggest that Run (n = 1-4) clusters serve as the electron donators. The result of projected density of states (PDOS) shows that strong adsorption of Ru atom on the γ-Al2O3 surface correlates with strong interaction between d orbital of Ru atom and p orbital of Al or O atom of the Al2O3 support.

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

Comparison of Atomic Oxygen Erosion Yields of Materials at Various Energy and Impact Angles

NASA Technical Reports Server (NTRS)

Banks, Bruce A.; Waters, Deborah L.; Thorson, Stephen D.; deGroh, Kim, K.; Snyder, Aaron; Miller, Sharon

2006-01-01

The atomic oxygen erosion yields of various materials, measured in volume of material oxidized per incident atomic oxygen atom, are compared to the commonly accepted standard of Kapton H (DuPont) polyimide. The ratios of the erosion yield of Kapton H to the erosion yield of various materials are not consistent at different atomic oxygen energies. Although it is most convenient to use isotropic thermal energy RF plasma ashers to assess atomic oxygen durability, the results can be misleading because the relative erosion rates at thermal energies are not necessarily the same as low Earth orbital (LEO) energies of approx.4.5 eV. An experimental investigation of the relative atomic oxygen erosion yields of a wide variety of polymers and carbon was conducted using isotropic thermal energy (approx.0.1 eV) and hyperthermal energy (approx.70 eV) atomic oxygen using an RF plasma asher and an end Hall ion source. For hyperthermal energies, the atomic oxygen erosion yields relative to normal incident Kapton H were compared for sweeping atomic oxygen arrival with that of normal incidence arrival. The results of isotropic thermal energy, normal incident, and sweeping incident atomic oxygen are also compared with measured or projected LEO values.

Relativistic Corrections to the Energy of the Electron in a Hydrogenlike Atom

NASA Astrophysics Data System (ADS)

Skobelev, V. V.

2017-11-01

Using the previously found solution of the Dirac equation for an electron in the field of the nucleus ( Ze), expressed in terms of the eigenfunction of the spin projection operator Σ3, in the expansion in the small parameter ( Zα), α = e 2/ ħc ≈ 1/137, relativistic and spin-orbit corrections to the energy of the electron in a hydrogenlike atom are calculated, where the latter, in our view, are represented in an easier to visualize form in comparison with previously known classical results. This work may be of methodological interest in the sense of some modification of the corresponding sections of the traditional course on quantum mechanics.

Non-empirical exchange-correlation parameterizations based on exact conditions from correlated orbital theory.

PubMed

Haiduke, Roberto Luiz A; Bartlett, Rodney J

2018-05-14

Some of the exact conditions provided by the correlated orbital theory are employed to propose new non-empirical parameterizations for exchange-correlation functionals from Density Functional Theory (DFT). This reparameterization process is based on range-separated functionals with 100% exact exchange for long-range interelectronic interactions. The functionals developed here, CAM-QTP-02 and LC-QTP, show mitigated self-interaction error, correctly predict vertical ionization potentials as the negative of eigenvalues for occupied orbitals, and provide nice excitation energies, even for challenging charge-transfer excited states. Moreover, some improvements are observed for reaction barrier heights with respect to the other functionals belonging to the quantum theory project (QTP) family. Finally, the most important achievement of these new functionals is an excellent description of vertical electron affinities (EAs) of atoms and molecules as the negative of appropriate virtual orbital eigenvalues. In this case, the mean absolute deviations for EAs in molecules are smaller than 0.10 eV, showing that physical interpretation can indeed be ascribed to some unoccupied orbitals from DFT.

Non-empirical exchange-correlation parameterizations based on exact conditions from correlated orbital theory

NASA Astrophysics Data System (ADS)

Haiduke, Roberto Luiz A.; Bartlett, Rodney J.

2018-05-01

Some of the exact conditions provided by the correlated orbital theory are employed to propose new non-empirical parameterizations for exchange-correlation functionals from Density Functional Theory (DFT). This reparameterization process is based on range-separated functionals with 100% exact exchange for long-range interelectronic interactions. The functionals developed here, CAM-QTP-02 and LC-QTP, show mitigated self-interaction error, correctly predict vertical ionization potentials as the negative of eigenvalues for occupied orbitals, and provide nice excitation energies, even for challenging charge-transfer excited states. Moreover, some improvements are observed for reaction barrier heights with respect to the other functionals belonging to the quantum theory project (QTP) family. Finally, the most important achievement of these new functionals is an excellent description of vertical electron affinities (EAs) of atoms and molecules as the negative of appropriate virtual orbital eigenvalues. In this case, the mean absolute deviations for EAs in molecules are smaller than 0.10 eV, showing that physical interpretation can indeed be ascribed to some unoccupied orbitals from DFT.

Dynamical screening of the van der Waals interaction between graphene layers.

PubMed

Dappe, Y J; Bolcatto, P G; Ortega, J; Flores, F

2012-10-24

The interaction between graphene layers is analyzed combining local orbital DFT and second order perturbation theory. For this purpose we use the linear combination of atomic orbitals-orbital occupancy (LCAO-OO) formalism, that allows us to separate the interaction energy as the sum of a weak chemical interaction between graphene layers plus the van der Waals interaction (Dappe et al 2006 Phys. Rev. B 74 205434). In this work, the weak chemical interaction is calculated by means of corrected-LDA calculations using an atomic-like sp(3)d(5) basis set. The van der Waals interaction is calculated by means of second order perturbation theory using an atom-atom interaction approximation and the atomic-like-orbital occupancies. We also analyze the effect of dynamical screening in the van der Waals interaction using a simple model. We find that this dynamical screening reduces by 40% the van der Waals interaction. Taking this effect into account, we obtain a graphene-graphene interaction energy of 70 ± 5 meV/atom in reasonable agreement with the experimental evidence.

QED effects on individual atomic orbital energies

NASA Astrophysics Data System (ADS)

Kozioł, Karol; Aucar, Gustavo A.

2018-04-01

Several issues, concerning QED corrections, that are important in precise atomic calculations are presented. The leading QED corrections, self-energy and vacuum polarization, to the orbital energy for selected atoms with 30 ≤ Z ≤ 118 have been calculated. The sum of QED and Breit contributions to the orbital energy is analyzed. It has been found that for ns subshells the Breit and QED contributions are of comparative size, but for np and nd subshells the Breit contribution takes a major part of the QED+Breit sum. It has also, been found that the Breit to leading QED contributions ratio for ns subshells is almost independent of Z. The Z-dependence of QED and Breit+QED contributions per subshell is shown. The fitting coefficients may be used to estimate QED effects on inner molecular orbitals. We present results of our calculations for QED contributions to orbital energy of valence ns-subshell for group 1 and 11 atoms and discuss about the reliability of these numbers by comparing them with experimental first ionization potential data.

Relative Stabilities and Reactivities of Isolated Versus Conjugated Alkenes: Reconciliation Via a Molecular Orbital Approach

NASA Astrophysics Data System (ADS)

Sotiriou-Leventis, Chariklia; Hanna, Samir B.; Leventis, Nicholas

1996-04-01

The well-accepted practice of generating a pair of molecular orbitals, one of lower energy and another of higher energy than the original pair of overlapping atomic orbitals, and the concept of a particle in a one-dimensional box are implemented in a simplified, nonmathematical method that explains the relative stabilities and reactivities of alkenes with conjugated versus isolated double bonds. In this method, Huckel-type MO's of higher polyenes are constructed by energy rules of linear combination of atomic orbitals. One additional rule is obeyed: bonding molecular orbitals overlap only with bonding molecular orbitals, and antibonding molecular orbitals overlap only with antibonding molecular orbitals.

Comparison of S-adsorption on (111) and (100) facets of Cu nanoclusters

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

Boschen, Jeffery S.; Lee, Jiyoung; Windus, Theresa L.

2016-10-31

In order to gain insight into the nature of chemical bonding of sulfur atoms on coinage metal surfaces, we compare the adsorption energy and structural parameters for sulfur at four-fold hollow (4fh) sites on (100) facets and at three-fold hollow (3fh) sites on (111) facets of Cu nanoclusters. Consistent results are obtained from localized atomic orbital and plane-wave based density functional theory using the same functionals. PBE and its hybrid counterpart (PBE0 or HSE06) also give similar results. 4fh sites are preferred over 3fh sites with stronger bonding by ~0.6 eV for nanocluster sizes above ~280 atoms. However, for smallermore » sizes there are strong variations in the binding strength and the extent of the binding site preference. In addition, we show that suitable averaging over clusters of different sizes, or smearing the occupancy of orbitals, provide useful strategies to aid assessment of the behavior in extended surface systems. From site-projected density of states analysis using the smearing technique, we show that S adsorbed on a 4fh site has similar bonding interactions with the substrate as that on a 3fh site, but with much weaker antibonding interactions.« less

Rashba spin-orbit coupling and orbital chirality in magnetic bilayers

NASA Astrophysics Data System (ADS)

Lee, Hyun-Woo

2013-03-01

The phenomenon of the Rashba spin-orbit coupling is examined theoretically for an ultrathin magnetic layer in contact with a non-magnetic heavy metal layer. From first-principles calculation, large Rashba parameter of order 1 eV .Å is obtained, which is strong enough to generate large spin transfer torque of spin-orbit coupling origin. Large Rashba parameter is attributed to the orbital mixing of 3 d magnetic atoms and non-magnetic heavy elements with significant atomic spin-orbit coupling. Interestingly the magnitude and sign of the parameter vary from energy bands to bands, which we attribute to band-specific chiral ordering of orbital angular momentum. Through a simple tight-binding model analysis, we demonstrate that d-orbital hybridization allowed by the breaking of structural inversion symmetry generates band-specific chiral ordering of orbital angular momentum, which combines with atomic spin-orbit coupling to give rise to band-specific Rashba parameter. The band-dependence of the Rashba parameter is discussed in connection with recent experiments and we argue that the dependence may be utilized to enhance device application potentials. This work is supported by NRF grant (2010-0008529, 2011-0015631, 2010-0014109, 2011-0030789).

A Molecular Dynamics of Cold Neutral Atoms Captured by Carbon Nanotube Under Electric Field and Thermal Effect as a Selective Atoms Sensor.

PubMed

Santos, Elson C; Neto, Abel F G; Maneschy, Carlos E; Chen, James; Ramalho, Teodorico C; Neto, A M J C

2015-05-01

Here we analyzed several physical behaviors through computational simulation of systems consisting of a zig-zag type carbon nanotube and relaxed cold atoms (Rb, Au, Si and Ar). These atoms were chosen due to their different chemical properties. The atoms individually were relaxed on the outside of the nanotube during the simulations. Each system was found under the influence of a uniform electric field parallel to the carbon nanotube and under the thermal effect of the initial temperature at the simulations. Because of the electric field, the cold atoms orbited the carbon nanotube while increasing the initial temperature allowed the variation of the radius of the orbiting atoms. We calculated the following quantities: kinetic energy, potential energy and total energy and in situ temperature, molar entropy variation and average radius of the orbit of the atoms. Our data suggest that only the action of electric field is enough to generate the attractive potential and this system could be used as a selected atoms sensor.

Oxygen atom reaction with shuttle materials at orbital altitudes

NASA Technical Reports Server (NTRS)

Leger, L. J.

1982-01-01

Surfaces of materials used in the space shuttle orbiter payload bay and exposed during STS-1 through STS-3 were examined after flight. Paints and polymers, in particular Kapton used on the television camera thermal blanket, showed significant change. Generally, the change was a loss of surface gloss on the polymer with apparent aging on the paint surfaces. The Kapton surfaces showed the greatest change, and postflight analyses showed mass loss of 4.8 percent on STS-2 and 35 percent on STS-3 for most heavily affected surfaces. Strong shadow patterns were evident. The greatest mass loss was measured on surfaces which were exposed to solar radiation in conjunction with exposure in the vehicle velocity vector. A mechanism which involves the interaction of atomic oxygen with organic polymer surfaces is proposed. Atomic oxygen is the major ambient species at low orbital altitudes and presents a flux of 8 x 10 to the 14th power atoms/cu cm sec for reaction. Correlation of the expected mass loss based on ground-based oxygen atom/polymer reaction rates shows lower mass loss of the Kapton than measured. Consideration of solar heating effects on reaction rates as well as the high oxygen atom energy due to the orbiter's orbital velocity brings the predicted and measured mass loss in surprisingly good agreement. Flight sample surface morphology comparison with ground based Kapton/oxygen atom exposures provides additional support for the oxygen interaction mechanism.

Automated Construction of Molecular Active Spaces from Atomic Valence Orbitals.

PubMed

Sayfutyarova, Elvira R; Sun, Qiming; Chan, Garnet Kin-Lic; Knizia, Gerald

2017-09-12

We introduce the atomic valence active space (AVAS), a simple and well-defined automated technique for constructing active orbital spaces for use in multiconfiguration and multireference (MR) electronic structure calculations. Concretely, the technique constructs active molecular orbitals capable of describing all relevant electronic configurations emerging from a targeted set of atomic valence orbitals (e.g., the metal d orbitals in a coordination complex). This is achieved via a linear transformation of the occupied and unoccupied orbital spaces from an easily obtainable single-reference wave function (such as from a Hartree-Fock or Kohn-Sham calculations) based on projectors to targeted atomic valence orbitals. We discuss the premises, theory, and implementation of the idea, and several of its variations are tested. To investigate the performance and accuracy, we calculate the excitation energies for various transition-metal complexes in typical application scenarios. Additionally, we follow the homolytic bond breaking process of a Fenton reaction along its reaction coordinate. While the described AVAS technique is not a universal solution to the active space problem, its premises are fulfilled in many application scenarios of transition-metal chemistry and bond dissociation processes. In these cases the technique makes MR calculations easier to execute, easier to reproduce by any user, and simplifies the determination of the appropriate size of the active space required for accurate results.

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

Spin-orbit-coupled fermions in an optical lattice clock

NASA Astrophysics Data System (ADS)

Kolkowitz, S.; Bromley, S. L.; Bothwell, T.; Wall, M. L.; Marti, G. E.; Koller, A. P.; Zhang, X.; Rey, A. M.; Ye, J.

2017-02-01

Engineered spin-orbit coupling (SOC) in cold-atom systems can enable the study of new synthetic materials and complex condensed matter phenomena. However, spontaneous emission in alkali-atom spin-orbit-coupled systems is hindered by heating, limiting the observation of many-body effects and motivating research into potential alternatives. Here we demonstrate that spin-orbit-coupled fermions can be engineered to occur naturally in a one-dimensional optical lattice clock. In contrast to previous SOC experiments, here the SOC is both generated and probed using a direct ultra-narrow optical clock transition between two electronic orbital states in 87Sr atoms. We use clock spectroscopy to prepare lattice band populations, internal electronic states and quasi-momenta, and to produce spin-orbit-coupled dynamics. The exceptionally long lifetime of the excited clock state (160 seconds) eliminates decoherence and atom loss from spontaneous emission at all relevant experimental timescales, allowing subsequent momentum- and spin-resolved in situ probing of the SOC band structure and eigenstates. We use these capabilities to study Bloch oscillations, spin-momentum locking and Van Hove singularities in the transition density of states. Our results lay the groundwork for using fermionic optical lattice clocks to probe new phases of matter.

Applying Molecular Bonding Concepts to the Solid State

NASA Astrophysics Data System (ADS)

Dunnington, Benjamin D.

In this thesis, we describe the extension and application of Natural Bond Orbital (NBO) analysis to periodic systems. This enables the translation of rigorous, quantum mechanical calculation results of solid systems into the localized lone pairs and two-center bonds of Lewis structures. Such localized bonding descriptions form the basic language of chemistry, and application of these ideas to solids allows for the understanding of complex phenomena in bulk systems using readily accessible concepts from molecular science. In addition to the algorithmic adjustments needed for to account for periodic boundary conditions in the NBO process, we also discuss methodology to interface the ubiquitous plane wave basis sets of the solid state with the atom-centered basis functions needed as input for NBO analysis. We will describe one method using projection of the plane wave eigenstates, and a second projection-free method that involves the direct calculation of matrix elements of the plane wave Hamiltonian in an atom-centered basis. The reliance of many localized, post-computational analysis techniques on an atom-centered description of the orbitals, means these interfaces will have applicability beyond our NBO development. An ideal area for application of such molecular descriptions of periodic systems is heterogeneous catalysis, where reactants from a gas/liquid phase react on a solid catalyst surface. Previous studies of these systems have originated from the delocalized perspective of the bulk catalyst. NBO provides an explicit description of the perturbative effect of the catalyst on the covalent bonds of the reactant, which is correlated with the catalytic activity of the material. Such a shift to an adsorbate focused description of surface reactivity will enable understanding of catalysis across a variety of materials.

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.

Symmetry and equivalence restrictions in electronic structure calculations

NASA Technical Reports Server (NTRS)

Bauschlicher, Charles W., Jr.; Taylor, Peter R.

1988-01-01

A simple method for obtaining MCSCF orbitals and CI natural orbitals adapted to degenerate point groups, with full symmetry and equivalnece restrictions, is described. Among several advantages accruing from this method are the ability to perform atomic SCF calculations on states for which the SCF energy expression cannot be written in terms of Coulomb and exchange integrals over real orbitals, and the generation of symmetry-adapted atomic natural orbitals for use in a recently proposed method for basis set contraction.

Measure synchronization in a spin-orbit-coupled bosonic Josephson junction

NASA Astrophysics Data System (ADS)

Wang, Wen-Yuan; Liu, Jie; Fu, Li-Bin

2015-11-01

We present measure synchronization (MS) in a bosonic Josephson junction with spin-orbit coupling. The two atomic hyperfine states are coupled by a Raman dressing scheme, and they are regarded as two orientations of a pseudo-spin-1 /2 system. A feature specific to a spin-orbit-coupled (SOC) bosonic Josephson junction is that the transition from non-MS to MS dynamics can be modulated by Raman laser intensity, even in the absence of interspin atomic interaction. A phase diagram of non-MS and MS dynamics as functions of Raman laser intensity and Josephson tunneling amplitude is presented. Taking into account interspin atomic interactions, the system exhibits MS breaking dynamics resulting from the competition between intraspin and interspin atomic interactions. When interspin atomic interactions dominate in the competition, the system always exhibits MS dynamics. For interspin interaction weaker than intraspin interaction, a window for non-MS dynamics is present. Since SOC Bose-Einstein condensates provide a powerful platform for studies on physical problems in various fields, the study of MS dynamics is valuable in researching the collective coherent dynamical behavior in a spin-orbit-coupled bosonic Josephson junction.

An efficient and near linear scaling pair natural orbital based local coupled cluster method.

PubMed

Riplinger, Christoph; Neese, Frank

2013-01-21

In previous publications, it was shown that an efficient local coupled cluster method with single- and double excitations can be based on the concept of pair natural orbitals (PNOs) [F. Neese, A. Hansen, and D. G. Liakos, J. Chem. Phys. 131, 064103 (2009)]. The resulting local pair natural orbital-coupled-cluster single double (LPNO-CCSD) method has since been proven to be highly reliable and efficient. For large molecules, the number of amplitudes to be determined is reduced by a factor of 10(5)-10(6) relative to a canonical CCSD calculation on the same system with the same basis set. In the original method, the PNOs were expanded in the set of canonical virtual orbitals and single excitations were not truncated. This led to a number of fifth order scaling steps that eventually rendered the method computationally expensive for large molecules (e.g., >100 atoms). In the present work, these limitations are overcome by a complete redesign of the LPNO-CCSD method. The new method is based on the combination of the concepts of PNOs and projected atomic orbitals (PAOs). Thus, each PNO is expanded in a set of PAOs that in turn belong to a given electron pair specific domain. In this way, it is possible to fully exploit locality while maintaining the extremely high compactness of the original LPNO-CCSD wavefunction. No terms are dropped from the CCSD equations and domains are chosen conservatively. The correlation energy loss due to the domains remains below <0.05%, which implies typically 15-20 but occasionally up to 30 atoms per domain on average. The new method has been given the acronym DLPNO-CCSD ("domain based LPNO-CCSD"). The method is nearly linear scaling with respect to system size. The original LPNO-CCSD method had three adjustable truncation thresholds that were chosen conservatively and do not need to be changed for actual applications. In the present treatment, no additional truncation parameters have been introduced. Any additional truncation is performed on the basis of the three original thresholds. There are no real-space cutoffs. Single excitations are truncated using singles-specific natural orbitals. Pairs are prescreened according to a multipole expansion of a pair correlation energy estimate based on local orbital specific virtual orbitals (LOSVs). Like its LPNO-CCSD predecessor, the method is completely of black box character and does not require any user adjustments. It is shown here that DLPNO-CCSD is as accurate as LPNO-CCSD while leading to computational savings exceeding one order of magnitude for larger systems. The largest calculations reported here featured >8800 basis functions and >450 atoms. In all larger test calculations done so far, the LPNO-CCSD step took less time than the preceding Hartree-Fock calculation, provided no approximations have been introduced in the latter. Thus, based on the present development reliable CCSD calculations on large molecules with unprecedented efficiency and accuracy are realized.

From the Orbital Implementation of the Kinetic Theory to the Polarization Propagator Method in the Study of Energy Deposition Problems

NASA Astrophysics Data System (ADS)

Cabrera-Trujillo, R.; Cruz, S. A.; Soullard, J.

The energy deposited by swift atomic-ion projectiles when colliding with a given target material has been a topic of special scientific interest for the last century due to the variety of applications of ion beams in modern materials technology as well as in medical physics. In this work, we summarize our contributions in this field as a consequence of fruitful discussions and enlightening ideas put forward by one of the main protagonists in stopping power theory during the last three decades: Jens Oddershede. Our review, mainly motivated by Jens' work, evolves from the extension of the orbital implementation of the kinetic theory of stopping through the orbital local plasma approximation, its use in studies of orbital and total mean excitation energies for the study of atomic and molecular stopping until the advances on generalized oscillator strength and sum rules in the study of stopping cross sections. Finally, as a tribute to Jens' work on the orbital implementation of the kinetic theory of stopping, in this work we present new results on the use of the Thomas-Fermi-Dirac-Weizsäcker density functional for the calculation of orbital and total atomic mean excitation energies. The results are applied to free-atoms and and extension is done to confined atoms - taking Si as an example - whereby target pressure effects on stopping are derived. Hence, evidence of the far-yield of Jens' ideas is given.

Density Functional Theory Study of Leaching Performance of Different Acids on Pyrochlore (100) Surface

NASA Astrophysics Data System (ADS)

Yang, Xiuli; Fang, Qing; Ouyang, Hui

2018-04-01

Pyrochlore leaching using hydrofluoric, sulfuric, and hydrochloric acids has been studied via experimental methods for years, but the interactions between niobium atoms on the pyrochlore surface and different acids have not been investigated. In this work, first-principles calculations based on density functional theory were used to elucidate the leaching performance of these three acids from the viewpoint of geometrical and electronic structures. The calculation results indicate that sulfate, chloride, and fluoride anions influence the geometric structure of pyrochlore (100) to different extents, decreasing in the order: sulfate, fluoride, chloride. Orbitals of O1 and O2 atoms of sulfate hybridized with those of surface niobium atom. Fluorine orbitals hybridized with those of surface niobium atoms. However, no obvious overlap exists between any orbitals of chlorine and surface niobium, revealing that chlorine does not interact chemically with surface niobium atoms.

Atomic selectivity in dissociative electron attachment to dihalobenzenes.

PubMed

Kim, Namdoo; Sohn, Taeil; Lee, Sang Hak; Nandi, Dhananjay; Kim, Seong Keun

2013-10-21

We investigated electron attachment to three dihalobenzene molecules, bromochlorobenzene (BCB), bromoiodobenzene (BIB) and chloroiodobenzene (CIB), by molecular beam photoelectron spectroscopy. The most prominent product of electron attachment in the anion mass spectra was the atomic fragment of the less electronegative halogen of the two, i.e., Br(-) for BCB and I(-) for BIB and CIB. Photoelectron spectroscopy and ab initio calculations suggested that the approaching electron prefers to attack the less electronegative atom, a seemingly counterintuitive finding but consistent with the mass spectrometric result. For the iodine-containing species BIB and CIB, the photoelectron spectrum consists of bands from both the molecular anion and atomic I(-), the latter of which is produced by photodissociation of the former. Molecular orbital analysis revealed that a large degree of orbital energy reordering takes place upon electron attachment. These phenomena were shown to be readily explained by simple molecular orbital theory and the electronegativity of the halogen atoms.

Density Functional Theory Study of Leaching Performance of Different Acids on Pyrochlore (100) Surface

NASA Astrophysics Data System (ADS)

Yang, Xiuli; Fang, Qing; Ouyang, Hui

2018-06-01

Pyrochlore leaching using hydrofluoric, sulfuric, and hydrochloric acids has been studied via experimental methods for years, but the interactions between niobium atoms on the pyrochlore surface and different acids have not been investigated. In this work, first-principles calculations based on density functional theory were used to elucidate the leaching performance of these three acids from the viewpoint of geometrical and electronic structures. The calculation results indicate that sulfate, chloride, and fluoride anions influence the geometric structure of pyrochlore (100) to different extents, decreasing in the order: sulfate, fluoride, chloride. Orbitals of O1 and O2 atoms of sulfate hybridized with those of surface niobium atom. Fluorine orbitals hybridized with those of surface niobium atoms. However, no obvious overlap exists between any orbitals of chlorine and surface niobium, revealing that chlorine does not interact chemically with surface niobium atoms.

Ab-initio atomic level stress and role of d-orbitals in CuZr, CuZn and CuY

NASA Astrophysics Data System (ADS)

Ojha, Madhusudan; Nicholson, Don M.; Egami, Takeshi

2015-03-01

Atomic level stress offers a new tool to characterize materials within the local approximation to density functional theory (DFT). Ab-initio atomic level stresses in B2 structures of CuZr, CuZn and CuY are calculated and results are explained on the basis of d-orbital contributions to Density of States (DOS). The overlap of d-orbital DOS plays an important role in the relative magnitude of atomic level stresses in these structures. The trends in atomic level stresses that we observed in these simple B2 structures are also seen in complex structures such as liquids, glasses and solid solutions. The stresses are however modified by the different coordination and relaxed separation distances in these complex structures. We used the Locally Self-Consistent Multiple Scattering (LSMS) code and Vienna Ab-initio Simulation Package (VASP) for ab-initio calculations.

Quantum theory of an atom in proximity to a superconductor

NASA Astrophysics Data System (ADS)

Le Dall, Matthias; Diniz, Igor; Dias da Silva, Luis G. G. V.; de Sousa, Rogério

2018-02-01

The impact of superconducting correlations on localized electronic states is important for a wide range of experiments in fundamental and applied superconductivity. This includes scanning tunneling microscopy of atomic impurities at the surface of superconductors, as well as superconducting-ion-chip spectroscopy of neutral ions and Rydberg states. Moreover, atomlike centers close to the surface are currently believed to be the main source of noise and decoherence in qubits based on superconducting devices. The proximity effect is known to dress atomic orbitals in Cooper-pair-like states known as Yu-Shiba-Rusinov (YSR) states, but the impact of superconductivity on the measured orbital splittings and optical-noise transitions is not known. Here we study the interplay between orbital degeneracy and particle-number admixture in atomic states, beyond the usual classical spin approximation. We model the atom as a generalized Anderson model interacting with a conventional s -wave superconductor. In the limit of zero on-site Coulomb repulsion (U =0 ), we obtain YSR subgap energy levels that are identical to the ones obtained from the classical spin model. When Δ is large and U >0 , the YSR spectra are no longer quasiparticle-like, and the highly degenerate orbital subspaces are split according to their spin, orbital, and number-parity symmetry. We show that U >0 activates additional poles in the atomic Green's function, suggesting an alternative explanation for the peak splittings recently observed in scanning tunneling microscopy of orbitally-degenerate impurities in superconductors. We describe optical excitation and absorption of photons by YSR states, showing that many additional optical channels open up in comparison to the nonsuperconducting case. Conversely, the additional dissipation channels imply increased electromagnetic noise due to impurities in superconducting devices.

Charge exchange cross sections in slow collisions of Si3+ with Hydrogen atom

NASA Astrophysics Data System (ADS)

Joseph, Dwayne; Quashie, Edwin; Saha, Bidhan

2011-05-01

In recent years both the experimental and theoretical studies of electron transfer in ion-atom collisions have progressed considerably. Accurate determination of the cross sections and an understanding of the dynamics of the electron-capture process by multiply charged ions from atomic hydrogen over a wide range of projectile velocities are important in various field ranging from fusion plasma to astrophysics. The soft X-ray emission from comets has been explained by charge transfer of solar wind ions, among them Si3+, with neutrals in the cometary gas vapor. The cross sections are evaluated using the (a) full quantum and (b) semi-classical molecular orbital close coupling (MOCC) methods. Adiabatic potentials and wave functions for relavent singlet and triplet states are generated using the MRDCI structure codes. Details will be presented at the conference. In recent years both the experimental and theoretical studies of electron transfer in ion-atom collisions have progressed considerably. Accurate determination of the cross sections and an understanding of the dynamics of the electron-capture process by multiply charged ions from atomic hydrogen over a wide range of projectile velocities are important in various field ranging from fusion plasma to astrophysics. The soft X-ray emission from comets has been explained by charge transfer of solar wind ions, among them Si3+, with neutrals in the cometary gas vapor. The cross sections are evaluated using the (a) full quantum and (b) semi-classical molecular orbital close coupling (MOCC) methods. Adiabatic potentials and wave functions for relavent singlet and triplet states are generated using the MRDCI structure codes. Details will be presented at the conference. Work supported by NSF CREST project (grant #0630370).

Roothaan-Hartree-Fock ground-state atomic wave functions: Slater-type orbital expansions and expectation values for Z = 2-54

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

Bunge, C.F.; Barrientos, J.A.; Bunge, A.V.

1993-01-01

Roothaan-Hartree-Fock orbitals expressed in a Slater-type basis are reported for the ground states of He through Xe. Energy accuracy ranges between 8 and 10 significant figures, reducing by between 21 and 2,770 times the energy errors of the previous such compilation (E. Clementi and C. Roetti, Atomic Data and Nuclear Data Tables 14, 177, 1974). For each atom, the total energy, kinetic energy, potential energy, virial ratio, electron density at the nucleus, and the Kato cusp are given together with radial expectation values [l angle]r[sup n][r angle] with n from [minus]3 to 2 for each orbital, orbital energies, and orbitalmore » expansion coefficients. 29 refs., 1 tab.« less

Space Shuttle Projects

NASA Image and Video Library

1984-04-01

The Long Duration Exposure Facility (LDEF) was designed by the Marshall Space Flight Center (MSFC) to test the performance of spacecraft materials, components, and systems that have been exposed to the environment of micrometeoroids and space debris for an extended period of time. The LDEF proved invaluable to the development of future spacecraft and the International Space Station (ISS). The LDEF carried 57 science and technology experiments, the work of more than 200 investigators. MSFC`s experiments included: Trapped Proton Energy Determination to determine protons trapped in the Earth's magnetic field and the impact of radiation particles; Linear Energy Transfer Spectrum Measurement Experiment which measures the linear energy transfer spectrum behind different shielding configurations; Atomic oxygen-Simulated Out-gassing, an experiment that exposes thermal control surfaces to atomic oxygen to measure the damaging out-gassed products; Thermal Control Surfaces Experiment to determine the effects of the near-Earth orbital environment and the shuttle induced environment on spacecraft thermal control surfaces; Transverse Flat-Plate Heat Pipe Experiment, to evaluate the zero-gravity performance of a number of transverse flat plate heat pipe modules and their ability to transport large quantities of heat; Solar Array Materials Passive LDEF Experiment to examine the effects of space on mechanical, electrical, and optical properties of lightweight solar array materials; and the Effects of Solar Radiation on Glasses. Launched aboard the Space Shuttle Orbiter Challenger's STS-41C mission April 6, 1984, the LDEF remained in orbit for five years until January 1990 when it was retrieved by the Space Shuttle Orbiter Columbia STS-32 mission and brought back to Earth for close examination and analysis.

About the atomic structures of icosahedral quasicrystals

NASA Astrophysics Data System (ADS)

Quiquandon, Marianne; Gratias, Denis

2014-01-01

This paper is a survey of the crystallographic methods that have been developed these last twenty five years to decipher the atomic structures of the icosahedral stable quasicrystals since their discovery in 1982 by D. Shechtman. After a brief recall of the notion of quasiperiodicity and the natural description of Z-modules in 3-dim as projection of regular lattices in N>3-dim spaces, we give the basic geometrical ingredients useful to describe icosahedral quasicrystals as irrational 3-dim cuts of ordinary crystals in 6-dim space. Atoms are described by atomic surfaces (ASs) that are bounded volumes in the internal (or perpendicular) 3-dim space and the intersections of which with the physical space are the actual atomic positions. The main part of the paper is devoted to finding the major properties of quasicrystalline icosahedral structures. As experimentally demonstrated, they can be described with a surprisingly few high symmetry ASs located at high symmetry special points in 6-dim space. The atomic structures are best described by aggregations and intersections of high symmetry compact interpenetrating atomic clusters. We show here that the experimentally relevant clusters are derived from one generic cluster made of two concentric triacontahedra scaled by τ and an external icosidodecahedron. Depending on which ones of the orbits of this cluster are eventually occupied by atoms, the actual atomic clusters are of type Bergman, Mackay, Tsai and others….

Gallium Compounds: A Possible Problem for the G2 Approaches

NASA Technical Reports Server (NTRS)

Bauschlicher, Charles W., Jr.; Melius, Carl F.; Allendorf, Mark D.; Arnold, James (Technical Monitor)

1998-01-01

The G2 atomization energies of fluorine and oxygen containing Ga compounds are greatly in error. This arises from an inversion of the Ga 3d core orbital and the F 2s or O 2s valence orbitals. Adding the Ga 3d orbital to the correlation treatment or removing the F 2s orbitals from the correlation treatment are shown to eliminate the problem. Removing the O 2s orbital from the correlation treatment reduces the error, but it can still be more than 6 kcal/mol. It is concluded that the experimental atomization energy of GaF2 is too large.

Koopmans' theorem in the Hartree-Fock method. General formulation

NASA Astrophysics Data System (ADS)

Plakhutin, Boris N.

2018-03-01

This work presents a general formulation of Koopmans' theorem (KT) in the Hartree-Fock (HF) method which is applicable to molecular and atomic systems with arbitrary orbital occupancies and total electronic spin including orbitally degenerate (OD) systems. The new formulation is based on the full set of variational conditions imposed upon the HF orbitals by the variational principle for the total energy and the conditions imposed by KT on the orbitals of an ionized electronic shell [B. N. Plakhutin and E. R. Davidson, J. Chem. Phys. 140, 014102 (2014)]. Based on these conditions, a general form of the restricted open-shell HF method is developed, whose eigenvalues (orbital energies) obey KT for the whole energy spectrum. Particular attention is paid to the treatment of OD systems, for which the new method gives a number of unexpected results. For example, the present method gives four different orbital energies for the triply degenerate atomic level 2p in the second row atoms B to F. Based on both KT conditions and a parallel treatment of atoms B to F within a limited configuration interaction approach, we prove that these four orbital energies, each of which is triply degenerate, are related via KT to the energies of different spin-dependent ionization and electron attachment processes (2p)N → (2p ) N ±1. A discussion is also presented of specific limitations of the validity of KT in the HF method which arise in OD systems. The practical applicability of the theory is verified by comparing KT estimates of the ionization potentials I2s and I2p for the second row open-shell atoms Li to F with the relevant experimental data.

Measurement of the Atomic Orbital Composition of the Near-Fermi-Level Electronic States in the Lanthanum Monopnictides LaBi and LaSb

NASA Astrophysics Data System (ADS)

Nummy, Thomas; Waugh, Justin; Parham, Stephen; Li, Haoxiang; Zhou, Xiaoqing; Plumb, Nick; Tafti, Fazel; Dessau, Daniel

Angle resolved photoemission spectroscopy (ARPES) is used to measure the electronic structure of the Extreme Magnetoresistance (XMR) topological semimetal candidates LaBi and LaSb. Using a wide range of photon energies the true bulk states are cleanly disentangled from the various types of surface states, which may exist due to surface projections of bulk states as well as for topological reasons. The orbital content of the near-EF states are extracted using varying photon polarizations. The measured bulk bands are somewhat lighter and are energy shifted compared to the results of Density Functional calculations, which is a minor effect in LaBi and a more serious effect in LaSb. This bulk band structure puts LaBi in the v = 1 class of Topological Insulators (or semimetals), consistent with the measured Dirac-like surface states. LaSb on the other hand is at the verge of a topological band inversion, with a less-clear case for any distinctly topological surface states. The low-dimensional cigar-shaped bulk Fermi surfaces for both compounds are separated out by orbital content, with a crossover from pnictide d orbitals to La p orbitals around the Fermi surface, which through strong spin-orbit coupling may be relevant for the Extreme Magnetoresistance. NSF GRFP.

ACES microwave link requirements.

PubMed

Uhrich, P M; Guillernot, P; Aubry, P; Gonzalez, F; Salomon, C

2000-01-01

Atomic Clock Ensemble in Space (ACES) is a project of the European Space Agency on-board the future International Space Station (ISS). The payload consists mainly of two atomic frequency standards, one space hydrogen maser (SHM) prepared by the Observatoire de Neuchatel (Switzerland), and one cold atom caesium clock called PHARAO prepared by the CNES (France), with the participation of the BNM-LPTF, the ENS-LKB, and the CNRS-LHA. Because of the anticipated performances of these clocks on-board the ISS, the requirements of the links between the payload and the clocks on the Earth are at the limits of the known potential of the optical or microwave techniques. The microwave link (MWL) requirements are described in this paper. Taking into account the characteristics of the ISS orbit, and fixing an arbitrary limit to the additional noise brought to the clock readings by the MWL, the computation of the required stability leads to two kinds of requirements: the first one at the subpicosecond level over each single continuous pass of the ISS above any Earth station, and the second one at the level of one part in 10(16) and below over a one day or more averaging period. Moreover, the ISS orbit parameters should lead to a knowledge of the ACES clock position at the m level, and of the ACES clock speed at the mm/s level.

Comments on the interaction of materials with atomic oxygen

NASA Technical Reports Server (NTRS)

Torre, Larry P.; Pippin, H. Gary

1987-01-01

An explanation of the relative resistance of various materials to attack by atomic oxygen is presented. Data from both ground based and on-orbit experiments is interpreted. The results indicate the importance of bond strengths, size and structure of pendant groups, and fluorination to the resistance of certain polymers to atomic oxygen. A theory which provides a partial explanation of the degradation of materials in low Earth orbit due to surface recombination of oxygen atoms is also included. Finally, a section commenting on mechanisms of material degradation is provided.

PARCS-Primary Atomic Reference Clock in Space

NASA Astrophysics Data System (ADS)

Ashby, Neil

2000-04-01

The purpose of the PARCS project is to place an advanced Cesium clock on the International Space Station (ISS). The project has been approved by NASA at the level of Science Concept Review. Groups at the National Institute of Standards and Technology, Jet Propulsion Laboratory, University of Colorado, and Harvard-Smithsonian Astrophysical Observatory, University of Torino are collaborating on clock design and construction. The microgravity space environment allows laser-cooled Cs atoms to spend longer times in the beam, resulting in improved clock performance. Clock stabilities of 3 × 10-14 at one second and accuracies of 1 × 10-16 are projected. With improved clock performance, significant improvements in several fundamental special and general relativity experiments are expected. For an ISS orbit at 400 km altitude and eccentricity 0.02, the gravitational frequency shift should be measureable about 35 times better than the previous best, Gravity Probe A. Improvements in testing Local Position Invariance and in a Kennedy-Thorndike experiment are expected. Areas of technology such as world-wide timing and time transfer and navigation will also directly benefit from such a high-performance clock in space. This paper will briefly describe the PARCS clock. The principal limitations on performance of relativity experiments, scientific objectives and benefits, and projected outcomes, will be discussed.

SparseMaps—A systematic infrastructure for reduced-scaling electronic structure methods. III. Linear-scaling multireference domain-based pair natural orbital N-electron valence perturbation theory

NASA Astrophysics Data System (ADS)

Guo, Yang; Sivalingam, Kantharuban; Valeev, Edward F.; Neese, Frank

2016-03-01

Multi-reference (MR) electronic structure methods, such as MR configuration interaction or MR perturbation theory, can provide reliable energies and properties for many molecular phenomena like bond breaking, excited states, transition states or magnetic properties of transition metal complexes and clusters. However, owing to their inherent complexity, most MR methods are still too computationally expensive for large systems. Therefore the development of more computationally attractive MR approaches is necessary to enable routine application for large-scale chemical systems. Among the state-of-the-art MR methods, second-order N-electron valence state perturbation theory (NEVPT2) is an efficient, size-consistent, and intruder-state-free method. However, there are still two important bottlenecks in practical applications of NEVPT2 to large systems: (a) the high computational cost of NEVPT2 for large molecules, even with moderate active spaces and (b) the prohibitive cost for treating large active spaces. In this work, we address problem (a) by developing a linear scaling "partially contracted" NEVPT2 method. This development uses the idea of domain-based local pair natural orbitals (DLPNOs) to form a highly efficient algorithm. As shown previously in the framework of single-reference methods, the DLPNO concept leads to an enormous reduction in computational effort while at the same time providing high accuracy (approaching 99.9% of the correlation energy), robustness, and black-box character. In the DLPNO approach, the virtual space is spanned by pair natural orbitals that are expanded in terms of projected atomic orbitals in large orbital domains, while the inactive space is spanned by localized orbitals. The active orbitals are left untouched. Our implementation features a highly efficient "electron pair prescreening" that skips the negligible inactive pairs. The surviving pairs are treated using the partially contracted NEVPT2 formalism. A detailed comparison between the partial and strong contraction schemes is made, with conclusions that discourage the strong contraction scheme as a basis for local correlation methods due to its non-invariance with respect to rotations in the inactive and external subspaces. A minimal set of conservatively chosen truncation thresholds controls the accuracy of the method. With the default thresholds, about 99.9% of the canonical partially contracted NEVPT2 correlation energy is recovered while the crossover of the computational cost with the already very efficient canonical method occurs reasonably early; in linear chain type compounds at a chain length of around 80 atoms. Calculations are reported for systems with more than 300 atoms and 5400 basis functions.

Interfacial charge-transfer transitions in a TiO2-benzenedithiol complex with Ti-S-C linkages.

PubMed

Fujisawa, Jun-ichi; Muroga, Ryuki; Hanaya, Minoru

2015-11-28

Interfacial charge-transfer (ICT) transitions between organic materials and inorganic semiconductors are a new mechanism for light absorption at organic-semiconductor interfaces. ICT transitions cause one-step interfacial charge separation without loss of energy. This feature is potentially useful to realize efficient organic-inorganic hybrid solar cells. ICT transitions have been examined by employing titanium dioxide (TiO2) nanoparticles chemisorbed with π-conjugated molecules via Ti-O-C linkages. Here, we report ICT transitions in a TiO2 and 1,2-benzenedithiol (BDT) complex with Ti-S-C linkages. BDT adsorbs on TiO2 by the bridging bidentate coordination of the sulfur atoms to surface titanium atoms. The TiO2-BDT complex shows ICT transitions from the BDT moiety to the conduction band of TiO2 in the visible region. The ICT transitions occur by orbital overlaps between the d orbitals of the surface titanium atoms and the π orbitals of the benzene ring. Our density-functional-theory (DFT) analysis reveals that the 3p valence orbitals of the sulfur bridging atoms contribute to more than 50% of the highest occupied molecular orbital (HOMO) and the 3d-3p(sulfur)-π interaction via the Ti-S-C linkage enhances the electronic mixing between the titanium atoms and the benzene moiety as compared to the 3d-2p(oxygen)-πvia the Ti-O-C linkage. This result indicates the important role of the heavier-atom linkers for strong organic-inorganic electronic couplings.

Ab initio calculation of hyperfine splitting constants of molecules

NASA Astrophysics Data System (ADS)

Ohta, K.; Nakatsuji, H.; Hirao, K.; Yonezawa, T.

1980-08-01

Hyperfine splitting (hfs) constants of molecules, methyl, ethyl, vinyl, allyl, cyclopropyl, formyl, O3-, NH2, NO2, and NF2 radicals have been calculated by the pseudo-orbital (PO) theory, the unrestricted HF (UHF), projected UHF (PUHF) and single excitation (SE) CI theories. The pseudo-orbital (PO) theory is based on the symmetry-adapted-cluster (SAC) expansion proposed previously. Several contractions of the Gaussian basis sets of double-zeta accuracy have been examined. The UHF results were consistently too large to compare with experiments and the PUHF results were too small. For molecules studied here, the PO theory and SECI theory gave relatively close results. They were in fair agreement with experiments. The first-order spin-polarization self-consistency effect, which was shown to be important for atoms, is relatively small for the molecules. The present result also shows an importance of eliminating orbital-transformation dependence from conventional first-order perturbation calculations. The present calculations have explained well several important variations in the experimental hfs constants.

Spacecraft Tests of General Relativity

NASA Technical Reports Server (NTRS)

Anderson, John D.

1997-01-01

Current spacecraft tests of general relativity depend on coherent radio tracking referred to atomic frequency standards at the ground stations. This paper addresses the possibility of improved tests using essentially the current system, but with the added possibility of a space-borne atomic clock. Outside of the obvious measurement of the gravitational frequency shift of the spacecraft clock, a successor to the suborbital flight of a Scout D rocket in 1976 (GP-A Project), other metric tests would benefit most directly by a possible improved sensitivity for the reduced coherent data. For purposes of illustration, two possible missions are discussed. The first is a highly eccentric Earth orbiter, and the second a solar-conjunction experiment to measure the Shapiro time delay using coherent Doppler data instead of the conventional ranging modulation.

Atomic orbital-based SOS-MP2 with tensor hypercontraction. I. GPU-based tensor construction and exploiting sparsity

NASA Astrophysics Data System (ADS)

Song, Chenchen; Martínez, Todd J.

2016-05-01

We present a tensor hypercontracted (THC) scaled opposite spin second order Møller-Plesset perturbation theory (SOS-MP2) method. By using THC, we reduce the formal scaling of SOS-MP2 with respect to molecular size from quartic to cubic. We achieve further efficiency by exploiting sparsity in the atomic orbitals and using graphical processing units (GPUs) to accelerate integral construction and matrix multiplication. The practical scaling of GPU-accelerated atomic orbital-based THC-SOS-MP2 calculations is found to be N2.6 for reference data sets of water clusters and alanine polypeptides containing up to 1600 basis functions. The errors in correlation energy with respect to density-fitting-SOS-MP2 are less than 0.5 kcal/mol for all systems tested (up to 162 atoms).

Atomic orbital-based SOS-MP2 with tensor hypercontraction. I. GPU-based tensor construction and exploiting sparsity.

PubMed

Song, Chenchen; Martínez, Todd J

2016-05-07

We present a tensor hypercontracted (THC) scaled opposite spin second order Møller-Plesset perturbation theory (SOS-MP2) method. By using THC, we reduce the formal scaling of SOS-MP2 with respect to molecular size from quartic to cubic. We achieve further efficiency by exploiting sparsity in the atomic orbitals and using graphical processing units (GPUs) to accelerate integral construction and matrix multiplication. The practical scaling of GPU-accelerated atomic orbital-based THC-SOS-MP2 calculations is found to be N(2.6) for reference data sets of water clusters and alanine polypeptides containing up to 1600 basis functions. The errors in correlation energy with respect to density-fitting-SOS-MP2 are less than 0.5 kcal/mol for all systems tested (up to 162 atoms).

Charge transfer in single and multiple scattering events at metal surfaces: a wavepacket study of the Na(+)/Cu(100) system.

PubMed

Sindona, A; Pisarra, M; Maletta, S; Riccardi, P; Falcone, G

2010-12-01

Resonant neutralization of hyperthermal energy Na(+) ions impinging on Cu(100) surfaces is studied, focusing on two specific collision events: one in which the projectile is reflected off the surface, the other in which the incident atom penetrates the outer surface layers initiating a series of scattering processes, within the target, and coming out together with a single surface atom. A semi-empirical model potential is adopted that embeds: (i) the electronic structure of the sample, (ii) the central field of the projectile, and (iii) the contribution of the Cu atom ejected in multiple scattering events. The evolution of the ionization orbital of the scattered atom is simulated, backwards in time, using a wavepacket propagation algorithm. The output of the approach is the neutralization probability, obtained by projecting the time-reversed valence wavefunction of the projectile onto the initially filled conduction band states. The results are in agreement with available data from the literature (Keller et al 1995 Phys. Rev. Lett. 75 1654) indicating that the motion of surface atoms, exiting the targets with kinetic energies of the order of a few electronvolts, plays a significant role in the final charge state of projectiles.

Super-elite plasma rings and the orbits of planets and satellites isomorphic to the orbits of electrons in the Bohr's model of the hydrogen atom

NASA Astrophysics Data System (ADS)

Rabinovich, B. I.

2007-10-01

This paper continues the series of papers [1 5] and generalizes the previous results to a proto-ring of magnetized plasma whose density decreases in the radial direction. The problem of quantization of the sector and orbital velocities, and of the radii and periods of revolution of elite plasma rings is considered. A new concept of super-elite rings is introduced. Their isomorphism with the orbits of the planets and planetary satellites in the Solar System is proved. This isomorphism also extends to the orbits of electrons in the Bohr’s model of the hydrogen atom.

Simulating Chiral Magnetic and Separation Effects with Spin-Orbit Coupled Atomic Gases

PubMed Central

Huang, Xu-Guang

2016-01-01

The chiral magnetic and chiral separation effects—quantum-anomaly-induced electric current and chiral current along an external magnetic field in parity-odd quark-gluon plasma—have received intense studies in the community of heavy-ion collision physics. We show that analogous effects occur in rotating trapped Fermi gases with Weyl-Zeeman spin-orbit coupling where the rotation plays the role of an external magnetic field. These effects can induce a mass quadrupole in the atomic cloud along the rotation axis which may be tested in future experiments. Our results suggest that the spin-orbit coupled atomic gases are potential simulators of the chiral magnetic and separation effects. PMID:26868084

Control of Wannier orbitals for generating tunable Ising interactions of ultracold atoms in an optical lattice

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

Inaba, Kensuke; Tamaki, Kiyoshi; Igeta, Kazuhiro

2014-12-04

In this study, we propose a method for generating cluster states of atoms in an optical lattice. By utilizing the quantum properties of Wannier orbitals, we create an tunable Ising interaction between atoms without inducing the spin-exchange interactions. We investigate the cause of errors that occur during entanglement generations, and then we propose an error-management scheme, which allows us to create high-fidelity cluster states in a short time.

Atomic-scale visualization of surface-assisted orbital order

PubMed Central

Kim, Howon; Yoshida, Yasuo; Lee, Chi-Cheng; Chang, Tay-Rong; Jeng, Horng-Tay; Lin, Hsin; Haga, Yoshinori; Fisk, Zachary; Hasegawa, Yukio

2017-01-01

Orbital-related physics attracts growing interest in condensed matter research, but direct real-space access of the orbital degree of freedom is challenging. We report a first, real-space, imaging of a surface-assisted orbital ordered structure on a cobalt-terminated surface of the well-studied heavy fermion compound CeCoIn5. Within small tip-sample distances, the cobalt atoms on a cleaved (001) surface take on dumbbell shapes alternatingly aligned in the [100] and [010] directions in scanning tunneling microscopy topographies. First-principles calculations reveal that this structure is a consequence of the staggered dxz-dyz orbital order triggered by enhanced on-site Coulomb interaction at the surface. This so far overlooked surface-assisted orbital ordering may prevail in transition metal oxides, heavy fermion superconductors, and other materials. PMID:28948229

Quantum-Classical Connection for Hydrogen Atom-Like Systems

ERIC Educational Resources Information Center

Syam, Debapriyo; Roy, Arup

2011-01-01

The Bohr-Sommerfeld quantum theory specifies the rules of quantization for circular and elliptical orbits for a one-electron hydrogen atom-like system. This article illustrates how a formula connecting the principal quantum number "n" and the length of the major axis of an elliptical orbit may be arrived at starting from the quantum…

INTERNATIONAL CONFERENCE ON SEMICONDUCTOR INJECTION LASERS SELCO-87: Method for calculation of electrical and optical properties of laser active media

NASA Astrophysics Data System (ADS)

Aleksandrov, D. G.; Filipov, F. I.

1988-11-01

A method is proposed for calculation of the electron band structure of multicomponent semiconductor solid solutions. Use is made of virtual atomic orbitals formed from real orbitals. The method represents essentially an approximation of a multicomponent solid solution by a binary one. The matrix elements of the Hamiltonian are obtained in the methods of linear combinations of atomic and bound orbitals. Some approximations used in these methods are described.

Intrinsic Magnetic Flux of the Electron's Orbital and Spin Motion

NASA Astrophysics Data System (ADS)

Wan, K. K.; Saglam, M.

2006-06-01

In analogy with the fact that there are magnetic moments associated respectively with the electron's orbital and spin motion in an atom we present several analyses on a proposal to introduce a concept of intrinsic magnetic flux associated with the electron's orbital and spin motion. It would be interesting to test or to demonstrate Faraday's and Lenz's laws of electromagnetic induction arising directly from the flux change due to transition of states in an atom and to examine applications of this concept of intrinsic flux.

Size Dependence of S-bonding on (111) Facets of Cu Nanoclusters

DOE PAGES

Boschen, Jeffery S.; Lee, Jiyoung; Windus, Theresa L.; ...

2016-04-21

We demonstrate a strong damped oscillatory size dependence of the adsorption energy for sulfur on the (111) facets of tetrahedral Cu nanoclusters up to sizes of ~300 atoms. This behavior reflects quantum size effects. Consistent results are obtained from density functional theory analyses utilizing either atomic orbital or plane-wave bases and using the same Perdew–Burke–Ernzerhof functional. Behavior is interpreted via molecular orbitals (MO), density of states (DOS), and crystal orbital Hamilton population (COHP) analyses.

The Deep Space Atomic Clock: Ushering in a New Paradigm for Radio Navigation and Science

NASA Technical Reports Server (NTRS)

Ely, Todd; Seubert, Jill; Prestage, John; Tjoelker, Robert

2013-01-01

The Deep Space Atomic Clock (DSAC) mission will demonstrate the on-orbit performance of a high-accuracy, high-stability miniaturized mercury ion atomic clock during a year-long experiment in Low Earth Orbit. DSAC's timing error requirement provides the frequency stability necessary to perform deep space navigation based solely on one-way radiometric tracking data. Compared to a two-way tracking paradigm, DSAC-enabled one-way tracking will benefit navigation and radio science by increasing the quantity and quality of tracking data. Additionally, DSAC also enables fully-autonomous onboard navigation useful for time-sensitive situations. The technology behind the mercury ion atomic clock and a DSAC mission overview are presented. Example deep space applications of DSAC, including navigation of a Mars orbiter and Europa flyby gravity science, highlight the benefits of DSAC-enabled one-way Doppler tracking.

Semiclassical quantization of Bohr orbits in the helium atom

NASA Astrophysics Data System (ADS)

Belov, V. V.; Maksimov, V. A.

2007-05-01

We use the complex WKB-Maslov method to construct the semiclassical spectral series corresponding to the resonance Bohr orbits in the helium atom. The semiclassical energy levels represented as the Rydberg tetra series correspond to the doubly symmetrically excited states of helium-like atoms. This level series contains the Rydberg triple series reported by Richter and Wintgen in 1991, which corresponds to the Z2+e-e- configuration of electrons observed by Eichmann and his collaborators in experiments on the laser excitation of the barium atom in 1992. The lower-level extrapolation of the formula obtained for the semiclassical spectrum gives the value of the ground state energy, which differs by 6% from the experimental value obtained by Bergeson and his collaborators in 1998. We also calculate the fine structure of the semiclassical spectrum due to the spin-orbit and spin-spin interactions of electrons.

Atomic orbital-based SOS-MP2 with tensor hypercontraction. I. GPU-based tensor construction and exploiting sparsity

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

Song, Chenchen; Martínez, Todd J.; SLAC National Accelerator Laboratory, Menlo Park, California 94025

We present a tensor hypercontracted (THC) scaled opposite spin second order Møller-Plesset perturbation theory (SOS-MP2) method. By using THC, we reduce the formal scaling of SOS-MP2 with respect to molecular size from quartic to cubic. We achieve further efficiency by exploiting sparsity in the atomic orbitals and using graphical processing units (GPUs) to accelerate integral construction and matrix multiplication. The practical scaling of GPU-accelerated atomic orbital-based THC-SOS-MP2 calculations is found to be N{sup 2.6} for reference data sets of water clusters and alanine polypeptides containing up to 1600 basis functions. The errors in correlation energy with respect to density-fitting-SOS-MP2 aremore » less than 0.5 kcal/mol for all systems tested (up to 162 atoms).« less

Materials selection for long life in low earth orbit - A critical evaluation of atomic oxygen testing with thermal atom systems

NASA Technical Reports Server (NTRS)

Koontz, S. L.; Albyn, K.; Leger, L.

1990-01-01

The use of thermal atom test methods as a materials selection and screening technique for low-earth orbit (LEO) spacecraft is critically evaluated. The chemistry and physics of thermal atom environments are compared with the LEO environment. The relative reactivities of a number of materials determined in thermal atom environments are compared with those observed in LEO and in high-quality LEO simulations. Reaction efficiencies (cu cm/atom) measured in a new type of thermal atom apparatus are one-thousandth to one ten-thousandth those observed in LEO, and many materials showing nearly identical reactivities in LEO show relative reactivities differing by as much as a factor of eight in thermal atom systems. A simple phenomenological kinetic model for the reaction of oxygen atoms with organic materials can be used to explain the differences in reactivity in different environments. Certain speciic thermal atom test environments can be used as reliable materials screening tools.

X-ray microprobe of orbital alignment in strong-field ionized atoms.

PubMed

Young, L; Arms, D A; Dufresne, E M; Dunford, R W; Ederer, D L; Höhr, C; Kanter, E P; Krässig, B; Landahl, E C; Peterson, E R; Rudati, J; Santra, R; Southworth, S H

2006-08-25

We have developed a synchrotron-based, time-resolved x-ray microprobe to investigate optical strong-field processes at intermediate intensities (10(14) - 10(15) W/cm2). This quantum-state specific probe has enabled the direct observation of orbital alignment in the residual ion produced by strong-field ionization of krypton atoms via resonant, polarized x-ray absorption. We found strong alignment to persist for a period long compared to the spin-orbit coupling time scale (6.2 fs). The observed degree of alignment can be explained by models that incorporate spin-orbit coupling. The methodology is applicable to a wide range of problems.

Diverse forms of bonding in two-dimensional Si allotropes: Nematic orbitals in the MoS2 structure

NASA Astrophysics Data System (ADS)

Gimbert, Florian; Lee, Chi-Cheng; Friedlein, Rainer; Fleurence, Antoine; Yamada-Takamura, Yukiko; Ozaki, Taisuke

2014-10-01

The interplay of sp2- and sp3-type bonding defines silicon allotropes in two- and three-dimensional forms. A two-dimensional phase bearing structural resemblance to a single MoS2 layer is found to possess a lower total energy than low-buckled silicene and to be stable in terms of its phonon dispersion relations. A set of cigar-shaped nematic orbitals originating from the Si sp2 orbitals realizes bonding with a sixfold coordination of the inner Si atoms of the layer. The identification of these nematic orbitals advocates diverse Si bonding configurations different from those of C atoms.

LETTER TO THE EDITOR: Quantum manifestations of closed orbits in the photoexcitation scaled spectrum of the hydrogen atom in crossed fields

NASA Astrophysics Data System (ADS)

Rao, Jianguo; Delande, D.; Taylor, K. T.

2001-06-01

The scaled photoexcitation spectrum of the hydrogen atom in crossed electric and magnetic fields has been obtained by means of accurate quantum mechanical calculation using a new algorithm. Closed orbits in the corresponding classical system have also been obtained, using a new, efficient and practical searching procedure. Two new classes of closed orbit have been identified. Fourier transforming each photoexcitation quantum spectrum to yield a plot against scaled action has allowed direct comparison between peaks in such plots and the scaled action values of closed orbits. Excellent agreement has been found with all peaks assigned.

Atomic Oxygen Fluence Monitor

NASA Technical Reports Server (NTRS)

Banks, Bruce A.

2011-01-01

This innovation enables a means for actively measuring atomic oxygen fluence (accumulated atoms of atomic oxygen per area) that has impinged upon spacecraft surfaces. Telemetered data from the device provides spacecraft designers, researchers, and mission managers with real-time measurement of atomic oxygen fluence, which is useful for prediction of the durability of spacecraft materials and components. The innovation is a compact fluence measuring device that allows in-space measurement and transmittance of measured atomic oxygen fluence as a function of time based on atomic oxygen erosion yields (the erosion yield of a material is the volume of material that is oxidized per incident oxygen atom) of materials that have been measured in low Earth orbit. It has a linear electrical response to atomic oxygen fluence, and is capable of measuring high atomic oxygen fluences (up to >10(exp 22) atoms/sq cm), which are representative of multi-year low-Earth orbital missions (such as the International Space Station). The durability or remaining structural lifetime of solar arrays that consist of polymer blankets on which the solar cells are attached can be predicted if one knows the atomic oxygen fluence that the solar array blanket has been exposed to. In addition, numerous organizations that launch space experiments into low-Earth orbit want to know the accumulated atomic oxygen fluence that their materials or components have been exposed to. The device is based on the erosion yield of pyrolytic graphite. It uses two 12deg inclined wedges of graphite that are over a grit-blasted fused silica window covering a photodiode. As the wedges erode, a greater area of solar illumination reaches the photodiode. A reference photodiode is also used that receives unobstructed solar illumination and is oriented in the same direction as the pyrolytic graphite covered photodiode. The short-circuit current from the photodiodes is measured and either sent to an onboard data logger, or transmitted to a receiving station on Earth. By comparison of the short-circuit currents from the fluence-measuring photodiode and the reference photodiode, one can compute the accumulated atomic oxygen fluence arriving in the direction that the fluence monitor is pointing. The device produces a signal that is linear with atomic oxygen fluence using a material whose atomic oxygen erosion yield has been measured over a period of several years in low-Earth orbit.

Ab initio relativistic effective potentials with spin--orbit operators. III. Rb through Xe

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

LaJohn, L.A.; Christiansen, P.A.; Ross, R.B.

A refined version of the ''shape consistent'' effective potential procedure of Christiansen, Lee, and Pitzer was used to compute averaged relativistic effective potentials (AREP) and spin--orbit operators for the elements Rb through Xe. Particular attention was given to the partitioning of the core and valence space and, where appropriate, more than one set of potentials is provided. These are tabulated in analytic form. Gaussian basis sets with contraction coefficients for the lowest energy state of each atom are given. The reliability of the transition metal AREPs was examined by comparing computed atomic excitation energies with accurate all-electron relativistic values. Themore » spin--orbit operators were tested in calculations on selected atoms.« less

Spatial Distribution of Io's Neutral Oxygen Cloud Observed by Hisaki

NASA Astrophysics Data System (ADS)

Koga, Ryoichi; Tsuchiya, Fuminori; Kagitani, Masato; Sakanoi, Takeshi; Yoneda, Mizuki; Yoshioka, Kazuo; Yoshikawa, Ichiro; Kimura, Tomoki; Murakami, Go; Yamazaki, Atsushi; Smith, H. Todd; Bagenal, Fran

2018-05-01

We report on the spatial distribution of a neutral oxygen cloud surrounding Jupiter's moon Io and along Io's orbit observed by the Hisaki satellite. Atomic oxygen and sulfur in Io's atmosphere escape from the exosphere mainly through atmospheric sputtering. Some of the neutral atoms escape from Io's gravitational sphere and form neutral clouds around Jupiter. The extreme ultraviolet spectrograph called EXCEED (Extreme Ultraviolet Spectroscope for Exospheric Dynamics) installed on the Japan Aerospace Exploration Agency's Hisaki satellite observed the Io plasma torus continuously in 2014-2015, and we derived the spatial distribution of atomic oxygen emissions at 130.4 nm. The results show that Io's oxygen cloud is composed of two regions, namely, a dense region near Io and a diffuse region with a longitudinally homogeneous distribution along Io's orbit. The dense region mainly extends on the leading side of Io and inside of Io's orbit. The emissions spread out to 7.6 Jupiter radii (RJ). Based on Hisaki observations, we estimated the radial distribution of the atomic oxygen number density and oxygen ion source rate. The peak atomic oxygen number density is 80 cm-3, which is spread 1.2 RJ in the north-south direction. We found more oxygen atoms inside Io's orbit than a previous study. We estimated the total oxygen ion source rate to be 410 kg/s, which is consistent with the value derived from a previous study that used a physical chemistry model based on Hisaki observations of ultraviolet emission ions in the Io plasma torus.

Durability Issues for the Protection of Materials from Atomic Oxygen Attack in Low Earth Orbit

NASA Astrophysics Data System (ADS)

Banks, B. A.; Lenczewski, M.; Demko, R.

2002-01-01

Low Earth orbital atomic oxygen is capable of eroding most polymeric materials typically used on spacecraft. Solar array blankets, thermal control polymers, and carbon fiber matrix composites are readily oxidized to become thinner and less capable of supporting the loads imposed upon them. Protective coatings have been developed that are or become durable to atomic oxygen to prevent oxidative erosion of the underlying polymers. However, the details of the chemistry, surface roughness and coating configuration can play a significant role as to whether or not the coating provides long duration atomic oxygen protection. Identical coatings on different surface roughness surfaces can produce drastically have drastically different durability results. Poor choice of protective coatings or self-protecting materials can also result in contamination of surrounding spacecraft surfaces. Such contamination can deposit on optical or thermal control surfaces resulting in changes in solar absorbtance, transmittance and reflectance of surfaces. Examples of successful and unsuccessful techniques used for atomic oxygen durability or protection will be presented based on actual results from low Earth orbital spacecraft. Investigations of the causes of undesired consequences or protective coating failures will be presented including ground laboratory experimental analysis as well as computational modeling. Atomic oxygen protective coating results from various low Earth orbital missions including the Long Duration Exposure Facility, the European Retrievable Carrier, Mir, and International Space Station will be presented to illustrate examples of protection successes as well as failures including analyses of the causes for the differences and proposed solutions.

SU(3) Orbital Kondo Effect with Ultracold Atoms

NASA Astrophysics Data System (ADS)

Nishida, Yusuke

2013-09-01

We propose a simple but novel scheme to realize the Kondo effect with ultracold atoms. Our system consists of a Fermi sea of spinless fermions interacting with an impurity atom of different species which is confined by an isotropic potential. The interspecies attraction can be tuned with an s-wave Feshbach resonance so that the impurity atom and a spinless fermion form a bound dimer that occupies a threefold-degenerate p orbital of the confinement potential. Many-body scatterings of this dimer and surrounding spinless fermions occur with exchanging their angular momenta and thus exhibit the SU(3) orbital Kondo effect. The associated Kondo temperature has a universal leading exponent given by TK∝exp⁡[-π/(3apkF3)] that depends only on an effective p-wave scattering volume ap and a Fermi wave vector kF. We also elucidate a Kondo singlet formation at zero temperature and an anisotropic interdimer interaction mediated by surrounding spinless fermions. The Kondo effect thus realized in ultracold atom experiments may be observed as an increasing atom loss by lowering the temperature or with radio-frequency spectroscopy. Our scheme and its extension to a dense Kondo lattice will be useful to develop new insights into yet unresolved aspects of Kondo physics.

Atomic oxygen effects on candidate coatings for long-term spacecraft in low earth orbit

NASA Technical Reports Server (NTRS)

Lan, E. H.; Smith, Charles A.; Cross, J. B.

1988-01-01

Candidate atomic oxygen protective coatings for long-term low Earth orbit (LEO) spacecraft were evaluated using the Los Alamos National Laboratory O-atom exposure facility. The coatings studied include Teflon, Al2O3, SiO2, and SWS-V-10, a silicon material. Preliminary results indicate that sputtered PTFE Teflon (0.1 micrometers) has a fluence lifetime of 10 to the 19th power O-atoms/cm (2), and sputtered silicon dioxide (0.1 micrometers), aluminum oxide (0.1 micrometers), and SWS-V-10, a silicone, (4 micrometers) have fluence lifetimes of 10 to the 20th power to 10 to the 21st power O-atoms/cm (2). There are large variations in fluence lifetime data for these coatings.

The Effect of Low Earth Orbit Atomic Oxygen Exposure on Phenylphosphine Oxide-Containing Polymers

NASA Technical Reports Server (NTRS)

Connell, John W.

2000-01-01

Thin films of phenylphosphine oxide-containing polymers were exposed to low Earth orbit aboard a space shuttle flight (STS-85) as part of flight experiment designated Evaluation of Space Environment and Effects on Materials (ESEM). This flight experiment was a cooperative effort between the NASA Langley Research Center (LaRC) and the National Space Development Agency of Japan (NASDA). The thin film samples described herein were part of an atomic oxygen exposure experiment (AOE) and were exposed to primarily atomic oxygen (1 X 1019 atoms/cm2). The thin film samples consisted of three phosphine oxide containing polymers (arylene ether, benzimidazole and imide). Based on post-flight analyses using atomic force microscopy, X-ray photoelectron spectroscopy, and weight loss data, it was found that atomic oxygen exposure of these materials efficiently produces a phosphate layer at the surface of the samples. This layer provides a barrier towards further attack by AO. Consequently, these materials do not exhibit linear erosion rates which is in contrast with most organic polymers. Qualitatively, the results obtained from these analyses compare favorably with those obtained from samples exposed to atomic oxygen and or oxygen plasma in ground based exposure experiments. The results of the low Earth orbit atomic oxygen exposure on these materials will be compared with those of ground based exposure to AO.

The Effects of Heteroatoms Si and S on Tuning the Optical Properties of Rhodamine- and Fluorescein-Based Fluorescence Probes: A Theoretical Analysis.

PubMed

Zhou, Panwang; Ning, Cai; Alsaedi, Ahmed; Han, Keli

2016-10-05

The effects of the incorporated heteroatoms Si and S on tuning the optical properties of rhodamine- and fluorescein-based fluorescence probes is investigated using DFT and time-dependent DFT with four different functionals. As previously proposed, the large redshift (90 nm) produced by a Si atom in both the absorption and emission spectra can be attributed to the σ*-π* conjugation between the σ* orbital of the Si atom and the π* orbital of the adjacent carbon atoms. However, the presence of a Si atom does not alter the fluorescence quenching mechanism of the nonfluorescent forms of the investigated compounds. For the first time, these theoretical results indicate that the n orbital of the S atom plays an important role in determining the optical properties of the nonfluorescent form of rhodamine-based fluorescence probes. It alters the fluorescence quenching mechanism by lowering the energy of the dark nπ* state, which is due to breakage of the C10-S52 bond upon photoexcitation. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

Li, Jingcheng; Wang, Yu; Li, Bin, E-mail: libin@mail.ustc.edu.cn, E-mail: bwang@ustc.edu.cn

We investigate the modification of electronic properties of single cobalt phthalocyanine (CoPc) molecule by an extra Co atom co-adsorbed on Au (111) surface using scanning tunneling microscopy (STM), joint with density functional theory (DFT) calculations. By manipulating CoPc molecules using the STM tip to contact individually adsorbed Co atom, two types of relatively stable complexes can be formed, denoted as CoPc-Co(I) and CoPc-Co(II). In CoPc-Co(I), the Co atom is at an intramolecular site close to aza-N atom of CoPc, which induces significant modifications of the electronic states of CoPc, such as energy shifts and splitting of nonlocal molecular orbitals. However,more » in CoPc-Co(II) where the Co atom is underneath a benzene lobe of CoPc, it only slightly modifies the electronic states of CoPc, and mainly local characteristics of specific molecular orbitals are affected, even though CoPc-Co(II) is more stable than CoPc-Co(I). Our DFT calculations give consistent results with the experiments, and related analyses based on the molecular orbital theory reveal mechanism behind the experimental observations.« less

Doughnut shape atom traps with arbitrary inclination

NASA Astrophysics Data System (ADS)

Masegosa, R. R. Y.; Moya-Cessa, H.; Chavez-Cerda, S.

2006-02-01

Since the invention of magneto-optical trap (MOT), there have been several experimental and theoretical studies of the density distribution in these devices. To the best of our knowledge, only horizontal orbital traps have been observed, perpendicular to the coil axis. In this work we report the observation of distributions of trapped atoms in pure circular orbits without a nucleus whose orbital plane is tilted up to 90 degrees with respect to the horizontal plane. We have used a stabilized time phase optical array in our experiments and conventional equipment used for MOT.

Comparison of theoretical and experimental values of the number of metallic orbitals per atom in hypoelectronic and hyperelectronic metals

PubMed Central

Pauling, Linus; Kamb, Barclay

1985-01-01

The statistical resonating-valence-bond theory of metals is applied in the purely theoretical calculation of the composition of the Ni-Cu alloy at the foot of the curve of saturation ferromagnetic moment, which marks the boundary between hypoelectronic and hyperelectronic metals and determines the value of the number of metallic orbitals per atom. The results, Ni44Cu56 and 0.722 metallic orbitals, agree with the observed values. This agreement provides strong support of the theory. PMID:16593633

Realization of localized Bohr-like wave packets.

PubMed

Mestayer, J J; Wyker, B; Lancaster, J C; Dunning, F B; Reinhold, C O; Yoshida, S; Burgdörfer, J

2008-06-20

We demonstrate a protocol to create localized wave packets in very-high-n Rydberg states which travel in nearly circular orbits around the nucleus. Although these wave packets slowly dephase and eventually lose their localization, their motion can be monitored over several orbital periods. These wave packets represent the closest analog yet achieved to the original Bohr model of the hydrogen atom, i.e., an electron in a circular classical orbit around the nucleus. The possible extension of the approach to create "planetary atoms" in highly correlated stable multiply excited states is discussed.

Pre-Service Science Teachers' Images and Misconceptions of Atomic Orbital and Self-Ionization Concepts

ERIC Educational Resources Information Center

Türk, Gülseda Eyceyurt; Tüzün, Ümmüye Nur

2018-01-01

The purpose of this study was to uncover pre-service science teachers' images and misconceptions regarding atomic orbital and self-ionization concepts. This study involved a total of 68 pre-service science teachers working at a public university during the 2015-2016 academic year. In this qualitative study, data were collated with the use of…

Is There a Need to Discuss Atomic Orbital Overlap When Teaching Hydrogen-Halide Bond Strength and Acidity Trends in Organic Chemistry?

ERIC Educational Resources Information Center

Devarajan, Deepa; Gustafson, Samantha J.; Bickelhaupt, F. Matthias; Ess, Daniel H.

2015-01-01

Undergraduate organic chemistry textbooks and Internet websites use a variety of approaches for presenting and explaining the impact of halogen atom size on trends in bond strengths and/or acidity of hydrogen halides. In particular, several textbooks and Internet websites explain these trends by invoking decreasing orbital overlap between the…

Translation and integration of numerical atomic orbitals in linear molecules

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

Heinäsmäki, Sami, E-mail: sami.heinasmaki@gmail.com

2014-02-14

We present algorithms for translation and integration of atomic orbitals for LCAO calculations in linear molecules. The method applies to arbitrary radial functions given on a numerical mesh. The algorithms are based on pseudospectral differentiation matrices in two dimensions and the corresponding two-dimensional Gaussian quadratures. As a result, multicenter overlap and Coulomb integrals can be evaluated effectively.

Reinventing atomic magnetic simulations with spin-orbit coupling

DOE PAGES

Perera, Meewanage Dilina N.; Eisenbach, Markus; Nicholson, Don M.; ...

2016-02-10

We propose a powerful extension to the combined molecular and spin dynamics method that fully captures the coupling between the atomic and spin subsystems via spin-orbit interactions. Moreover, the foundation of this method lies in the inclusion of the local magnetic anisotropies that arise as a consequence of the lattice symmetry breaking due to phonons or crystallographic defects. By using canonical simulations of bcc iron with the system coupled to a phonon heat bath, we show that our extension enables the previously unachievable angular momentum exchange between the atomic and spin degrees of freedom.

SparseMaps—A systematic infrastructure for reduced-scaling electronic structure methods. III. Linear-scaling multireference domain-based pair natural orbital N-electron valence perturbation theory

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

Guo, Yang; Sivalingam, Kantharuban; Neese, Frank, E-mail: Frank.Neese@cec.mpg.de

2016-03-07

Multi-reference (MR) electronic structure methods, such as MR configuration interaction or MR perturbation theory, can provide reliable energies and properties for many molecular phenomena like bond breaking, excited states, transition states or magnetic properties of transition metal complexes and clusters. However, owing to their inherent complexity, most MR methods are still too computationally expensive for large systems. Therefore the development of more computationally attractive MR approaches is necessary to enable routine application for large-scale chemical systems. Among the state-of-the-art MR methods, second-order N-electron valence state perturbation theory (NEVPT2) is an efficient, size-consistent, and intruder-state-free method. However, there are still twomore » important bottlenecks in practical applications of NEVPT2 to large systems: (a) the high computational cost of NEVPT2 for large molecules, even with moderate active spaces and (b) the prohibitive cost for treating large active spaces. In this work, we address problem (a) by developing a linear scaling “partially contracted” NEVPT2 method. This development uses the idea of domain-based local pair natural orbitals (DLPNOs) to form a highly efficient algorithm. As shown previously in the framework of single-reference methods, the DLPNO concept leads to an enormous reduction in computational effort while at the same time providing high accuracy (approaching 99.9% of the correlation energy), robustness, and black-box character. In the DLPNO approach, the virtual space is spanned by pair natural orbitals that are expanded in terms of projected atomic orbitals in large orbital domains, while the inactive space is spanned by localized orbitals. The active orbitals are left untouched. Our implementation features a highly efficient “electron pair prescreening” that skips the negligible inactive pairs. The surviving pairs are treated using the partially contracted NEVPT2 formalism. A detailed comparison between the partial and strong contraction schemes is made, with conclusions that discourage the strong contraction scheme as a basis for local correlation methods due to its non-invariance with respect to rotations in the inactive and external subspaces. A minimal set of conservatively chosen truncation thresholds controls the accuracy of the method. With the default thresholds, about 99.9% of the canonical partially contracted NEVPT2 correlation energy is recovered while the crossover of the computational cost with the already very efficient canonical method occurs reasonably early; in linear chain type compounds at a chain length of around 80 atoms. Calculations are reported for systems with more than 300 atoms and 5400 basis functions.« less

Spin-dependent electronic transport properties of transition metal atoms doped α-armchair graphyne nanoribbons

NASA Astrophysics Data System (ADS)

Fotoohi, Somayeh; Haji-Nasiri, Saeed

2018-04-01

Spin-dependent electronic transport properties of single 3d transition metal (TM) atoms doped α-armchair graphyne nanoribbons (α-AGyNR) are investigated by non-equilibrium Green's function (NEGF) method combined with density functional theory (DFT). It is found that all of the impurity atoms considered in this study (Fe, Co, Ni) prefer to occupy the sp-hybridized C atom site in α-AGyNR, and the obtained structures remain planar. The results show that highly localized impurity states are appeared around the Fermi level which correspond to the 3d orbitals of TM atoms, as can be derived from the projected density of states (PDOS). Moreover, Fe, Co, and Ni doped α-AGyNRs exhibit magnetic properties due to the strong spin splitting property of the energy levels. Also for each case, the calculated current-voltage characteristic per super-cell shows that the spin degeneracy in the system is obviously broken and the current becomes strongly spin dependent. Furthermore, a high spin-filtering effect around 90% is found under the certain bias voltages in Ni doped α-AGyNR. Additionally, the structure with Ni impurity reveals transfer characteristic that is suitable for designing a spin current switch. Our findings provide a high possibility to design the next generation spin nanodevices with novel functionalities.

Search for transient ultralight dark matter signatures with networks of precision measurement devices using a Bayesian statistics method

NASA Astrophysics Data System (ADS)

Roberts, B. M.; Blewitt, G.; Dailey, C.; Derevianko, A.

2018-04-01

We analyze the prospects of employing a distributed global network of precision measurement devices as a dark matter and exotic physics observatory. In particular, we consider the atomic clocks of the global positioning system (GPS), consisting of a constellation of 32 medium-Earth orbit satellites equipped with either Cs or Rb microwave clocks and a number of Earth-based receiver stations, some of which employ highly-stable H-maser atomic clocks. High-accuracy timing data is available for almost two decades. By analyzing the satellite and terrestrial atomic clock data, it is possible to search for transient signatures of exotic physics, such as "clumpy" dark matter and dark energy, effectively transforming the GPS constellation into a 50 000 km aperture sensor array. Here we characterize the noise of the GPS satellite atomic clocks, describe the search method based on Bayesian statistics, and test the method using simulated clock data. We present the projected discovery reach using our method, and demonstrate that it can surpass the existing constrains by several order of magnitude for certain models. Our method is not limited in scope to GPS or atomic clock networks, and can also be applied to other networks of precision measurement devices.

Covalent bonds are created by the drive of electron waves to lower their kinetic energy through expansion

PubMed Central

Schmidt, Michael W.; Ivanic, Joseph; Ruedenberg, Klaus

2014-01-01

An analysis based on the variation principle shows that in the molecules H2+, H2, B2, C2, N2, O2, F2, covalent bonding is driven by the attenuation of the kinetic energy that results from the delocalization of the electronic wave function. For molecular geometries around the equilibrium distance, two features of the wave function contribute to this delocalization: (i) Superposition of atomic orbitals extends the electronic wave function from one atom to two or more atoms; (ii) intra-atomic contraction of the atomic orbitals further increases the inter-atomic delocalization. The inter-atomic kinetic energy lowering that (perhaps counter-intuitively) is a consequence of the intra-atomic contractions drives these contractions (which per se would increase the energy). Since the contractions necessarily encompass both, the intra-atomic kinetic and potential energy changes (which add to a positive total), the fact that the intra-atomic potential energy change renders the total potential binding energy negative does not alter the fact that it is the kinetic delocalization energy that drives the bond formation. PMID:24880263

Covalent bonds are created by the drive of electron waves to lower their kinetic energy through expansion.

PubMed

Schmidt, Michael W; Ivanic, Joseph; Ruedenberg, Klaus

2014-05-28

An analysis based on the variation principle shows that in the molecules H2 (+), H2, B2, C2, N2, O2, F2, covalent bonding is driven by the attenuation of the kinetic energy that results from the delocalization of the electronic wave function. For molecular geometries around the equilibrium distance, two features of the wave function contribute to this delocalization: (i) Superposition of atomic orbitals extends the electronic wave function from one atom to two or more atoms; (ii) intra-atomic contraction of the atomic orbitals further increases the inter-atomic delocalization. The inter-atomic kinetic energy lowering that (perhaps counter-intuitively) is a consequence of the intra-atomic contractions drives these contractions (which per se would increase the energy). Since the contractions necessarily encompass both, the intra-atomic kinetic and potential energy changes (which add to a positive total), the fact that the intra-atomic potential energy change renders the total potential binding energy negative does not alter the fact that it is the kinetic delocalization energy that drives the bond formation.

Synthetic Spin-Orbit and Light Field Coupling in Ultra-cold Quantum Gases

NASA Astrophysics Data System (ADS)

Dong, Lin

Ultra-cold quantum gases subjected to light-induced synthetic gauge potentials have become an emergent field of theoretical and experimental studies. Because of the novel application of two-photon Raman transitions, ultra-cold neutral atoms behave like charged particles in magnetic field. The Raman coupling naturally gives rise to an effective spin-orbit interaction which couples the atoms center-of-mass motion to its selected pseudo-spin degrees of freedom. Combined with unprecedented controllability of interactions, geometry, disorder strength, spectroscopy, and high resolution measurement of momentum distribution, etc., we are truly in an exciting era of fulfilling and going beyond Richard Feynman's vision. of realizing quantum simulators to better understand the quantum mechanical nature of the universe, manifested immensely in the ultra-cold regimes. In this dissertation, we present a collection of theoretical progresses made by the doctoral candidate and his colleagues and collaborators. From the past few years of work, we mainly address three aspects of the synthetic spin-orbit and light field induced coupling in ultracold quantum gases: a) The ground-state physics of singleparticle system, two-body bound states, and many-body systems, all of which are subjected to spin-orbit coupling originated from synthetic gauge potentials; b) The symmetry breaking, topological phase transition and quench dynamics, which are conveniently offered by the realized experimental setup; c) The proposal and implications of light field induced dynamical spin-orbit coupling for atoms inside optical cavity. Our work represents an important advancement of theoretical understanding to the active research frontier of ultra-cold atom physics with spin-orbit coupling.

The NASA atomic oxygen effects test program

NASA Technical Reports Server (NTRS)

Banks, Bruce A.; Rutledge, Sharon K.; Brady, Joyce A.

1988-01-01

The NASA Atomic Oxygen Effects Test Program was established to compare the low earth orbital simulation characteristics of existing atomic oxygen test facilities and utilize the collective data from a multitude of simulation facilities to promote understanding of mechanisms and erosion yield dependence upon energy, flux, metastables, charge, and environmental species. Four materials chosen for this evaluation include Kapton HN polyimide, FEP Teflon, polyethylene, and graphite single crystals. The conditions and results of atomic oxygen exposure of these materials is reported by the participating organizations and then assembled to identify degrees of dependency of erosion yields that may not be observable from any single atomic oxygen low earth orbital simulation facility. To date, the program includes 30 test facilities. Characteristics of the participating test facilities and results to date are reported.

Low Earth orbital atomic oxygen micrometeoroid, and debris interactions with photovoltaic arrays

NASA Technical Reports Server (NTRS)

Banks, Bruce A.; Rutledge, Sharon K.; Degroh, Kim K.

1991-01-01

Polyimide Kapton solar array blankets can be protected from atomic oxygen in low earth orbit if SiO sub x thin film coatings are applied to their surfaces. The useful lifetime of a blanket protected in this manner strongly depends on the number and size of defects in the protective coatings. Atomic oxygen degradation is dominated by undercutting at defects in protective coatings caused by substrate roughness and processing rather than micrometeoroid or debris impacts. Recent findings from the Long Duration Exposure Facility (LDEF) and ground based studies show that interactions between atomic oxygen and silicones may cause grazing and contamination problems which may lead to solar array degradation.

No need for external orthogonality in subsystem density-functional theory.

PubMed

Unsleber, Jan P; Neugebauer, Johannes; Jacob, Christoph R

2016-08-03

Recent reports on the necessity of using externally orthogonal orbitals in subsystem density-functional theory (SDFT) [Annu. Rep. Comput. Chem., 8, 2012, 53; J. Phys. Chem. A, 118, 2014, 9182] are re-investigated. We show that in the basis-set limit, supermolecular Kohn-Sham-DFT (KS-DFT) densities can exactly be represented as a sum of subsystem densities, even if the subsystem orbitals are not externally orthogonal. This is illustrated using both an analytical example and in basis-set free numerical calculations for an atomic test case. We further show that even with finite basis sets, SDFT calculations using accurate reconstructed potentials can closely approach the supermolecular KS-DFT density, and that the deviations between SDFT and KS-DFT decrease as the basis-set limit is approached. Our results demonstrate that formally, there is no need to enforce external orthogonality in SDFT, even though this might be a useful strategy when developing projection-based DFT embedding schemes.

Space Shuttle Projects

NASA Image and Video Library

1984-04-07

This is an onboard photo of the deployment of the Long Duration Exposure Facility (LDEF) from the cargo bay of the Space Shuttle Orbiter Challenger STS-41C mission, April 7, 1984. After a five year stay in space, the LDEF was retrieved during the STS-32 mission by the Space Shuttle Orbiter Columbia in January 1990 and was returned to Earth for close examination and analysis. The LDEF was designed by the Marshall Space Flight Center (MSFC) to test the performance of spacecraft materials, components, and systems that have been exposed to the environment of micrometeoroids, space debris, radiation particles, atomic oxygen, and solar radiation for an extended period of time. Proving invaluable to the development of both future spacecraft and the International Space Station (ISS), the LDEF carried 57 science and technology experiments, the work of more than 200 investigators, 33 private companies, 21 universities, 7 NASA centers, 9 Department of Defense laboratories, and 8 forein countries.

Irregular wave functions of a hydrogen atom in a uniform magnetic field

NASA Technical Reports Server (NTRS)

Wintgen, D.; Hoenig, A.

1989-01-01

The highly excited irregular wave functions of a hydrogen atom in a uniform magnetic field are investigated analytically, with wave function scarring by periodic orbits considered quantitatively. The results obtained confirm that the contributions of closed classical orbits to the spatial wave functions vanish in the semiclassical limit. Their disappearance, however, is slow. This discussion is illustrated by numerical examples.

Visualization of a Large Set of Hydrogen Atomic Orbital Contours Using New and Expanded Sets of Parametric Equations

ERIC Educational Resources Information Center

Rhile, Ian J.

2014-01-01

Atomic orbitals are a theme throughout the undergraduate chemistry curriculum, and visualizing them has been a theme in this journal. Contour plots as isosurfaces or contour lines in a plane are the most familiar representations of the hydrogen wave functions. In these representations, a surface of a fixed value of the wave function ? is plotted…

Magnetic properties of Mg12O12 nanocage doped with transition metal atoms (Mn, Fe, Co and Ni): DFT study

NASA Astrophysics Data System (ADS)

Javan, Masoud Bezi

2015-07-01

Binding energy of the Mg12O12 nanocage doped with transition metals (TM=Mn, Fe, Co and Ni) in endohedrally, exohedrally and substitutionally forms were studied using density functional theory with the generalized gradient approximation exchange-correlation functional along 6 different paths inside and outside of the Mg12O12 nanocage. The most stable structures were determined with full geometry optimization near the minimum of the binding energy curves of all the examined paths inside and outside of the Mg12O12 nanocage. The results reveal that for all stable structures, the Ni atom has a larger binding energy than the other TM atoms. It is also found that for all complexes additional peaks contributed by TM-3d, 4s and 4p states appear in the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) gap of the host MgO cluster. The mid-gap states are mainly due to the hybridization between TM-3d, 4s and 4p orbitals and the cage π orbitals. The magnetic moment of the endohedrally doped TM atoms in the Mg12O12 are preserved to some extent due to the interaction between the TM and Mg12O12 nanocage, in contrast to the completely quenched magnetic moment of the Fe and Ni atoms in the Mg11(TM)O12 complexes. Furthermore, charge population analysis shows that charge transfer occurs from TM atom to the cage for endohedrally and substitutionally doping.

Optical angular momentum and atoms

PubMed Central

2017-01-01

Any coherent interaction of light and atoms needs to conserve energy, linear momentum and angular momentum. What happens to an atom’s angular momentum if it encounters light that carries orbital angular momentum (OAM)? This is a particularly intriguing question as the angular momentum of atoms is quantized, incorporating the intrinsic spin angular momentum of the individual electrons as well as the OAM associated with their spatial distribution. In addition, a mechanical angular momentum can arise from the rotation of the entire atom, which for very cold atoms is also quantized. Atoms therefore allow us to probe and access the quantum properties of light’s OAM, aiding our fundamental understanding of light–matter interactions, and moreover, allowing us to construct OAM-based applications, including quantum memories, frequency converters for shaped light and OAM-based sensors. This article is part of the themed issue ‘Optical orbital angular momentum’. PMID:28069766

Heavy ligand atom induced large magnetic anisotropy in Mn(ii) complexes.

PubMed

Chowdhury, Sabyasachi Roy; Mishra, Sabyashachi

2017-06-28

In the search for single molecule magnets, metal ions are considered pivotal towards achieving large magnetic anisotropy barriers. In this context, the influence of ligands with heavy elements, showing large spin-orbit coupling, on magnetic anisotropy barriers was investigated using a series of Mn(ii)-based complexes, in which the metal ion did not have any orbital contribution. The mixing of metal and ligand orbitals was achieved by explicitly correlating the metal and ligand valence electrons with CASSCF calculations. The CASSCF wave functions were further used for evaluating spin-orbit coupling and zero-field splitting parameters for these complexes. For Mn(ii) complexes with heavy ligand atoms, such as Br and I, several interesting inter-state mixings occur via the spin-orbit operator, which results in large magnetic anisotropy in these Mn(ii) complexes.

Quantum simulation. Spectroscopic observation of SU(N)-symmetric interactions in Sr orbital magnetism.

PubMed

Zhang, X; Bishof, M; Bromley, S L; Kraus, C V; Safronova, M S; Zoller, P; Rey, A M; Ye, J

2014-09-19

SU(N) symmetry can emerge in a quantum system with N single-particle spin states when spin is decoupled from interparticle interactions. Taking advantage of the high measurement precision offered by an ultrastable laser, we report a spectroscopic observation of SU(N ≤ 10) symmetry in (87)Sr. By encoding the electronic orbital degree of freedom in two clock states while keeping the system open to as many as 10 nuclear spin sublevels, we probed the non-equilibrium two-orbital SU(N) magnetism via Ramsey spectroscopy of atoms confined in an array of two-dimensional optical traps; we studied the spin-orbital quantum dynamics and determined the relevant interaction parameters. This study lays the groundwork for using alkaline-earth atoms as testbeds for important orbital models. Copyright © 2014, American Association for the Advancement of Science.

Elucidating Hyperconjugation from Electronegativity to Predict Drug Conformational Energy in a High Throughput Manner.

PubMed

Liu, Zhaomin; Pottel, Joshua; Shahamat, Moeed; Tomberg, Anna; Labute, Paul; Moitessier, Nicolas

2016-04-25

Computational chemists use structure-based drug design and molecular dynamics of drug/protein complexes which require an accurate description of the conformational space of drugs. Organic chemists use qualitative chemical principles such as the effect of electronegativity on hyperconjugation, the impact of steric clashes on stereochemical outcome of reactions, and the consequence of resonance on the shape of molecules to rationalize experimental observations. While computational chemists speak about electron densities and molecular orbitals, organic chemists speak about partial charges and localized molecular orbitals. Attempts to reconcile these two parallel approaches such as programs for natural bond orbitals and intrinsic atomic orbitals computing Lewis structures-like orbitals and reaction mechanism have appeared. In the past, we have shown that encoding and quantifying chemistry knowledge and qualitative principles can lead to predictive methods. In the same vein, we thought to understand the conformational behaviors of molecules and to encode this knowledge back into a molecular mechanics tool computing conformational potential energy and to develop an alternative to atom types and training of force fields on large sets of molecules. Herein, we describe a conceptually new approach to model torsion energies based on fundamental chemistry principles. To demonstrate our approach, torsional energy parameters were derived on-the-fly from atomic properties. When the torsional energy terms implemented in GAFF, Parm@Frosst, and MMFF94 were substituted by our method, the accuracy of these force fields to reproduce MP2-derived torsional energy profiles and their transferability to a variety of functional groups and drug fragments were overall improved. In addition, our method did not rely on atom types and consequently did not suffer from poor automated atom type assignments.

Molecular-orbital models for the catalytic activity and selectivity of coordinatively unsaturated platinum surfaces and complexes

NASA Astrophysics Data System (ADS)

Balazs, A. C.; Johnson, K. H.

1982-01-01

Electronic structures have been calculated for 5-, 6-, and 10-atom Pt clusters, as well as for a Pt(PH 3) 4 coordination complex, using the self-consistent-field X-alpha scattered-wave (SCF-Xα-SW) molecular-orbital technique. The 10-atom cluster models the local geometry of a flat, unreconstructed Pt(100) surface, while the 5- and 6-atom clusters show features of a stepped Pt surface. Pt(PH 3) 4 resembles the chemically similar homogeneous catalyst Pt(PPh 3) 4. Common to all these coordinatively unsaturated complexes are orbitals lying near or coinciding with the highest occupied molecular orbital ("Fermi level") which show pronounced d lobes pointing directly into the vacuum. Under the hypothesis that these molecular orbitals are mainly responsible for the chemical activities of the above species, one can account for the relative similarities and differences in catalytic activity and selectivity displayed by unreconstructed Pt(100) surfaces, stepped Pt surfaces or particles, and isolated Pt(PPh 3) 4 coordination complexes. The relevance of these findings to catalyst-support interactions is also discussed. Finally, relativistic corrections to the electronic structures are calculated and their implications on catalytic properties discussed.

Linear-scaling implementation of molecular response theory in self-consistent field electronic-structure theory.

PubMed

Coriani, Sonia; Høst, Stinne; Jansík, Branislav; Thøgersen, Lea; Olsen, Jeppe; Jørgensen, Poul; Reine, Simen; Pawłowski, Filip; Helgaker, Trygve; Sałek, Paweł

2007-04-21

A linear-scaling implementation of Hartree-Fock and Kohn-Sham self-consistent field theories for the calculation of frequency-dependent molecular response properties and excitation energies is presented, based on a nonredundant exponential parametrization of the one-electron density matrix in the atomic-orbital basis, avoiding the use of canonical orbitals. The response equations are solved iteratively, by an atomic-orbital subspace method equivalent to that of molecular-orbital theory. Important features of the subspace method are the use of paired trial vectors (to preserve the algebraic structure of the response equations), a nondiagonal preconditioner (for rapid convergence), and the generation of good initial guesses (for robust solution). As a result, the performance of the iterative method is the same as in canonical molecular-orbital theory, with five to ten iterations needed for convergence. As in traditional direct Hartree-Fock and Kohn-Sham theories, the calculations are dominated by the construction of the effective Fock/Kohn-Sham matrix, once in each iteration. Linear complexity is achieved by using sparse-matrix algebra, as illustrated in calculations of excitation energies and frequency-dependent polarizabilities of polyalanine peptides containing up to 1400 atoms.

Force on an electric/magnetic dipole and classical approach to spin-orbit coupling in hydrogen-like atoms

NASA Astrophysics Data System (ADS)

Kholmetskii, A. L.; Missevitch, O. V.; Yarman, T.

2017-09-01

We carry out the classical analysis of spin-orbit coupling in hydrogen-like atoms, using the modern expressions for the force and energy of an electric/magnetic dipole in an electromagnetic field. We disclose a novel physical meaning of this effect and show that for a laboratory observer the energy of spin-orbit interaction is represented solely by the mechanical energy of the spinning electron (considered as a gyroscope) due to the Thomas precession of its spin. Concurrently we disclose some errors in the old and new publications on this subject.

Effects on optical systems from interactions with oxygen atoms in low earth orbits

NASA Technical Reports Server (NTRS)

Peters, P. N.; Swann, J. T.; Gregory, J. C.

1986-01-01

Modifications of material surface properties due to interactions with ambient atomic oxygen have been observed on surfaces facing the orbital direction in low earth orbits. Some effects are very damaging to surface optical properties while some are more subtle and even beneficial. Most combustible materials are heavily etched, and some coatings, such as silver and osmium, are seriously degraded or removed as volatile oxides. The growth of oxide films on metals and semiconductors considered stable in dry air was measured. Material removal, surface roughness, reflectance, and optical densities are reported. Effects of temperature, contamination, and overcoatings are noted.

Effects on optical systems from interactions with oxygen atoms in low earth orbits

NASA Astrophysics Data System (ADS)

Peters, P. N.; Swann, J. T.; Gregory, J. C.

1986-04-01

Modifications of material surface properties due to interactions with ambient atomic oxygen have been observed on surfaces facing the orbital direction in low earth orbits. Some effects are very damaging to surface optical properties while some are more subtle and even beneficial. Most combustible materials are heavily etched, and some coatings, such as silver and osmium, are seriously degraded or removed as volatile oxides. The growth of oxide films on metals and semiconductors considered stable in dry air was measured. Material removal, surface roughness, reflectance, and optical densities are reported. Effects of temperature, contamination, and overcoatings are noted.

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

Ball, J.B. Jr.

Direct oblique sagittal CT was used to evaluate trauma to 77 orbits. Sixty-seven orbital wall fractures with intact orbital rims (36 floor, 22 medial wall, nine roof) were identified in 47 orbits. Since persistent diplopia and/or enophthalmos may warrant surgical repair of orbital floor fractures, optimal imaging should include an evaluation of extraocular muscle status, the nature and amount of displaced orbital contents, and an accurate definition of fracture margins. For orbital floor fractures, a combination of the direct oblique sagittal and direct coronal projections optimally displayed all fracture margins, the fracture's relationship to the inferior orbital rim and medialmore » orbital wall, and the amount of displacement into the maxillary sinus. Inferior rectus muscle status with 36 floor fractures was best seen on the direct oblique sagittal projection in 30 fractures (83.3%) and was equally well seen on sagittal and coronal projections in two fractures (5.5%). Floor fractures were missed on 100% of axial, 5.5% of sagittal, and 0% of coronal projections. Since the direct oblique sagittal projection complements the direct coronal projection in evaluating orbital floor fractures, it should not be performed alone. A technical approach to the CT evaluation or orbital wall fractures is presented.« less

Spatial assignment of symmetry adapted perturbation theory interaction energy components: The atomic SAPT partition

NASA Astrophysics Data System (ADS)

Parrish, Robert M.; Sherrill, C. David

2014-07-01

We develop a physically-motivated assignment of symmetry adapted perturbation theory for intermolecular interactions (SAPT) into atom-pairwise contributions (the A-SAPT partition). The basic precept of A-SAPT is that the many-body interaction energy components are computed normally under the formalism of SAPT, following which a spatially-localized two-body quasiparticle interaction is extracted from the many-body interaction terms. For electrostatics and induction source terms, the relevant quasiparticles are atoms, which are obtained in this work through the iterative stockholder analysis (ISA) procedure. For the exchange, induction response, and dispersion terms, the relevant quasiparticles are local occupied orbitals, which are obtained in this work through the Pipek-Mezey procedure. The local orbital atomic charges obtained from ISA additionally allow the terms involving local orbitals to be assigned in an atom-pairwise manner. Further summation over the atoms of one or the other monomer allows for a chemically intuitive visualization of the contribution of each atom and interaction component to the overall noncovalent interaction strength. Herein, we present the intuitive development and mathematical form for A-SAPT applied in the SAPT0 approximation (the A-SAPT0 partition). We also provide an efficient series of algorithms for the computation of the A-SAPT0 partition with essentially the same computational cost as the corresponding SAPT0 decomposition. We probe the sensitivity of the A-SAPT0 partition to the ISA grid and convergence parameter, orbital localization metric, and induction coupling treatment, and recommend a set of practical choices which closes the definition of the A-SAPT0 partition. We demonstrate the utility and computational tractability of the A-SAPT0 partition in the context of side-on cation-π interactions and the intercalation of DNA by proflavine. A-SAPT0 clearly shows the key processes in these complicated noncovalent interactions, in systems with up to 220 atoms and 2845 basis functions.

Spatial assignment of symmetry adapted perturbation theory interaction energy components: The atomic SAPT partition

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

Parrish, Robert M.; Sherrill, C. David, E-mail: sherrill@gatech.edu

2014-07-28

We develop a physically-motivated assignment of symmetry adapted perturbation theory for intermolecular interactions (SAPT) into atom-pairwise contributions (the A-SAPT partition). The basic precept of A-SAPT is that the many-body interaction energy components are computed normally under the formalism of SAPT, following which a spatially-localized two-body quasiparticle interaction is extracted from the many-body interaction terms. For electrostatics and induction source terms, the relevant quasiparticles are atoms, which are obtained in this work through the iterative stockholder analysis (ISA) procedure. For the exchange, induction response, and dispersion terms, the relevant quasiparticles are local occupied orbitals, which are obtained in this work throughmore » the Pipek-Mezey procedure. The local orbital atomic charges obtained from ISA additionally allow the terms involving local orbitals to be assigned in an atom-pairwise manner. Further summation over the atoms of one or the other monomer allows for a chemically intuitive visualization of the contribution of each atom and interaction component to the overall noncovalent interaction strength. Herein, we present the intuitive development and mathematical form for A-SAPT applied in the SAPT0 approximation (the A-SAPT0 partition). We also provide an efficient series of algorithms for the computation of the A-SAPT0 partition with essentially the same computational cost as the corresponding SAPT0 decomposition. We probe the sensitivity of the A-SAPT0 partition to the ISA grid and convergence parameter, orbital localization metric, and induction coupling treatment, and recommend a set of practical choices which closes the definition of the A-SAPT0 partition. We demonstrate the utility and computational tractability of the A-SAPT0 partition in the context of side-on cation-π interactions and the intercalation of DNA by proflavine. A-SAPT0 clearly shows the key processes in these complicated noncovalent interactions, in systems with up to 220 atoms and 2845 basis functions.« less

Natural chemical shielding analysis of nuclear magnetic resonance shielding tensors from gauge-including atomic orbital calculations

NASA Astrophysics Data System (ADS)

Bohmann, Jonathan A.; Weinhold, Frank; Farrar, Thomas C.

1997-07-01

Nuclear magnetic shielding tensors computed by the gauge including atomic orbital (GIAO) method in the Hartree-Fock self-consistent-field (HF-SCF) framework are partitioned into magnetic contributions from chemical bonds and lone pairs by means of natural chemical shielding (NCS) analysis, an extension of natural bond orbital (NBO) analysis. NCS analysis complements the description provided by alternative localized orbital methods by directly calculating chemical shieldings due to delocalized features in the electronic structure, such as bond conjugation and hyperconjugation. Examples of NCS tensor decomposition are reported for CH4, CO, and H2CO, for which a graphical mnemonic due to Cornwell is used to illustrate the effect of hyperconjugative delocalization on the carbon shielding.

Issues and Effects of Atomic Oxygen Interactions With Silicone Contamination on Spacecraft in Low Earth Orbit

NASA Technical Reports Server (NTRS)

Banks, Bruce; Rutledge, Sharon; Sechkar, Edward; Stueber, Thomas; Snyder, Aaron; deGroh, Kim; Haytas, Christy; Brinker, David

2000-01-01

The continued presence and use of silicones on spacecraft in low Earth orbit (LEO) has been found to cause the deposition of contaminant films on surfaces which are also exposed to atomic oxygen. The composition and optical properties of the resulting SiO(x)- based (where x is near 2) contaminant films may be dependent upon the relative rates of arrival of atomic oxygen, silicone contaminant and hydrocarbons. This paper presents results of in-space silicone contamination tests, ground laboratory simulation tests and analytical modeling to identify controlling processes that affect contaminant characteristics.

The Colorado Ultraviolet Transit Experiment (CUTE): a dedicated cubesat mission for the study of exoplanetary mass loss and magnetic fields

NASA Astrophysics Data System (ADS)

Fleming, Brian T.; France, Kevin; Nell, Nicholas; Kohnert, Richard; Pool, Kelsey; Egan, Arika; Fossati, Luca; Koskinen, Tommi; Vidotto, Aline A.; Hoadley, Keri; Desert, Jean-Michel; Beasley, Matthew; Petit, Pascal

2017-08-01

The Colorado Ultraviolet Transit Experiment (CUTE) is a near-UV (2550 - 3300 Å) 6U cubesat mission designed to monitor transiting hot Jupiters to quantify their atmospheric mass loss and magnetic fields. CUTE will probe both atomic (Mg and Fe) and molecular (OH) lines for evidence of enhanced transit absorption, and to search for evidence of early ingress due to bow shocks ahead of the planet's orbital motion. As a dedicated mission, CUTE will observe > 60 spectroscopic transits of hot Jupiters over a nominal seven month mission. This represents the equivalent of > 700 orbits of the only other instrument capable of these measurements, the Hubble Space Telescope. CUTE efficiently utilizes the available cubesat volume by means of an innovative optical design to achieve a projected effective area of ˜ 22 cm2 , low instrumental background, and a spectral resolving power of R ˜ 3000 over the entire science bandpass. These performance characteristics enable CUTE to discern a transit depth of < 1% in individual spectral absorption lines. We present the CUTE optical and mechanical design, a summary of the science motivation and expected results, and an overview of the projected fabrication, calibration and launch timeline.

Recurrence spectra of a helium atom in parallel electric and magnetic fields

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

Wang, Dehua; Department of Mathematics and Physics, Shandong Architecture and Engineering Institute, Jinan 250014, People's Republic of China; Ding, Shiliang

2003-08-01

A model potential for the general Rydberg atom is put forward, which includes not only the Coulomb interaction potential and the core-attractive potential, but also the exchange potential between the excited electron and other electrons. Using the region-splitting consistent and iterative method, we calculated the scaled recurrence spectra of the helium atom in parallel electric and magnetic fields and the closed orbits in the corresponding classical system have also been obtained. In order to remove the Coulomb singularity of the classical motion of Hamiltonian, we implement the Kustaanheimo-Stiefel transformation, which transforms the system from a three-dimensional to a four-dimensional one.more » The Fourier-transformed spectra of the helium atom has allowed direct comparison between peaks in such a plot and the scaled action values of closed orbits. Considering the exchange potential, the number of the closed orbits increased, which led to more peaks in the recurrence spectra. The results are compared with those of the hydrogen case, which shows that the core-scattered effects and the electron exchange potential play an important role in the multielectron Rydberg atom.« less

Transfer of Orbital and Spin angular momentum from non-paraxial optical vortex to atomic BEC

NASA Astrophysics Data System (ADS)

Bhowmik, Anal; Mondal, Pradip Kumar; Majumder, Sonjoy; Deb, Bimalendu

2017-04-01

Allen and co-workers first brought up the realization that optical vortex can carry well defined orbital angular momentum (OAM) associated with its spatial mode. Spin angular momentum (SAM) of the light, associated with the polarization, interacts with the internal electronic motion of the atom. The exchange of orbital angular momentum (OAM) between optical vortex and the center-of-mass (CM) motion of an atom or molecule is well known in paraxial approximation. We show that, how the total angular momentum (TAM) of non-paraxial optical vortex is shared with atom, in terms of OAM and SAM. Both the angular momenta are now possible to be transferred to the internal electronic and external CM motion of atom. Here we have studied how the Rabi frequencies of the excitations of two-photon Raman transitions with respect to focusing angles. Also, we investigate the properties of the vortex superposed state for a Bose-Einstein condensate condensate by a single non-paraxial vortex beam. The density distribution of the vortex-antivortex superposed state has a petal structure which is determined by the quantum circulations and proportion of the vortex and antivortex.

Mechanical, electronic, and thermodynamic properties of zirconium carbide from first-principles calculations

NASA Astrophysics Data System (ADS)

Yang, Xiao-Yong; Lu, Yong; Zheng, Fa-Wei; Zhang, Ping

2015-11-01

Mechanical, electronic, and thermodynamic properties of zirconium carbide have been systematically studied using the ab initio calculations. The calculated equilibrium lattice parameter, bulk modulus, and elastic constants are all well consistent with the experimental data. The electronic band structure indicates that the mixture of C 2p and Zr 4d and 4p orbitals around the Fermi level makes a large covalent contribution to the chemical bonds between the C and Zr atoms. The Bader charge analysis suggests that there are about 1.71 electrons transferred from each Zr atom to its nearest C atom. Therefore, the Zr-C bond displays a mixed ionic/covalent character. The calculated phonon dispersions of ZrC are stable, coinciding with the experimental measurement. A drastic expansion in the volume of ZrC is seen with increasing temperature, while the bulk modulus decreases linearly. Based on the calculated phonon dispersion curves and within the quasi-harmonic approximation, the temperature dependence of the heat capacities is obtained, which gives a good description compared with the available experimental data. Project supported by the National Natural Science Foundation of China (Grant No. 51071032).

Illustrating Concepts in Physical Organic Chemistry with 3D Printed Orbitals

ERIC Educational Resources Information Center

Robertson, Michael J.; Jorgensen, William L.

2015-01-01

Orbital theory provides a powerful tool for rationalizing and understanding many phenomena in chemistry. In most introductory chemistry courses, students are introduced to atomic and molecular orbitals in the form of two-dimensional drawings. In this work, we describe a general method for producing 3D printing files of orbital models that can be…

Exospheric perturbations by radiation pressure. II - Solution for orbits in the ecliptic plane

NASA Technical Reports Server (NTRS)

Chamberlain, J. W.

1980-01-01

A previous study (Chamberlain, 1979) gave solutions for the mean time rates of change of orbital elements of satellite atoms in an exosphere influenced by solar radiation pressure; each element was assumed to behave independently. In the present paper, the instantaneous rates of changes for three elements (e, Omega, and phi = omega + Omega) are integrated simultaneously for the case of the inclination i = 0. The results confirm the validity of using mean rates when the orbits are tighly bound to the planet, and serve as examples to be reproduced by the complicated numerical solutions required for arbitrary inclination. Strongly bound hydrogen atoms perturbed in earth orbit by radiation pressure do not seem a likely cause of the geotail extending in the anti-sun direction. Instead, radiation pressure will cause those particles' orbits to form a broad fan-shaped tail and to deteriorate into the earth's atmosphere.

A Comparison of Atomic Oxygen Degradation in Low Earth Orbit and in a Plasma Etcher

NASA Technical Reports Server (NTRS)

Townsend, Jacqueline A.; Park, Gloria

1997-01-01

In low Earth orbit (LEO) significant degradation of certain materials occurs from exposure to atomic oxygen (AO). Orbital opportunities to study this degradation for specific materials are limited and expensive. While plasma etchers are commonly used in ground-based studies because of their low cost and convenience, the environment produced in an etcher chamber differs greatly from the LEO environment. Because of the differences in environment, the validity of using etcher data has remained an open question. In this paper, degradation data for 22 materials from the orbital experiment Evaluation of Oxygen Interaction with Materials (EOIM-3) are compared with data from EOIM-3 control specimens exposed in a typical plasma etcher. This comparison indicates that, when carefully considered, plasma etcher results can produce order-of-magnitude estimates of orbital degradation. This allows the etcher to be used to screen unacceptable materials from further, more expensive tests.

Orbital Magnetization of Quantum Spin Hall Insulator Nanoparticles.

PubMed

Potasz, P; Fernández-Rossier, J

2015-09-09

Both spin and orbital degrees of freedom contribute to the magnetic moment of isolated atoms. However, when inserted in crystals, atomic orbital moments are quenched because of the lack of rotational symmetry that protects them when isolated. Thus, the dominant contribution to the magnetization of magnetic materials comes from electronic spin. Here we show that nanoislands of quantum spin Hall insulators can host robust orbital edge magnetism whenever their highest occupied Kramers doublet is singly occupied, upgrading the spin edge current into a charge current. The resulting orbital magnetization scales linearly with size, outweighing the spin contribution for islands of a few nm in size. This linear scaling is specific of the Dirac edge states and very different from Schrodinger electrons in quantum rings. By modeling Bi(111) flakes, whose edge states have been recently observed, we show that orbital magnetization is robust with respect to disorder, thermal agitation, shape of the island, and crystallographic direction of the edges, reflecting its topological protection.

Effects of strong laser fields on hadronic helium atoms

NASA Astrophysics Data System (ADS)

Lee, Han-Chieh; Jiang, Tsin-Fu

2015-12-01

The metastable hadronic helium atoms in microseconds lifetime are available in laboratory, and two-photon spectroscopy was reported recently. This exotic helium atom has an electron in the ground state and a negative hadron rotating around the helium nucleus. We theoretically study the excitation on hadronic helium by femtosecond pulse and elucidate the influence of moleculelike structure and rotation behavior on the photoelectron spectra and high-order harmonic generation. Because of the moleculelike structure, the electronic ground state consists of several angular orbitals. These angular orbitals can enhance photoelectron spectra at high energies, and also influence the harmonic generation spectra considerably. In particular, the harmonic spectra can occur at even harmonic orders because of the transition between these angular orbitals and continuum states. On the other side, the rotation behavior of hadron can induce a frequency shift in the harmonic spectra. The magnitude of the frequency shift depends on the orbiting speed of the hadron, which is considerable because the rotation period is in a few femtoseconds, a time scale that is comparable to that of infrared laser and is feasible in current laser experiments.

Multireference quantum chemistry through a joint density matrix renormalization group and canonical transformation theory.

PubMed

Yanai, Takeshi; Kurashige, Yuki; Neuscamman, Eric; Chan, Garnet Kin-Lic

2010-01-14

We describe the joint application of the density matrix renormalization group and canonical transformation theory to multireference quantum chemistry. The density matrix renormalization group provides the ability to describe static correlation in large active spaces, while the canonical transformation theory provides a high-order description of the dynamic correlation effects. We demonstrate the joint theory in two benchmark systems designed to test the dynamic and static correlation capabilities of the methods, namely, (i) total correlation energies in long polyenes and (ii) the isomerization curve of the [Cu(2)O(2)](2+) core. The largest complete active spaces and atomic orbital basis sets treated by the joint DMRG-CT theory in these systems correspond to a (24e,24o) active space and 268 atomic orbitals in the polyenes and a (28e,32o) active space and 278 atomic orbitals in [Cu(2)O(2)](2+).

Halogen atom effect on the photophysical properties of substituted aza-BODIPY derivatives.

PubMed

De Simone, B C; Mazzone, G; Pirillo, J; Russo, N; Sicilia, E

2017-01-18

The influence of halogen atom substitution (Br and I), in different amounts and positions in an aza-BODIPY skeleton, on the photophysical properties of some aza-BODIPY derivatives has been investigated by using density functional theory and its time-dependent extension. The heavy atom effect on excitation energies, singlet-triplet energy gaps and spin-orbit matrix elements has been considered. The maximum absorption within the therapeutic window has been confirmed for all the aza-BODIPY derivatives. The feasible intersystem spin crossing pathways for the population of the lowest triplet state, that will depend on the values of the spin-orbit matrix elements, the energy gap as well as the orbital composition of the involved states have been found to most likely involve the S 1 and T 1 or T 2 states. The outcomes of computations support the potential therapeutic use of these compounds as photosensitizers in photodynamic therapy.

Enhanced magneto-optical Kerr effect at Fe/insulator interfaces

NASA Astrophysics Data System (ADS)

Gu, Bo; Takahashi, Saburo; Maekawa, Sadamichi

2017-12-01

Using density functional theory calculations, we have found an enhanced magneto-optical Kerr effect in Fe/insulator interfaces. The results of our study indicate that interfacial Fe atoms in the Fe films have a low-dimensional nature, which causes the following two effects: (i) The diagonal component σx x of the optical conductivity decreases dramatically because the hopping integral for electrons between Fe atoms is suppressed by the low dimensionality. (ii) The off-diagonal component σx y of the optical conductivity does not change at low photon energies, but it is enhanced at photon energies around 2 eV, where we obtain enhanced orbital magnetic moments and spin-orbit correlations for the interfacial Fe atoms. A large Kerr angle develops in proportion to the ratio σx y/σx x . Our findings indicate an efficient way to enhance the effect of spin-orbit coupling at metal/insulator interfaces without using heavy elements.

An ESR study of the UV degradation of FEP

NASA Technical Reports Server (NTRS)

George, G. A.; Hill, D. J. T.; Odonnell, J. H.; Pomery, P. J.; Rasoul, F.

1992-01-01

Spacecraft in low earth orbit are subjected to significant levels of high energy radiation, including ultraviolet (UV) and visible ultraviolet (VUV) wavelengths. The effects of UV radiation are enhanced over those at the surface of the earth, where the only incident wavelengths are greater than 290 nm. In low earth orbit the incident UV wavelengths extend below 290 nm into the VUV region, where the Lyman alpha-emissions of atomic hydrogen occur at 121 nm. In addition to electromagnetic radiation, in low earth orbit polymer materials may also be subjected to atomic oxygen particle radiation, which will result in direct oxidation of the polymer.

Scanning tunneling microscopy current from localized basis orbital density functional theory

NASA Astrophysics Data System (ADS)

Gustafsson, Alexander; Paulsson, Magnus

2016-03-01

We present a method capable of calculating elastic scanning tunneling microscopy (STM) currents from localized atomic orbital density functional theory (DFT). To overcome the poor accuracy of the localized orbital description of the wave functions far away from the atoms, we propagate the wave functions, using the total DFT potential. From the propagated wave functions, the Bardeen's perturbative approach provides the tunneling current. To illustrate the method we investigate carbon monoxide adsorbed on a Cu(111) surface and recover the depression/protrusion observed experimentally with normal/CO-functionalized STM tips. The theory furthermore allows us to discuss the significance of s - and p -wave tips.

Issues and Consequences of Atomic Oxygen Undercutting of Protected Polymers in Low Earth Orbit

NASA Technical Reports Server (NTRS)

Banks, Bruce A.; Snyder, Aaron; Miller, Sharon K.; Demko, Rikako

2002-01-01

Hydrocarbon based polymers that are exposed to atomic oxygen in low Earth orbit are slowly oxidized which results in recession of their surface. Atomic oxygen protective coatings have been developed which are both durable to atomic oxygen and effective in protecting underlying polymers. However, scratches, pin window defects, polymer surface roughness and protective coating layer configuration can result in erosion and potential failure of protected thin polymer films even though the coatings are themselves atomic oxygen durable. This paper will present issues that cause protective coatings to become ineffective in some cases yet effective in others due to the details of their specific application. Observed in-space examples of failed and successfully protected materials using identical protective thin films will be discussed and analyzed. Proposed approaches to prevent the failures that have been observed will also be presented.

A Variational Monte Carlo Approach to Atomic Structure

ERIC Educational Resources Information Center

Davis, Stephen L.

2007-01-01

The practicality and usefulness of variational Monte Carlo calculations to atomic structure are demonstrated. It is found to succeed in quantitatively illustrating electron shielding, effective nuclear charge, l-dependence of the orbital energies, and singlet-tripetenergy splitting and ionization energy trends in atomic structure theory.

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.

Durability Issues for the Protection of Materials from Atomic Oxygen Attack in Low Earth Orbit

NASA Technical Reports Server (NTRS)

Banks, Bruce; Lenczewski, Mary; Demko, Rikako

2002-01-01

Low Earth orbital atomic oxygen is capable of eroding most polymeric materials typically used on spacecraft. Solar array blankets, thermal control polymers, and carbon fiber matrix composites are readily oxidized to become thinner and less capable of supporting the loads imposed upon them. Protective coatings have been developed that are durable to atomic oxygen to prevent oxidative erosion of the underlying polymers. However, the details of the surface roughness, coating defect density, and coating configuration can play a significant role as to whether or not the coating provides long duration atomic oxygen protection. Identical coatings on different surface roughness surfaces can have drastically different durability results. Examples and analysis of the causes of resultant differences in atomic oxygen protection are presented. Implications based on in-space experiences, ground laboratory testing, and computational modeling indicate that thin film vacuum-deposited aluminum protective coatings offer much less atomic oxygen protection than sputter-deposited silicon dioxide coatings.

LDEF microenvironments, observed and predicted

NASA Astrophysics Data System (ADS)

Bourassa, R. J.; Pippin, H. G.; Gillis, J. R.

1993-04-01

A computer model for prediction of atomic oxygen exposure of spacecraft in low earth orbit, referred to as the primary atomic oxygen model, was originally described at the First Long Duration Exposure Facility (LDEF) Post-Retrieval Symposium. The primary atomic oxygen model accounts for variations in orbit parameters, the condition of the atmosphere, and for the orientation of exposed surfaces relative to the direction of spacecraft motion. The use of the primary atomic oxygen model to define average atomic oxygen exposure conditions for a spacecraft is discussed and a second microenvironments computer model is described that accounts for shadowing and scattering of atomic oxygen by complex surface protrusions and indentations. Comparisons of observed and predicted erosion of fluorinated ethylene propylene (FEP) thermal control blankets using the models are presented. Experimental and theoretical results are in excellent agreement. Work is in progress to expand modeling capability to include ultraviolet radiation exposure and to obtain more detailed information on reflecting and scattering characteristics of material surfaces.

LDEF microenvironments, observed and predicted

NASA Technical Reports Server (NTRS)

Bourassa, R. J.; Pippin, H. G.; Gillis, J. R.

1993-01-01

A computer model for prediction of atomic oxygen exposure of spacecraft in low earth orbit, referred to as the primary atomic oxygen model, was originally described at the First Long Duration Exposure Facility (LDEF) Post-Retrieval Symposium. The primary atomic oxygen model accounts for variations in orbit parameters, the condition of the atmosphere, and for the orientation of exposed surfaces relative to the direction of spacecraft motion. The use of the primary atomic oxygen model to define average atomic oxygen exposure conditions for a spacecraft is discussed and a second microenvironments computer model is described that accounts for shadowing and scattering of atomic oxygen by complex surface protrusions and indentations. Comparisons of observed and predicted erosion of fluorinated ethylene propylene (FEP) thermal control blankets using the models are presented. Experimental and theoretical results are in excellent agreement. Work is in progress to expand modeling capability to include ultraviolet radiation exposure and to obtain more detailed information on reflecting and scattering characteristics of material surfaces.

Novel oxygen atom source for material degradation studies

NASA Technical Reports Server (NTRS)

Krech, R. H.; Caledonia, G. E.

1988-01-01

Physical Sciences Inc. (PSI) has developed a high flux pulsed source of energetic (8 km/s) atomic oxygen to bombard specimens in experiments on the aging and degradation of materials in a low earth orbit environment. The proof-of-concept of the PSI approach was demonstrated in a Phase 1 effort. In Phase 2 a large O-atom testing device (FAST-2) has been developed and characterized. Quantitative erosion testing of materials, components, and even small assemblies (such as solar cell arrays) can be performed with this source to determine which materials and/or components are most vulnerable to atomic oxygen degradation. The source is conservatively rated to irradiate a 100 sq cm area sample at greater than 10(exp 17) atoms/s, at a 10 Hz pulse rate. Samples can be exposed to an atomic oxygen fluence equivalent to the on-orbit ram direction exposure levels incident on Shuttle surfaces at 250 km during a week-long mission in a few hours.

An ab initio MO study of heavy atom effects on the zero-field splitting tensors of high-spin nitrenes: how the spin-orbit contributions are affected.

PubMed

Sugisaki, Kenji; Toyota, Kazuo; Sato, Kazunobu; Shiomi, Daisuke; Kitagawa, Masahiro; Takui, Takeji

2014-05-21

The CASSCF and the hybrid CASSCF-MRMP2 methods are applied to the calculations of spin-spin and spin-orbit contributions to the zero-field splitting tensors (D tensors) of the halogen-substituted spin-septet 2,4,6-trinitrenopyridines, focusing on the heavy atom effects on the spin-orbit term of the D tensors (D(SO) tensors). The calculations reproduced experimentally determined |D| values within an error of 15%. Halogen substitutions at the 3,5-positions are less influential in the spin-spin dipolar (D(SS)) term of 2,4,6-trinitrenopyridines, although the D(SO) terms are strongly affected by the introduction of heavier halogens. The absolute sign of the D(SO) value (D = D(ZZ) - (D(XX) + D(YY))/2) of 3,5-dibromo derivative 3 is predicted to be negative, which contradicts the Pederson-Khanna (PK) DFT result previously reported. The large negative contributions to the D(SO) value of 3 arise from the excited spin-septet states ascribed mainly to the excitations of in-plane lone pair of bromine atoms → SOMO of π nature. The importance of the excited states involving electron transitions from the lone pair orbital of the halogen atom is also confirmed in the D(SO) tensors of halogen-substituted para-phenylnitrenes. A new scheme based on the orbital region partitioning is proposed for the analysis of the D(SO) tensors as calculated by means of the PK-DFT approach.

Production of confluent hypergeometric beam by computer-generated hologram

NASA Astrophysics Data System (ADS)

Chen, Jiannong; Wang, Gang; Xu, Qinfeng

2011-02-01

Because of their spiral wave front, phase singularity, zero-intensity center and orbital angular momentum, dark hollow vortex beams have been found many applications in the field of atom optics such as atom cooling, atom transport and atom guiding. In this paper, a method for generating confluent hypergeometric beam by computer-generated hologram displayed on the spatial light modulator is presented. The hologram is formed by interference between a single ring Laguerre-Gaussian beam and a plane wave. The far-field Fraunhofer diffraction of this optical field transmitted from the hologram is the confluent hypergeometric beam. This beam is a circular symmetric beam which has a phase singularity, spiral wave front, zero-intensity center, and intrinsic orbital angular momentum. It is a new dark hollow vortex beam.

Microhartree precision in density functional theory calculations

NASA Astrophysics Data System (ADS)

Gulans, Andris; Kozhevnikov, Anton; Draxl, Claudia

2018-04-01

To address ultimate precision in density functional theory calculations we employ the full-potential linearized augmented plane-wave + local-orbital (LAPW + lo) method and justify its usage as a benchmark method. LAPW + lo and two completely unrelated numerical approaches, the multiresolution analysis (MRA) and the linear combination of atomic orbitals, yield total energies of atoms with mean deviations of 0.9 and 0.2 μ Ha , respectively. Spectacular agreement with the MRA is reached also for total and atomization energies of the G2-1 set consisting of 55 molecules. With the example of α iron we demonstrate the capability of LAPW + lo to reach μ Ha /atom precision also for periodic systems, which allows also for the distinction between the numerical precision and the accuracy of a given functional.

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

PubMed

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

2017-04-07

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

Correlation of nonorthogonality of best hybrid bond orbitals with bond strength of orthogonal orbitals

PubMed Central

Pauling, Linus

1976-01-01

An expression is derived for the bond length of two spd orbitals with maximum values in two directions forming a given bond angle by consideration of the nonorthogonality integral of two best orbitals in these directions. This equation is equivalent to the expression derived by formulating the pair of orthogonal orbitals. Similar expressions are derived for spdf orbitals. Applications are made to icosahedral and cuboctahedral bonds and to the packing of nucleons in atomic nuclei. PMID:16578736

Correlation of nonorthogonality of best hybrid bond orbitals with bond strength of orthogonal orbitals.

PubMed

Pauling, L

1976-02-01

An expression is derived for the bond length of two spd orbitals with maximum values in two directions forming a given bond angle by consideration of the nonorthogonality integral of two best orbitals in these directions. This equation is equivalent to the expression derived by formulating the pair of orthogonal orbitals. Similar expressions are derived for spdf orbitals. Applications are made to icosahedral and cuboctahedral bonds and to the packing of nucleons in atomic nuclei.

Visualisation and orbital-free parametrisation of the large-Z scaling of the kinetic energy density of atoms

NASA Astrophysics Data System (ADS)

Cancio, Antonio C.; Redd, Jeremy J.

2017-03-01

The scaling of neutral atoms to large Z, combining periodicity with a gradual trend to homogeneity, is a fundamental probe of density functional theory, one that has driven recent advances in understanding both the kinetic and exchange-correlation energies. Although research focus is normally upon the scaling of integrated energies, insights can also be gained from energy densities. We visualise the scaling of the positive-definite kinetic energy density (KED) in closed-shell atoms, in comparison to invariant quantities based upon the gradient and Laplacian of the density. We notice a striking fit of the KED within the core of any atom to a gradient expansion using both the gradient and the Laplacian, appearing as an asymptotic limit around which the KED oscillates. The gradient expansion is qualitatively different from that derived from first principles for a slowly varying electron gas and is correlated with a nonzero Pauli contribution to the KED near the nucleus. We propose and explore orbital-free meta-GGA models for the kinetic energy to describe these features, with some success, but the effects of quantum oscillations in the inner shells of atoms make a complete parametrisation difficult. We discuss implications for improved orbital-free description of molecular properties.

Charge versus orbital-occupancy ordering in manganites

NASA Astrophysics Data System (ADS)

Luo, Weidong; Varela, Maria; Tao, Jing; Pennycook, Stephen J.; Pantelides, Sokrates T.

2006-03-01

It is generally assumed that density-functional theory (DFT) in the local-spin-density approximation (LSDA) or the generalized- gradient approximation (GGA) is not adequate to describe mixed- valence manganites. Here we report benchmark DFT/GGA calculations for the ground-state structural, electronic and magnetic properties for both undoped and doped CaMnO3 and find the results to be in excellent agreement with available data, including new atomic-resolution Z-contrast imaging and electron-energy loss spectra. More specifically, we found that the DFT results predict two inequivalent Mn atoms in both 0.33 and 0.5 electron-doped CaMnO3, in agreement with experimental evidence of Mn^+3/Mn^+4 oxidation state ordering. The inequivalent Mn atoms are marked by their distinctive orbital occupancies, dissimilar local Jahn-Teller distortion and different magnetic moments from DFT calculations. We also show that the spherically integrated charges associated with the two inequivalent Mn atoms are the same, and they are actually the same as in the Mn metal. This charge neutrality with different orbital occupancies is the result of self-consistency and atomic relaxations in the crystal. We conclude that DFT without additional correlations can account for the observed properties of oxidation-state ordering in this system. The impact of the results on other mixed-valence systems will be discussed.

Quantitative structure-property relationships for octanol-water partition coefficients of polybrominated diphenyl ethers.

PubMed

Li, Linnan; Xie, Shaodong; Cai, Hao; Bai, Xuetao; Xue, Zhao

2008-08-01

Theoretical molecular descriptors were tested against logK(OW) values for polybrominated diphenyl ethers (PBDEs) using the Partial Least-Squares Regression method which can be used to analyze data with many variables and few observations. A quantitative structure-property relationship (QSPR) model was successfully developed with a high cross-validated value (Q(cum)(2)) of 0.961, indicating a good predictive ability and stability of the model. The predictive power of the QSPR model was further cross-validated. The values of logK(OW) for PBDEs are mainly governed by molecular surface area, energy of the lowest unoccupied molecular orbital and the net atomic charges on the oxygen atom. All these descriptors have been discussed to interpret the partitioning mechanism of PBDE chemicals. The bulk property of the molecules represented by molecular surface area is the leading factor, and K(OW) values increase with the increase of molecular surface area. Higher energy of the lowest unoccupied molecular orbital and higher net atomic charge on the oxygen atom of PBDEs result in smaller K(OW). The energy of the lowest unoccupied molecular orbital and the net atomic charge on PBDEs oxygen also play important roles in affecting the partition of PBDEs between octanol and water by influencing the interactions between PBDEs and solvent molecules.

Quantum Mechanical Studies of Molecular Hyperpolarizabilities.

DTIC Science & Technology

1980-04-30

exponent , reflects the screening of an electron in a given orbital by the interior electrons in the atom or molecule. In practice, when studying...Basis sets have evolved over the years in molecular quantum mechanics until sets of orbital exponents for the different atoms composing the molecule have...and R. P. Hurst , J. Chem. Phys. 46, 2356 (1967); S. P. LickmannI and J. W. Moskowitz, J. Chem. Phys. 54, 3622 7T971). 26. T. H. Dunning, J. Chem. Phys

Relativistic Spin-Orbit Heavy Atom on the Light Atom NMR Chemical Shifts: General Trends Across the Periodic Table Explained.

PubMed

Vícha, Jan; Komorovsky, Stanislav; Repisky, Michal; Marek, Radek; Straka, Michal

2018-06-12

The importance of relativistic effects on the NMR parameters in heavy-atom (HA) compounds, particularly the SO-HALA (Spin-Orbit Heavy Atom on the Light Atom) effect on NMR chemical shifts, has been known for about 40 years. Yet, a general correlation between the electronic structure and SO-HALA effect has been missing. By analyzing 1 H NMR chemical shifts of the sixth-period hydrides (Cs-At), we discovered general electronic-structure principles and mechanisms that dictate the size and sign of the SO-HALA NMR chemical shifts. In brief, partially occupied HA valence shells induce relativistic shielding at the light atom (LA) nuclei, while empty HA valence shells induce relativistic deshielding. In particular, the LA nucleus is relativistically shielded in 5d 2 -5d 8 and 6p 4 HA hydrides and deshielded in 4f 0 , 5d 0 , 6s 0 , and 6p 0 HA hydrides. This general and intuitive concept explains periodic trends in the 1 H NMR chemical shifts along the sixth-period hydrides (Cs-At) studied in this work. We present substantial evidence that the introduced principles have a general validity across the periodic table and can be extended to nonhydride LAs. The decades-old question of why compounds with occupied frontier π molecular orbitals (MOs) cause SO-HALA shielding at the LA nuclei, while the frontier σ MOs cause deshielding is answered. We further derive connection between the SO-HALA NMR chemical shifts and Spin-Orbit-induced Electron Deformation Density (SO-EDD), a property that can be obtained easily from differential electron densities and can be represented graphically. SO-EDD provides an intuitive understanding of the SO-HALA effect in terms of the depletion/concentration of the electron density at LA nuclei caused by spin-orbit coupling due to HA in the presence of a magnetic field. Using an analogy between the SO-EDD concept and arguments from classic NMR theory, the complex question of the SO-HALA NMR chemical shifts becomes easily understandable for a wide chemical audience.

Self-consistent average-atom scheme for electronic structure of hot and dense plasmas of mixture.

PubMed

Yuan, Jianmin

2002-10-01

An average-atom model is proposed to treat the electronic structures of hot and dense plasmas of mixture. It is assumed that the electron density consists of two parts. The first one is a uniform distribution with a constant value, which is equal to the electron density at the boundaries between the atoms. The second one is the total electron density minus the first constant distribution. The volume of each kind of atom is proportional to the sum of the charges of the second electron part and of the nucleus within each atomic sphere. By this way, one can make sure that electrical neutrality is satisfied within each atomic sphere. Because the integration of the electron charge within each atom needs the size of that atom in advance, the calculation is carried out in a usual self-consistent way. The occupation numbers of electron on the orbitals of each kind of atom are determined by the Fermi-Dirac distribution with the same chemical potential for all kinds of atoms. The wave functions and the orbital energies are calculated with the Dirac-Slater equations. As examples, the electronic structures of the mixture of Au and Cd, water (H2O), and CO2 at a few temperatures and densities are presented.

Accurate and balanced anisotropic Gaussian type orbital basis sets for atoms in strong magnetic fields.

PubMed

Zhu, Wuming; Trickey, S B

2017-12-28

In high magnetic field calculations, anisotropic Gaussian type orbital (AGTO) basis functions are capable of reconciling the competing demands of the spherically symmetric Coulombic interaction and cylindrical magnetic (B field) confinement. However, the best available a priori procedure for composing highly accurate AGTO sets for atoms in a strong B field [W. Zhu et al., Phys. Rev. A 90, 022504 (2014)] yields very large basis sets. Their size is problematical for use in any calculation with unfavorable computational cost scaling. Here we provide an alternative constructive procedure. It is based upon analysis of the underlying physics of atoms in B fields that allow identification of several principles for the construction of AGTO basis sets. Aided by numerical optimization and parameter fitting, followed by fine tuning of fitting parameters, we devise formulae for generating accurate AGTO basis sets in an arbitrary B field. For the hydrogen iso-electronic sequence, a set depends on B field strength, nuclear charge, and orbital quantum numbers. For multi-electron systems, the basis set formulae also include adjustment to account for orbital occupations. Tests of the new basis sets for atoms H through C (1 ≤ Z ≤ 6) and ions Li + , Be + , and B + , in a wide B field range (0 ≤ B ≤ 2000 a.u.), show an accuracy better than a few μhartree for single-electron systems and a few hundredths to a few mHs for multi-electron atoms. The relative errors are similar for different atoms and ions in a large B field range, from a few to a couple of tens of millionths, thereby confirming rather uniform accuracy across the nuclear charge Z and B field strength values. Residual basis set errors are two to three orders of magnitude smaller than the electronic correlation energies in multi-electron atoms, a signal of the usefulness of the new AGTO basis sets in correlated wavefunction or density functional calculations for atomic and molecular systems in an external strong B field.

Accurate and balanced anisotropic Gaussian type orbital basis sets for atoms in strong magnetic fields

NASA Astrophysics Data System (ADS)

Zhu, Wuming; Trickey, S. B.

2017-12-01

In high magnetic field calculations, anisotropic Gaussian type orbital (AGTO) basis functions are capable of reconciling the competing demands of the spherically symmetric Coulombic interaction and cylindrical magnetic (B field) confinement. However, the best available a priori procedure for composing highly accurate AGTO sets for atoms in a strong B field [W. Zhu et al., Phys. Rev. A 90, 022504 (2014)] yields very large basis sets. Their size is problematical for use in any calculation with unfavorable computational cost scaling. Here we provide an alternative constructive procedure. It is based upon analysis of the underlying physics of atoms in B fields that allow identification of several principles for the construction of AGTO basis sets. Aided by numerical optimization and parameter fitting, followed by fine tuning of fitting parameters, we devise formulae for generating accurate AGTO basis sets in an arbitrary B field. For the hydrogen iso-electronic sequence, a set depends on B field strength, nuclear charge, and orbital quantum numbers. For multi-electron systems, the basis set formulae also include adjustment to account for orbital occupations. Tests of the new basis sets for atoms H through C (1 ≤ Z ≤ 6) and ions Li+, Be+, and B+, in a wide B field range (0 ≤ B ≤ 2000 a.u.), show an accuracy better than a few μhartree for single-electron systems and a few hundredths to a few mHs for multi-electron atoms. The relative errors are similar for different atoms and ions in a large B field range, from a few to a couple of tens of millionths, thereby confirming rather uniform accuracy across the nuclear charge Z and B field strength values. Residual basis set errors are two to three orders of magnitude smaller than the electronic correlation energies in multi-electron atoms, a signal of the usefulness of the new AGTO basis sets in correlated wavefunction or density functional calculations for atomic and molecular systems in an external strong B field.

The relationship of the globe to the orbital rim.

PubMed

Eckstein, Lauren A; Shadpour, Joseph M; Menghani, Ravi; Goldberg, Robert A

2011-01-01

To present a novel method for accurately characterizing the position of the globe relative to the orbital rim. The appearance and function of the eyelids are dependent on the underlying orbital bony architecture and globe position; however, no comprehensive language to describe these complex 3-dimensional relationships exists. Three-dimensional orbital reconstructions were generated from computed tomographic scans of 15 Occidental and 12 Oriental orbits without orbital pathologic disease. Globe and orbital rim anatomy were identified and outlined. Reference points were measured along 2 independent axes: (1) the distance between a plane defined by the corneal apex and the sagittal projection of the orbital rim and (2) the distance between the circumference of the globe and the coronal projection of the orbital rim. For Occidental orbits, the mean (SD) elevation of the sagittal projection of the orbital rim relative to the anterior projection of the globe was 4.6 (4.2) mm superiorly, 5.9 (3.0) mm nasally, 12.6 (3.7) mm inferiorly, and 20.6 (2.6) mm laterally. The mean (SD) radial distance between the coronal projection of the orbital rim and the circumference of the globe was 3.7 (2.1) mm superiorly, 7.6 (1.8) mm nasally, 6.6 (2.2) mm inferiorly, and 4.6 (2.3) mm laterally. For Oriental orbits, the mean (SD) elevation of the sagittal projection of the orbital rim relative to the anterior projection of the globe was 5.0 (4.5) mm superiorly, 6.8 (4.1) mm nasally, 11.1 (4.3) mm inferiorly, and 17.5 (3.3) mm laterally. The mean (SD) radial distance between the coronal projection of the orbital rim and the circumference of the globe was 2.1 (1.2) mm superiorly, 8.2 (2.0) mm nasally, 6.5 (1.9) mm inferiorly, and 4.5 (1.7) mm laterally. Comparison of Occidental and Oriental orbital rim and globe configurations revealed quantitative and qualitative differences. In addition to differences in soft-tissue anatomy, bony architectural variations may contribute substantially to racial differences in the surface anatomy of the periorbital area. Anatomic analysis, based on 3-dimensional orbital imaging, may provide a rational approach to surgical planning for aesthetic and reconstructive orbitofacial surgery.

Time-reversal-invariant spin-orbit-coupled bilayer Bose-Einstein condensates

NASA Astrophysics Data System (ADS)

Maisberger, Matthew; Wang, Lin-Cheng; Sun, Kuei; Xu, Yong; Zhang, Chuanwei

2018-05-01

Time-reversal invariance plays a crucial role for many exotic quantum phases, particularly for topologically nontrivial states, in spin-orbit coupled electronic systems. Recently realized spin-orbit coupled cold-atom systems, however, lack the time-reversal symmetry due to the inevitable presence of an effective transverse Zeeman field. We address this issue by analyzing a realistic scheme to preserve time-reversal symmetry in spin-orbit-coupled ultracold atoms, with the use of Hermite-Gaussian-laser-induced Raman transitions that preserve spin-layer time-reversal symmetry. We find that the system's quantum states form Kramers pairs, resulting in symmetry-protected gap closing of the lowest two bands at arbitrarily large Raman coupling. We also show that Bose gases in this setup exhibit interaction-induced layer-stripe and uniform phases as well as intriguing spin-layer symmetry and spin-layer correlation.

Supramolecular aromaticity

NASA Astrophysics Data System (ADS)

Karabıyık, Hande; Sevinçek, Resul; Karabıyık, Hasan

2014-05-01

We report experimental and theoretical evidences for supramolecular aromaticity as a new concept to be widely used in researches about molecular crystals. CSD survey regarding frequently encountered resonance-assisted H-bonds (RAHBs) in formic acid, formamide, formimidamide, formic acid-formamide, and formamide-formimidamide dimers shows that supramolecular quasirings formed by RAHBs have remarkable electronic delocalization within themselves, which is reminiscent of aromaticity at supramolecular level. This study criticizes and reevaluates the validity of conventional judgment which states that ring systems formed by intermolecular H-bonds cannot be aromatic. Thus, the term aromaticity can be extended to supramolecular systems formed by RAHBs. Supramolecular aromaticity has a multi-fold nature involving both σ- and π-delocalization, and σ-delocalization through RAHBs takes on a task of compensating σ-deficiency within quasirings. Atomic composition in donor-acceptor set of the dimers is descriptive for supramolecular aromaticity. We revised bond-valence parameters for RAHBs and they suggest that hypervalent character of H atoms is more pronounced than their hypovalent character in RAHBs. The σ-delocalized bonding within H-bonded quasirings necessitates hypervalent character of H atoms. Quantum chemical calculations based on adiabatic Hydrogen Atom Transfer (HAT) between the monomers reveal that topological parameters at ring critical points (RCPs) of the quasirings correlate well with Shannon's entropic aromaticity index. The presence of additional LP orbital on O atoms implying more diffused LP-orbitals in donor-acceptor set leads to the formation of resonance-disabling states reducing supramolecular aromaticity of a quasiring and energetic cost of the electron transfer between the monomers. There is a nonignorable electron transfer between the monomers even in the cases where H atoms are close to donor or acceptor atom. NBO analyses have revealed that formally vacant LP* orbitals on H-atoms in TS geometries mediate intermolecular electron transfer as a result of the hyperconjugative stereoelectronic interactions.

Finite size effect on hydrogen bond cooperativity in (Ala)n polypeptides: A DFT study using numeric atom-centered orbitals

NASA Astrophysics Data System (ADS)

Blum, Volker; Ireta, Joel; Scheffler, Matthias

2007-03-01

An accurate representation of the energetic contribution Ehb of hydrogen bonds to structure formation is paramount to understand the secondary structure stability of proteins, both qualitatively and quantitatively. However, Ehb depends strongly on its environment, and even on the surrounding peptide conformation itself. For instance, a short α-helical polypeptide (Ala)4 can not be stabilized by its single hydrogen bond, whereas an infinite α-helical chain (Ala)∞ is clearly energetically stable over a fully extended conformation. We here use all-electron density functional calculations in the PBE generalized gradient approximation by a recently developed, computationally efficient numeric atom-centered orbital based code^1 to investigate this H-bond cooperativity that is intrinsic to Alanine-based polypeptides (Ala)n (n=1-20,∞). We compare finite and infinite prototypical helical conformations (α, π, 310) on equal footing, with both neutral and ionic termination for finite (Ala)n peptides. Moderately sized NAO basis sets allow to capture Ehb with meV accuracy, revealing a clear jump in Ehb (cooperativity) when two H-bonds first appear in line, followed by slower and more continuous increase of Ehb towards n->∞. ^1 V. Blum, R. Gehrke, P. Havu, V. Havu, M. Scheffler, The FHI Ab Initio Molecular Simulations (aims) Project, Fritz-Haber-Institut, Berlin (2006).

Electronic structure of stoichiometric and reduced ZnO from periodic relativistic all electron hybrid density functional calculations using numeric atom-centered orbitals.

PubMed

Viñes, Francesc; Illas, Francesc

2017-03-30

The atomic and electronic structure of stoichiometric and reduced ZnO wurtzite has been studied using a periodic relativistic all electron hybrid density functional (PBE0) approach and numeric atom-centered orbital basis set with quality equivalent to aug-cc-pVDZ. To assess the importance of relativistic effects, calculations were carried out without and with explicit inclusion of relativistic effects through the zero order regular approximation. The calculated band gap is ∼0.2 eV smaller than experiment, close to previous PBE0 results including relativistic calculation through the pseudopotential and ∼0.25 eV smaller than equivalent nonrelativistic all electron PBE0 calculations indicating possible sources of error in nonrelativistic all electron density functional calculations for systems containing elements with relatively high atomic number. The oxygen vacancy formation energy converges rather fast with the supercell size, the predicted value agrees with previously hybrid density functional calculations and analysis of the electronic structure evidences the presence of localized electrons at the vacancy site with a concomitant well localized peak in the density of states ∼0.5 eV above the top of the valence band and a significant relaxation of the Zn atoms near to the oxygen vacancy. Finally, present work shows that accurate results can be obtained in systems involving large supercells containing up to ∼450 atoms using a numeric atomic-centered orbital basis set within a full all electron description including scalar relativistic effects at an affordable cost. © 2017 Wiley Periodicals, Inc. © 2017 Wiley Periodicals, Inc.

A Comprehensive Analysis in Terms of Molecule-Intrinsic, Quasi-Atomic Orbitals. III. The Covalent Bonding Structure of Urea.

PubMed

West, Aaron C; Schmidt, Michael W; Gordon, Mark S; Ruedenberg, Klaus

2015-10-15

The analysis of molecular electron density matrices in terms of quasi-atomic orbitals, which was developed in previous investigations, is quantitatively exemplified by a detailed application to the urea molecule. The analysis is found to identify strong and weak covalent bonding interactions as well as intramolecular charge transfers. It yields a qualitative as well as quantitative ab initio description of the bonding structure of this molecule, which raises questions regarding some traditional rationalizations.

Empirical Monod-Beuneu relation of spin relaxation revisited for elemental metals

NASA Astrophysics Data System (ADS)

Szolnoki, L.; Kiss, A.; Forró, L.; Simon, F.

2014-03-01

Monod and Beuneu [P. Monod and F. Beuneu, Phys. Rev. B 19, 911 (1979), 10.1103/PhysRevB.19.911] established the validity of the Elliott-Yafet theory for elemental metals through correlating the experimental electron spin resonance linewidth with the so-called spin-orbit admixture coefficients and the momentum-relaxation theory. The spin-orbit admixture coefficients data were based on atomic spin-orbit splitting. We highlight two shortcomings of the previous description: (i) the momentum-relaxation involves the Debye temperature and the electron-phonon coupling whose variation among the elemental metals was neglected, (ii) the Elliott-Yafet theory involves matrix elements of the spin-orbit coupling (SOC), which are however not identical to the SOC induced energy splitting of the atomic levels, even though the two have similar magnitudes. We obtain the empirical spin-orbit admixture parameters for the alkali metals by considering the proper description of the momentum relaxation theory. In addition we present a model calculation, which highlights the difference between the SOC matrix element and energy splitting.

Adaptive frozen orbital treatment for the fragment molecular orbital method combined with density-functional tight-binding

NASA Astrophysics Data System (ADS)

Nishimoto, Yoshio; Fedorov, Dmitri G.

2018-02-01

The exactly analytic gradient is derived and implemented for the fragment molecular orbital (FMO) method combined with density-functional tight-binding (DFTB) using adaptive frozen orbitals. The response contributions which arise from freezing detached molecular orbitals on the border between fragments are computed by solving Z-vector equations. The accuracy of the energy, its gradient, and optimized structures is verified on a set of representative inorganic materials and polypeptides. FMO-DFTB is applied to optimize the structure of a silicon nano-wire, and the results are compared to those of density functional theory and experiment. FMO accelerates the DFTB calculation of a boron nitride nano-ring with 7872 atoms by a factor of 406. Molecular dynamics simulations using FMO-DFTB applied to a 10.7 μm chain of boron nitride nano-rings, consisting of about 1.2 × 106 atoms, reveal the rippling and twisting of nano-rings at room temperature.

Rashba spin-orbit coupling for neutral atoms

NASA Astrophysics Data System (ADS)

Campbell, Daniel; Juzeliūnas, Gediminas; Spielman, Ian

2011-05-01

We theoretically describe a new class of atom-laser coupling schemes which lead to effective spin-orbit coupled Hamiltonians for ultra-cold neutral atoms. By properly setting the optical phases, a pair of degenerate spin states emerge as the lowest energy states in the spectrum, and are thus immune to collisionally induced decay. These schemes use N cyclically coupled ground or metastable internal states but we will specialize to the four-level case for this talk. Time permitting, we will describe a possible implementation of this scheme for 87Rb that adds a controllable Dresselhaus component to the effective Hamiltonian in a natural way. NSF through PFC at JQI, ARO with funds from Atomtronics MURI and DARPA OLE, STREP NAMEQUAM.

Antihydrogen-hydrogen elastic scattering at thermal energies using an atomic-orbital technique

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

Sinha, Prabal K.; Chaudhuri, Puspitapallab; Ghosh, A.S.

2003-05-01

In view of the recent interest in the trapping of antihydrogen atom H(bar sign), at very low temperatures, H-bar-H scattering has been investigated at low incident energies using a close-coupling model with the basis set H-bar(1s,2s,2p-bar)+H(1s,2s,2p-bar). The predicted s-wave elastic phase shifts, scattering length, and effective range are in a good agreement with the other recent predictions of Jonsell et al. and of Armour and Chamberlain. The results indicate that the atomic orbital expansion model is suitable to study the H-bar-H scattering at ultracold temperatures.

Understanding the quantum nature of low-energy C(3P j ) + He inelastic collisions.

PubMed

Bergeat, Astrid; Chefdeville, Simon; Costes, Michel; Morales, Sébastien B; Naulin, Christian; Even, Uzi; Kłos, Jacek; Lique, François

2018-05-01

Inelastic collisions that occur between open-shell atoms and other atoms or molecules, and that promote a spin-orbit transition, involve multiple interaction potentials. They are non-adiabatic by nature and cannot be described within the Born-Oppenheimer approximation; in particular, their theoretical modelling becomes very challenging when the collision energies have values comparable to the spin-orbit splitting. Here we study inelastic collisions between carbon in its ground state C( 3 P j=0 ) and helium atoms-at collision energies in the vicinity of spin-orbit excitation thresholds (~0.2 and 0.5 kJ mol -1 )-that result in spin-orbit excitation to C( 3 P j=1 ) and C( 3 P j=2 ). State-to-state integral cross-sections are obtained from crossed-beam experiments with a beam source that provides an almost pure beam of C( 3 P j=0 ) . We observe very good agreement between experimental and theoretical results (acquired using newly calculated potential energy curves), which validates our characterization of the quantum dynamical resonances that are observed. Rate coefficients at very low temperatures suitable for chemical modelling of the interstellar medium are also calculated.

O-atom degradation mechanisms of materials

NASA Technical Reports Server (NTRS)

Coulter, Daniel R.; Liang, Ranty H.; Chung, Shirley Y.; Smith, Keri Oda; Gupta, Amitava

1987-01-01

The low Earth orbit environment is described and the critical issues relating to oxygen atom degradation are discussed. Some analytic techniques for studying the problem and preliminary results on the underlying degradation mechanisms are presented.

Low Earth orbital atomic oxygen and ultraviolet radiation effects on polymers

NASA Technical Reports Server (NTRS)

Dever, Joyce A.

1991-01-01

Because atomic oxygen and solar ultraviolet radiation present in the low earth orbital (LEO) environment can alter the chemistry of polymers resulting in degradation, their effects and mechanisms of degradation must be determined in order to determine the long term durability of polymeric surfaces to be exposed on missions such as Space Station Freedom. The effects of atomic oxygen on polymers which contain protective coatings must also be explored, since unique damage mechanisms can occur in areas where the protective coatings has failed. Mechanisms can be determined by utilizing results from previous LEO missions, by performing ground based LEO simulation tests and analysis, and by carrying out focussed space experiments. A survey is presented of the interactions and possible damage mechanisms for environmental atomic oxygen and UV radiation exposure of polymers commonly used in LEO.

Ballistic Anisotropic Magnetoresistance of Single-Atom Contacts.

PubMed

Schöneberg, J; Otte, F; Néel, N; Weismann, A; Mokrousov, Y; Kröger, J; Berndt, R; Heinze, S

2016-02-10

Anisotropic magnetoresistance, that is, the sensitivity of the electrical resistance of magnetic materials on the magnetization direction, is expected to be strongly enhanced in ballistic transport through nanoscale junctions. However, unambiguous experimental evidence of this effect is difficult to achieve. We utilize single-atom junctions to measure this ballistic anisotropic magnetoresistance (AMR). Single Co and Ir atoms are deposited on domains and domain walls of ferromagnetic Fe layers on W(110) to control their magnetization directions. They are contacted with nonmagnetic tips in a low-temperature scanning tunneling microscope to measure the junction conductances. Large changes of the magnetoresistance occur from the tunneling to the ballistic regime due to the competition of localized and delocalized d-orbitals, which are differently affected by spin-orbit coupling. This work shows that engineering the AMR at the single atom level is feasible.

Computer Series, 114: MO Theory Made Visible.

ERIC Educational Resources Information Center

Mealli, Carlo; Proserpio, Davide M.

1990-01-01

A collection of Molecular Orbital (MO) programs that have been integrated into routines and programs to illustrate MO theory are presented. Included are discussions of Computer Aided Composition of Atomic Orbitals (CACAO) and Walsh diagrams. (CW)

Self-Consistent-Field Calculation on Lithium Hydride for Undergraduates.

ERIC Educational Resources Information Center

Rioux, Frank; Harriss, Donald K.

1980-01-01

Describes a self-consistent-field-linear combination of atomic orbitals-molecular orbital calculation on the valence electrons of lithium hydride using the method of Roothaan. This description is intended for undergraduate physics students.

Surface passivation for tight-binding calculations of covalent solids.

PubMed

Bernstein, N

2007-07-04

Simulation of a cluster representing a finite portion of a larger covalently bonded system requires the passivation of the cluster surface. We compute the effects of an explicit hybrid orbital passivation (EHOP) on the atomic structure in a model bulk, three-dimensional, narrow gap semiconductor, which is very different from the wide gap, quasi-one-dimensional organic molecules where most passivation schemes have been studied in detail. The EHOP approach is directly applicable to minimal atomic orbital basis methods such as tight-binding. Each broken bond is passivated by a hybrid created from an explicitly expressed linear combination of basis orbitals, chosen to represent the contribution of the missing neighbour, e.g. a sp(3) hybrid for a single bond. The method is tested by computing the forces on atoms near a point defect as a function of cluster geometry. We show that, compared to alternatives such as pseudo-hydrogen passivation, the force on an atom converges to the correct bulk limit more quickly as a function of cluster radius, and that the force is more stable with respect to perturbations in the position of the cluster centre. The EHOP method also obviates the need for parameterizing the interactions between the system atoms and the passivating atoms. The method is useful for cluster calculations of non-periodic defects in large systems and for hybrid schemes that simulate large systems by treating finite regions with a quantum-mechanical model, coupled to an interatomic potential description of the rest of the system.

Surface passivation for tight-binding calculations of covalent solids

NASA Astrophysics Data System (ADS)

Bernstein, N.

2007-07-01

Simulation of a cluster representing a finite portion of a larger covalently bonded system requires the passivation of the cluster surface. We compute the effects of an explicit hybrid orbital passivation (EHOP) on the atomic structure in a model bulk, three-dimensional, narrow gap semiconductor, which is very different from the wide gap, quasi-one-dimensional organic molecules where most passivation schemes have been studied in detail. The EHOP approach is directly applicable to minimal atomic orbital basis methods such as tight-binding. Each broken bond is passivated by a hybrid created from an explicitly expressed linear combination of basis orbitals, chosen to represent the contribution of the missing neighbour, e.g. a sp3 hybrid for a single bond. The method is tested by computing the forces on atoms near a point defect as a function of cluster geometry. We show that, compared to alternatives such as pseudo-hydrogen passivation, the force on an atom converges to the correct bulk limit more quickly as a function of cluster radius, and that the force is more stable with respect to perturbations in the position of the cluster centre. The EHOP method also obviates the need for parameterizing the interactions between the system atoms and the passivating atoms. The method is useful for cluster calculations of non-periodic defects in large systems and for hybrid schemes that simulate large systems by treating finite regions with a quantum-mechanical model, coupled to an interatomic potential description of the rest of the system.

Observation of topological states in an optical Raman lattice with ultracold fermions

NASA Astrophysics Data System (ADS)

Song, Bo; He, Chengdong; Zhang, Long; Poon, Ting Fung Jeffrey; Hajiyev, Elnur; Ren, Zejian; Seo, Bojeong; Zhang, Shanchao; Liu, Xiong-Jun; Jo, Gyu-Boong

2017-04-01

The spin-orbit coupling with cold atoms, especially in optical lattices, provides a versatile platform to investigate the intriguing topological matters. In this talk, we will present the realization of one-dimensional spin-dependent lattice dressed by the periodic Raman field. Ultracold 173Yb fermions loaded into an optical Raman lattice reveal non-trivial spin textures due to the band topology, by which we measured topological invariants and determined a topological phase transition. In addition, we explored the non-equilibrium quench dynamics between the topological and the trivial states by suddenly changing the band topology of the optical Raman lattice. The optical Raman lattice demonstrated here opens a new avenue to study the spin-orbit coupling physics and furthermore to realize novel quantum matters such as symmetry-protected topological states. Funded by Croucher Foundation and Research Grants Council (RGC) of Hong Kong (Project ECS26300014, GRF16300215, GRF16311516, and Croucher Innovation Grants); MOST (Grant No. 2016YFA0301604) and NSFC (No. 11574008).

The Rubidium Atomic Clock and Basic Research

DTIC Science & Technology

2007-12-10

from orbiting GPS (global positioning system) satellites. Thankfully, you make it home without an exciting but har- rowing story to tell family...the vapor-cell atomic clock, -i\\till is elec- tronically tied to an atomic resonance, thereby transferring the stability of atomic structure to the...are applied to the resonance cell, there is a net transfer of atoms from F = 1 back into F = 2 and a decrease in transmitted light intensity. The

Lattice structures and electronic properties of MO/MoSe2 interface from first-principles calculations

NASA Astrophysics Data System (ADS)

Zhang, Yu; Tang, Fu-Ling; Xue, Hong-Tao; Lu, Wen-Jiang; Liu, Jiang-Fei; Huang, Min

2015-02-01

Using first-principles plane-wave calculations within density functional theory, we theoretically studied the atomic structure, bonding energy and electronic properties of the perfect Mo (110)/MoSe2 (100) interface with a lattice mismatch less than 4.2%. Compared with the perfect structure, the interface is somewhat relaxed, and its atomic positions and bond lengths change slightly. The calculated interface bonding energy is about -1.2 J/m2, indicating that this interface is very stable. The MoSe2 layer on the interface has some interface states near the Fermi level, the interface states are mainly caused by Mo 4d orbitals, while the Se atom almost have no contribution. On the interface, Mo-5s and Se-4p orbitals hybridize at about -6.5 to -5.0 eV, and Mo-4d and Se-4p orbitals hybridize at about -5.0 to -1.0 eV. These hybridizations greatly improve the bonding ability of Mo and Se atom in the interface. By Bader charge analysis, we find electron redistribution near the interface which promotes the bonding of the Mo and MoSe2 layer.

Low Earth orbit atomic oxygen simulation for durability evaluation of solar reflector surfaces

NASA Technical Reports Server (NTRS)

Degroh, Kim K.; Banks, Bruce A.

1992-01-01

To evaluate the performance and durability of solar reflector surfaces in the atomic oxygen environment typical of low Earth orbit (LEO), one must expose the reflector surface either directly to LEO or to ground-laboratory atomic oxygen environments. Although actual LEO exposures are most desired, such opportunities are typically scarce, expensive, and of limited duration. As a result, ground-laboratory exposures must be relied upon as the most practical long-term durability evaluation technique. Plasma ashers are widely used as LEO simulation facilities by producing atomic oxygen environments for durability evaluation of potential spacecraft materials. Atomic oxygen arrival differs between ground and space exposure in that plasma asher exposure produces isotropic arrival and space solar tracking produces sweeping arrival. Differences in initial impact reaction probability occur, dependent upon the energy and species existing in these environments. Due to the variations in ground-laboratory and space atomic oxygen, quantification of in-space performance based on plasma asher testing is not straightforward. The various atomic oxygen interactions that can occur with reflector surfaces, such as undercutting in organic substrates at protective coating defect sites, ground-laboratory techniques recommended for evaluating the atomic oxygen durability of reflectors based on asher exposures, and computational techniques which make use of ground-laboratory atomic oxygen exposure to predict in-space LEO durability are addressed.

Sensitive Technique Developed Using Atomic Force Microscopy to Measure the Low-Earth-Orbit Atomic Oxygen Erosion of Polymers

NASA Technical Reports Server (NTRS)

deGroh, Kim D.; Banks, Bruce A.; Clark, Gregory W.; Hammerstrom, Anne; Youngstrom, Erica; Kaminski, Carolyn; Fine, Elizabeth; Marx, Laura

2001-01-01

A recession measurement technique has been developed at the NASA Glenn Research Center to determine the atomic oxygen durability of polymers exposed to the space environment for short durations. Polymers such as polyimide Kapton and Teflon FEP (fluorinated ethylene propylene, DuPont) are commonly used in spacecraft because of their desirable properties, such as flexibility, low density, and in the case of FEP, low solar absorptance and high thermal emittance. Polymers on the exterior of spacecraft in the low- Earth-orbit environment are exposed to energetic atomic oxygen, resulting in erosion and potential structural loss. It is, therefore, important to understand the atomic oxygen erosion yield (E, the volume loss per incident oxygen atom) of polymers being considered in spacecraft design. Because long-term space exposure data are rare and very costly, short-term exposures, such as on the space shuttles, are often relied on for atomic oxygen erosion determination. The most common technique for determining E is through mass-loss measurements. For limited-duration exposure experiments, such as shuttle flight experiments, the atomic oxygen fluence is often so small that mass-loss measurements are not sensitive enough. Therefore, a recession measurement technique has been developed at Glenn to obtain accurate erosion yields of polymers exposed to low atomic oxygen fluences.

An accurate empirical method to predict the adsorption strength for π-orbital contained molecules on two dimensional materials.

PubMed

Li, Hongping; Wang, Changwei; Xun, Suhang; He, Jing; Jiang, Wei; Zhang, Ming; Zhu, Wenshuai; Li, Huaming

2018-06-01

To obtain the adsorption strength is the key point for materials design and parameters optimization in chemical engineering. Here we report a simple but accuracy method to estimate the adsorptive energies by counting the number of π-orbital involved atoms based on theoretical computations for hexagonal boron nitride (h-BN) and graphene. Computational results by density function theory (DFT) as well as spin-component scaled second-order Møller-Plesset perturbation theory (SCS-MP2) both confirm that the adsorptive energies correlate well with the number of π-orbital involved atoms for π-orbital contained molecules. The selected molecules (adsorbates) are commonly used in chemical industry, which contains C, N, S, O atoms. The predicted results for the proposed formulas agree well with the current and previous DFT calculated values both on h-BN and graphene surfaces. Further, it can be also used to predict the adsorptive energies for small π-orbital contained molecules on BN and carbon nanotubes. The interaction type for these adsorptions is typical π-π interaction. Further investigations show that the physical origin of these interactions source from the polar interactions between the adsorbents and adsorbates. Hence, for separation or removal of aromatic molecules, how to modify the aromaticity and polarity of both adsorbents and adsorbates will be the key points for experiments. Copyright © 2018 Elsevier Inc. All rights reserved.

Photonic orbital angular momentum in starlight. Further analysis of the 2011 Starfire Optical Range Observations

NASA Astrophysics Data System (ADS)

Oesch, Denis W.; Sanchez, Darryl J.

2014-07-01

Context. Each attempt by the Atmospheric Simulation and Adaptive-optics Laboratory Testbed (ASALT) research group to detect turbulence-induced photonic orbital angular momentum (POAM) has been successful, spanning laboratory, simulation and field experiments, with the possible exception of the 2011 Starfire Optical Range (SOR) astronomical observations, a search for POAM induced by astronomical sources. Aims: The purposes of this work are to discuss how POAM from astronomical turbulent assemblages of molecules or atoms (TAMA) would appear in observations and then to reanalyze the data from the 2011 SOR observations using a more refined technique as a demonstration of POAM in starlight. Methods: This work uses the method of projections used previously in analysis of terrestrial data. Results: Using the method of projections, the noise floor of the system was reevaluated and is found to be no greater than 1%. Reevaluation of the 2011 SOR observations reveals that a POAM signal is evident in all of the data. Conclusions: POAM signals have been found in every instance of extended propagation through turbulence conducted by the ASALT research group, including the 2011 SOR observations. POAM is an inevitable result of the propagation of optical waves through turbulence. We express our gratitude to the Air Force Office of Scientific Research for their support of this research.

Colorado Ultraviolet Transit Experiment: a dedicated CubeSat mission to study exoplanetary mass loss and magnetic fields

NASA Astrophysics Data System (ADS)

Fleming, Brian T.; France, Kevin; Nell, Nicholas; Kohnert, Richard; Pool, Kelsey; Egan, Arika; Fossati, Luca; Koskinen, Tommi; Vidotto, Aline A.; Hoadley, Keri; Desert, Jean-Michel; Beasley, Matthew; Petit, Pascal M.

2018-01-01

The Colorado Ultraviolet Transit Experiment (CUTE) is a near-UV (2550 to 3300 Å) 6U CubeSat mission designed to monitor transiting hot Jupiters to quantify their atmospheric mass loss and magnetic fields. CUTE will probe both atomic (Mg and Fe) and molecular (OH) lines for evidence of enhanced transit absorption, and to search for evidence of early ingress due to bow shocks ahead of the planet's orbital motion. As a dedicated mission, CUTE will observe ≳100 spectroscopic transits of hot Jupiters over a nominal 7-month mission. This represents the equivalent of >700 orbits of the only other instrument capable of these measurements, the Hubble Space Telescope. CUTE efficiently utilizes the available CubeSat volume by means of an innovative optical design to achieve a projected effective area of ˜28 cm2, low instrumental background, and a spectral resolving power of R˜3000 over the primary science bandpass. These performance characteristics enable CUTE to discern transit depths between 0.1% and 1% in individual spectral absorption lines. We present the CUTE optical and mechanical design, a summary of the science motivation and expected results, and an overview of the projected fabrication, calibration, and launch timeline.

Orbital debris removal and salvage system

NASA Technical Reports Server (NTRS)

1990-01-01

Four Texas A&M University projects are discussed. The first project is a design to eliminate a majority of orbital debris. The Orbital Debris and Salvage System will push the smaller particles into lower orbits where their orbits will decay at a higher rate. This will be done by momentum transfer via laser. The salvageable satellites will be delivered to the Space Station by an Orbital Transfer Vehicle. The rest of the debris will be collected by Salvage I. The second project is the design of a space based satellite system to prevent the depletion of atmospheric ozone. The focus is on ozone depletion in the Antarctic. The plan is to use an orbiting solar array system designed to transmit microwaves at a frequency of 22 GHz over the region in order to dissipate polar stratospheric clouds that form during the months beginning in August and ending in October. The third project, Project Poseidon, involves a conceptual design of a space based hurricane control system consisting of a network of 21 low-orbiting laser platforms arranged in three rings designed to heat the upper atmosphere of a developing tropical depression. Fusion power plants are proposed to provide power for the lasers. The fourth project, Project Donatello, involves a proposed Mars exploration initiative for the year 2050. The project is a conceptual design for a futuristic superfreighter that will transport large numbers of people and supplies to Mars for the construction of a full scale scientific and manufacturing complex.

X-ray photoelectron spectroscopic study of sulfur-nitrogen-fluorine compounds

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

Beach, D.B.; Jolly, W.L.; Mews, R.

1984-11-21

The gas-phase core binding energies of NSF, NSF/sub 3/, and several compounds of the types NSF/sub 2/R and F/sub 2/SNR have been determined. Qualitative interpretation of the data shows that N(p..pi..) ..-->.. S(d..pi..) bonding is probably important in the NSF/sub 2/R compounds and in NSF/sub 3/, that the bonding of the sulfur atom in NSF is similar to that in SO/sub 2/, and that the nitrogen atom of NSF/sub 3/ is more negatively charged than that of NSF (in spite of a stronger N-S bond in NSF/sub 3/). Quantitative interpretation of the data for NSF and NSF/sub 3/, together withmore » literature valence ionization potentials, shows that the HOMO of each molecule has principally nitrogen 2p character and is stabilized by interaction with a higher lying sulfur 3d orbital. The approximate atomic orbital contributions to the other molecuar orbitals of these molecules are deduced.« less

Atomic oxygen interaction with spacecraft materials: Relationship between orbital and ground-based testing for materials certification

NASA Technical Reports Server (NTRS)

Cross, Jon B.; Koontz, Steven L.; Lan, Esther H.

1993-01-01

The effects of atomic oxygen on boron nitride (BN), silicon nitride (Si3N4), Intelsat 6 solar cell interconnects, organic polymers, and MoS2 and WS2 dry lubricant, were studied in Low Earth Orbit (LEO) flight experiments and in a ground based simulation facility. Both the inflight and ground based experiments employed in situ electrical resistance measurements to detect penetration of atomic oxygen through materials and Electron Spectroscopy for Chemical Analysis (ESCA) analysis to measure chemical composition changes. Results are given. The ground based results on the materials studied to date show good qualitative correlation with the LEO flight results, thus validating the simulation fidelity of the ground based facility in terms of reproducing LEO flight results. In addition it was demonstrated that ground based simulation is capable of performing more detailed experiments than orbital exposures can presently perform. This allows the development of a fundamental understanding of the mechanisms involved in the LEO environment degradation of materials.

Tunable Spin-orbit Coupling and Quantum Phase Transition in a Trapped Bose-Einstein Condensate

PubMed Central

Zhang, Yongping; Chen, Gang; Zhang, Chuanwei

2013-01-01

Spin-orbit coupling (SOC), the intrinsic interaction between a particle spin and its motion, is responsible for various important phenomena, ranging from atomic fine structure to topological condensed matter physics. The recent experimental breakthrough on the realization of SOC for ultra-cold atoms provides a completely new platform for exploring spin-orbit coupled superfluid physics. However, the SOC strength in the experiment is not tunable. In this report, we propose a scheme for tuning the SOC strength through a fast and coherent modulation of the laser intensities. We show that the many-body interaction between atoms, together with the tunable SOC, can drive a quantum phase transition (QPT) from spin-balanced to spin-polarized ground states in a harmonic trapped Bose-Einstein condensate (BEC), which resembles the long-sought Dicke QPT. We characterize the QPT using the periods of collective oscillations of the BEC, which show pronounced peaks and damping around the quantum critical point. PMID:23727689

Degradation mechanisms of materials for large space systems in low Earth orbit

NASA Technical Reports Server (NTRS)

Gordon, William L.; Hoffman, R. W.

1987-01-01

Degradation was explored of various materials used in aerospace vehicles after severe loss of polymeric material coatings (Kapton) was observed on an early shuttle flight in low Earth orbit. Since atomic oxygen is the major component of the atmosphere at 300 km, and the shuttle's orbital velocity produced relative motion corresponding to approx. 5 eV of oxygen energy, it was natural to attribute much of this degradation to oxygen interaction. This assumption was tested using large volume vacuum systems and ion beam sources, in an exploratory effort to produce atomic oxygen of the appropriate energy, and to observe mass loss from various samples as well as optical radiation. Several investigations were initiated and the results of these investigations are presented in four papers. These papers are summarized. They are entitled: (1) The Space Shuttle Glow; (2) Laboratory Degradation of Kapton in a Low Energy Oxygen Ion Beam; (3) The Energy Dependence and Surface Morphology of Kapton Degradation Under Atomic Oxygen Bombardment; and (4) Surface Analysis of STS 8 Samples.

Photoabsorption of the molecular IH cation at the iodine 3 d absorption edge

NASA Astrophysics Data System (ADS)

Klumpp, Stephan; Guda, Alexander A.; Schubert, Kaja; Mertens, Karolin; Hellhund, Jonas; Müller, Alfred; Schippers, Stefan; Bari, Sadia; Martins, Michael

2018-03-01

Yields of atomic iodine Iq + (q ≥2 ) fragments resulting from photoexcitation and photoionization of the target ions IH+ and I+ have been measured in the photon-energy range 610-680 eV, which comprises the thresholds for iodine 3 d ionization. The measured ion-yield spectra show two strong and broad resonance features due to the excitation of the 3 d3 /2 ,5 /2 electrons into ɛ f states rather similar for both parent ions. In the 3 d pre-edge range, excitations into (n p π ) -like orbitals and into an additional σ* orbital are found for IH+, which have been identified by comparison of the atomic I+ and molecular IH+ data and with the help of (time-dependent) density functional theory (DFT) and atomic Hartree-Fock calculations. The (5 p π ) orbital is almost atomlike, whereas all other resonances of the IH+ primary ion show a more pronounced molecular character, which is deduced from the chemical shifts of the resonances and the theoretical analysis.

NH3 molecule adsorption on spinel-type ZnFe2O4 surface: A DFT and experimental comparison study

NASA Astrophysics Data System (ADS)

Zou, Cong-yang; Ji, Wenchao; Shen, Zhemin; Tang, Qingli; Fan, Maohong

2018-06-01

Ammonia (NH3) is a caustic environment pollutant which contributes to haze formation and water pollution. Zinc ferrite (ZnFe2O4) exhibits good catalytic activity in NH3 removal. The density functional theory (DFT) was applied to explore the interaction mechanism of NH3 molecule adsorption on spinel-type ZnFe2O4 (1 1 0) surface with GGA-PW91 method in atomic and electronic level. The results indicated that NH3 molecule preferred to adsorb on surface Zn atom with the formation of H3Nsbnd Zn coordinate bond over ZnFe2O4 (1 1 0) surface. The H3Nsbnd Zn state was exothermic process with adsorption energy of -203.125 kJ/mol. About 0.157e were transferred from NH3 molecule to the surface which resulted in strong interaction. Higher activation degree occurred in H3Nsbnd Zn configuration with two Nsbnd H bonds elongated and NH3 structure became more flat on the surface. The PDOS change of NH3 molecule was consistent with the result of adsorption energy. It was concluded that s orbital of NH3 (N) and s, p orbitals of Zn atom overlapped at -0.619 Ha. The p orbital of NH3 (N) has interaction with d orbital of Zn atom suggesting the hybridization between them. Based on NH3 removal experimental and XPS spectra results, NH3sbnd ZnFe2O4 interaction was mainly depended on the coordination between Zn atom and NH3 molecule. The DFT calculations have deepened our understanding on NH3sbnd ZnFe2O4 interaction system.

Electronic structure, magnetism, and optical properties of Fe2SiO4 fayalite at ambient and high pressures: A GGA+U study

NASA Astrophysics Data System (ADS)

Jiang, Xuefan; Guo, G. Y.

2004-04-01

The electronic structure, magnetism, and optical properties of Fe2SiO4 fayalite, the iron-rich end member of the olivine-type silicate, one of the most abundant minerals in Earth’s upper mantle, have been studied by density-functional theory within the generalized gradient approximation (GGA) with the on-site Coulomb energy U=4.5 eV taken into account (GGA+U). The stable insulating antiferromagnetic solution with an energy gap ˜1.49 eV and a spin magnetic moment of 3.65μB and an orbital magnetic moment of 0.044μB per iron atom is obtained. It is found that the gap opening in this fayalite results mainly from the strong on-site Coulomb interaction on the iron atoms. In this band structure, the top of valence bands consists mainly of the 3d orbitals of Fe2 atoms, and the bottom of the conduction bands is mainly composed of the 3d orbitals of Fe1 atoms. Therefore, since the electronic transition from the Fe2 3d to Fe1 3d states is weak, significant electronic transitions would appear only about 1 eV above the absorption edge when Fe-O orbitals are involved in the final states. In addition, our band-structure calculations can explain the observed phenomena including redshift near the absorption edge and the decrease of the electrical resistivity of Fe2SiO4 upon compression. The calculated Fe p partial density of states agree well with Fe K-edge x-ray absorption spectrum. The calculated lattice constants and atomic coordinates for Fe2SiO4 fayalite in orthorhombic structure are in good agreement with experiments.

Apollo Soyuz Test Project Commemorative plaque in orbit

NASA Image and Video Library

1975-07-17

AST-05-263 (17-18 July 1975) --- The Apollo-Soyuz Test Project (ASTP) Commemorative Plaque is assembled in the Soviet Soyuz Orbital Module during the joint U.S.-USSR Apollo-Soyuz Test Project docking mission in Earth orbit. The plaque is written both in English and Russian.

Beads + String = Atoms You Can See.

ERIC Educational Resources Information Center

Hermann, Christine K. F.

1998-01-01

Presents hands-on activities that give students a head start in learning the vocabulary and basic theory involved in understanding atomic structure. Uses beads to represent protons, neutrons, and electrons and string to represent orbitals. (DDR)

Wigner time delay and spin-orbit activated confinement resonances

NASA Astrophysics Data System (ADS)

Keating, D. A.; Deshmukh, P. C.; Manson, S. T.

2017-09-01

A study of the photoionization of spin-orbit split subshells of high-Z atoms confined in C60 has been performed using the relativistic-random-phase approximation. Specifically, Hg@C60 5p, Rn@C60 6p and Ra@C60 5d were investigated and the near-threshold confinement resonances in the j = l - 1/2 channels were found to engender structures in the j = l + 1/2 cross sections via correlation in the form of interchannel coupling. These structures are termed spin-orbit induced confinement resonances and they are found to profoundly influence the Wigner time delay spectrum resulting in time delays of tens or hundreds of attoseconds along with dramatic swings in time delay over small energy intervals. Pronounced relativistic effects in time delay are also found. These structures, including their manifestation in time delay spectra, are expected to be general phenomena in the photoionization of spin-orbit doublets in confined high-Z atoms.

Massive Gas Cloud Around Jupiter

NASA Technical Reports Server (NTRS)

2003-01-01

An innovative instrument on NASA's Cassini spacecraft makes the space environment around Jupiter visible, revealing a donut-shaped gas cloud encircling the planet.

The image was taken with the energetic neutral atom imaging technique by the Magnetospheric Imaging Instrument on Cassini as the spacecraft flew past Jupiter in early 2001 at a distance of about 10 million kilometers (6 million miles). This technique provides information about a source by detecting neutral atoms emitted by the source, comparable to how a camera reveals information about an object by detecting photons coming from the object.

The central object in this image represents energetic neutral atom emissions from Jupiter itself. The outer two objects represent emissions from a donut-shaped cloud, or torus, that shares an orbit with Jupiter's moon Europa. The cloud's emissions appear dot-like because of the viewing angle. The torus is viewed edge-on, and the image is brightest at the line-of-sight angles that pass through the greatest volume of it.

Cassini is a cooperative project of NASA, the European Space Agency and the Italian Space Agency. The Jet Propulsion Laboratory, a division of the California Institute of Technology in Pasadena, Calif., manages Cassini for NASA's Office of Space Science, Washington, D.C.

Atomic research

NASA Technical Reports Server (NTRS)

Hadaway, James B.; Connatser, Robert; Cothren, Bobby; Johnson, R. B.

1993-01-01

Work performed by the University of Alabama in Huntsville's (UAH) Center for Applied Optics (CAO) entitled Atomic Research is documented. Atomic oxygen (AO) effects on materials have long been a critical concern in designing spacecraft to withstand exposure to the Low Earth Orbit (LEO) environment. The objective of this research effort was to provide technical expertise in the design of instrumentation and experimental techniques for analyzing materials exposed to atomic oxygen in accelerated testing at NASA/MSFC. Such testing was required to answer fundamental questions concerning Space Station Freedom (SSF) candidate materials and materials exposed to atomic oxygen aboard the Long-Duration Exposure Facility (LDEF). The primary UAH task was to provide technical design, review, and analysis to MSFC in the development of a state-of-the-art 5eV atomic oxygen beam facility required to simulate the RAM-induced low earth orbit (LEO) AO environment. This development was to be accomplished primarily at NASA/MSFC. In support of this task, contamination effects and ultraviolet (UV) simulation testing was also to be carried out using NASA/MSFC facilities. Any materials analysis of LDEF samples was to be accomplished at UAH.

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

Jiang, Zhuoling; Wang, Hao; Sanvito, Stefano

Inelastic electron tunneling spectroscopy (IETS) of a single hydrogen atom on the Cu(100) surface in a scanning tunneling microscopy (STM) configuration has been investigated by employing the non-equilibrium Green’s function formalism combined with density functional theory. The electron-vibration interaction is treated at the level of lowest order expansion. Our calculations show that the single peak observed in the previous STM-IETS experiments is dominated by the perpendicular mode of the adsorbed H atom, while the parallel one only makes a negligible contribution even when the STM tip is laterally displaced from the top position of the H atom. This propensity ofmore » the IETS is deeply rooted in the symmetry of the vibrational modes and the characteristics of the conduction channel of the Cu-H-Cu tunneling junction, which is mainly composed of the 4s and 4p{sub z} atomic orbitals of the Cu apex atom and the 1s orbital of the adsorbed H atom. These findings are helpful for deepening our understanding of the propensity rules for IETS and promoting IETS as a more popular spectroscopic tool for molecular devices.« less

Materials samples face rigors of space.

PubMed

Flinn, Edward D

2002-07-01

The Materials International Space Station Experiment (MISSE) is described. This project is designed to conduct long duration materials tests on samples attached to the ISS. A batch of 750 material samples were delivered on STS-105 and attached to the ISS airlock. They will be exposed to the space environment for 18 months and are slated to return on STS-114. A second batch of 750 samples is being prepared. The experiment containers were used originally for the Mir Environmental Effects Payload, which tested a variety of substances, including some slated for use on the ISS. Researchers are particularly interested in the effects of atomic oxygen on the samples. Some samples are being tested to determine their use in radiation protection. As part of the MISSE project, ultrathin tether materials are being tested for use on the Propulsive Small Expendable Depoloyer System (ProSEDS), which will use a tether system to change a satellite's orbital altitude.

Testing general relativity and alternative theories of gravity with space-based atomic clocks and atom interferometers

NASA Astrophysics Data System (ADS)

Bondarescu, Ruxandra; Schärer, Andreas; Jetzer, Philippe; Angélil, Raymond; Saha, Prasenjit; Lundgren, Andrew

2015-05-01

The successful miniaturisation of extremely accurate atomic clocks and atom interferometers invites prospects for satellite missions to perform precision experiments. We discuss the effects predicted by general relativity and alternative theories of gravity that can be detected by a clock, which orbits the Earth. Our experiment relies on the precise tracking of the spacecraft using its observed tick-rate. The spacecraft's reconstructed four-dimensional trajectory will reveal the nature of gravitational perturbations in Earth's gravitational field, potentially differentiating between different theories of gravity. This mission can measure multiple relativistic effects all during the course of a single experiment, and constrain the Parametrized Post-Newtonian Parameters around the Earth. A satellite carrying a clock of fractional timing inaccuracy of Δ f / f ˜ 10-16 in an elliptic orbit around the Earth would constrain the PPN parameters |β - 1|, |γ - 1| ≲ 10-6. We also briefly review potential constraints by atom interferometers on scalar tensor theories and in particular on Chameleon and dilaton models.

Disparate ultrafast dynamics of itinerant and localized magnetic moments in gadolinium metal

PubMed Central

Frietsch, B.; Bowlan, J.; Carley, R.; Teichmann, M.; Wienholdt, S.; Hinzke, D.; Nowak, U.; Carva, K.; Oppeneer, P. M.; Weinelt, M.

2015-01-01

The Heisenberg–Dirac intra-atomic exchange coupling is responsible for the formation of the atomic spin moment and thus the strongest interaction in magnetism. Therefore, it is generally assumed that intra-atomic exchange leads to a quasi-instantaneous aligning process in the magnetic moment dynamics of spins in separate, on-site atomic orbitals. Following ultrashort optical excitation of gadolinium metal, we concurrently record in photoemission the 4f magnetic linear dichroism and 5d exchange splitting. Their dynamics differ by one order of magnitude, with decay constants of 14 versus 0.8 ps, respectively. Spin dynamics simulations based on an orbital-resolved Heisenberg Hamiltonian combined with first-principles calculations explain the particular dynamics of 5d and 4f spin moments well, and corroborate that the 5d exchange splitting traces closely the 5d spin-moment dynamics. Thus gadolinium shows disparate dynamics of the localized 4f and the itinerant 5d spin moments, demonstrating a breakdown of their intra-atomic exchange alignment on a picosecond timescale. PMID:26355196

Tables Of Gaussian-Type Orbital Basis Functions

NASA Technical Reports Server (NTRS)

Partridge, Harry

1992-01-01

NASA technical memorandum contains tables of estimated Hartree-Fock wave functions for atoms lithium through neon and potassium through krypton. Sets contain optimized Gaussian-type orbital exponents and coefficients, and near Hartree-Fock quality. Orbital exponents optimized by minimizing restricted Hartree-Fock energy via scaled Newton-Raphson scheme in which Hessian evaluated numerically by use of analytically determined gradients.

The role of terminations and coordination atoms on the pseudocapacitance of titanium carbonitride monolayers.

PubMed

Zhang, Wenqiang; Cheng, Chuan; Fang, Peilin; Tang, Bin; Zhang, Jindou; Huang, Guoming; Cong, Xin; Zhang, Bao; Ji, Xiao; Miao, Ling

2016-02-14

Nowadays, MXenes have received extensive concern as a prominent electrode material of electrochemical capacitors. As two important factors to the capacitance, the influence of the intrinsical terminations (F, O and OH) and coordination atoms (C and N) is investigated using first-principles calculations. According to the density of states aligned with the standard hydrogen electrode, it turns out that a Ti3CNO2 monolayer is proven to show an obvious pseudocapacitive behavior, while the bare, F and OH terminated Ti3CN monolayers may only present electrochemical double layer characters in an aqueous electrolyte. Moreover, the illustration of molecular orbitals over the Fermi level are mainly contributed by the d-orbitals of Ti atoms coordinated with O and N atoms, indicating that the redox pseudocapacitance of the Ti3CNO2 monolayer is promoted by the coordination N atoms. Then the superiority of N bonded Ti atoms in accepting charges can be visualized through the charge population. Further, the larger ratio of C/N in the coordination environment of Ti atoms indicates that more electrons can be stored. Our investigation can give an instructional advice in the MXenes-electrode production.

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

Schlagmüller, Michael; Liebisch, Tara Cubel; Engel, Felix

Within a dense environment (ρ ≈ 10 14 atoms/cm 3) at ultracold temperatures (T < 1 μK), a single atom excited to a Rydberg state acts as a reaction center for surrounding neutral atoms. At these temperatures, almost all neutral atoms within the Rydberg orbit are bound to the Rydberg core and interact with the Rydberg atom. We have studied the reaction rate and products for nS 87Rb Rydberg states, and we mainly observe a state change of the Rydberg electron to a high orbital angular momentum l, with the released energy being converted into kinetic energy of the Rydberg atom. Unexpectedly, the measurements show a threshold behavior at n ≈ 100 for the inelastic collision time leading to increased lifetimes of the Rydberg state independent of the densities investigated. Even at very high densities (ρ ≈ 4.8 x 10 14 cm -3), the lifetime of a Rydberg atom exceeds 10 μs at n > 140 compared to 1 μs at n = 90. In addition, a second observed reaction mechanism, namely, Rbmore » $$+\\atop{2}$$ molecule formation, was studied. Both reaction products are equally probable for n = 40, but the fraction of Rb + 2 created drops to below 10% for n ≥ 90.« less

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

Finzel, Kati, E-mail: kati.finzel@liu.se

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

Interaction of Rydberg atoms in circular states with the alkaline-earth Ca(4s{sup 2}) and Sr(5s{sup 2}) atoms

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

Mironchuk, E. S.; Narits, A. A.; Lebedev, V. S., E-mail: vlebedev@sci.lebedev.ru

2015-11-15

The resonant mechanism of interaction of alkaline-earth atoms having a low electron affinity to Rydberg atoms in circular (l = vertical bar m vertical bar = n–1) and near-circular states has been studied. To describe the dynamics of resonant processes accompanied by nonadiabatic transitions between ionic and Rydberg covalent terms of a quasimolecule, an approach based on the integration of coupled equations for the probability amplitudes has been developed taking into account the possibility of the decay of an anion in the Coulomb field of the positive ionic core of a highly excited atom. The approach involves the specific featuresmore » of the problem associated with the structure of the wavefunction of a Rydberg electron in states with high orbital angular momenta l ∼ n–1. This approach provides a much more accurate description of the dynamics of electronic transitions at collisions between atoms than that within the modified semiclassical Landau–Zener model. In addition, this approach makes it possible to effectively take into account many channels of the problem. The cross sections for resonant quenching of Rydberg states of the Li(nlm) atom with given principal n, orbital l = n–1, and magnetic m quantum numbers at thermal collisions with the Ca(4s{sup 2}) and Sr(5s{sup 2}) atoms have been calculated. The dependences of the results on n, m, and angle α between the relative velocity of the atoms and the normal to the plane of the orbit of the Rydberg electron have been obtained. The influence of orientational effects on the efficiency of the collisional destruction of circular and near-circular states has been studied. The results indicate a higher stability of such states to their perturbations by neutral particles as compared to usually studied nl states with low values of l (l ≪ n)« less

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

PubMed Central

Yang, Tao; Fukuda, Ryoichi; Hosokawa, Saburo; Tanaka, Tsunehiro

2017-01-01

Abstract Single‐atom catalysts have attracted much interest recently because of their excellent stability, high catalytic activity, and remarkable atom efficiency. Inspired by the recent experimental discovery of a highly efficient single‐atom catalyst Pd1/γ‐Al2O3, we conducted a comprehensive DFT study on geometries, stabilities and CO oxidation catalytic activities of M1/γ‐Al2O3 (M=Pd, Fe, Co, and Ni) by using slab‐model. One of the most important results here is that Ni1/Al2O3 catalyst exhibits higher activity in CO oxidation than Pd1/Al2O3. The CO oxidation occurs through the Mars van Krevelen mechanism, the rate‐determining step of which is the generation of CO2 from CO through abstraction of surface oxygen. The projected density of states (PDOS) of 2p orbitals of the surface O, the structure of CO‐adsorbed surface, charge polarization of CO and charge transfer from CO to surface are important factors for these catalysts. Although the binding energies of Fe and Co with Al2O3 are very large, those of Pd and Ni are small, indicating that the neighboring O atom is not strongly bound to Pd and Ni, which leads to an enhancement of the reactivity of the O atom toward CO. The metal oxidation state is suggested to be one of the crucial factors for the observed catalytic activity. PMID:28515795

Consequences of Atomic Oxygen Interaction With Silicone and Silicone Contamination on Surfaces in Low Earth Orbit

NASA Technical Reports Server (NTRS)

Banks, Bruce A.; deGroh, Kim K.; Rutledge, Sharon K.; Haytas, Christy A.

1999-01-01

The exposure of silicones to atomic oxygen in low Earth orbit causes oxidation of the surface, resulting in conversion of silicone to silica. This chemical conversion increases the elastic modulus of the surface and initiates the development of a tensile strain. Ultimately, with sufficient exposure, tensile strain leads to cracking of the surface enabling the underlying unexposed silicone to be converted to silica resulting in additional depth and extent of cracking. The use of silicone coatings for the protection of materials from atomic oxygen attack is limited because of the eventual exposure of underlying unprotected polymeric material due to deep tensile stress cracking of the oxidized silicone. The use of moderate to high volatility silicones in low Earth orbit has resulted in a silicone contamination arrival at surfaces which are simultaneously being bombarded with atomic oxygen, thus leading to conversion of the silicone contaminant to silica. As a result of these processes, a gradual accumulation of contamination occurs leading to deposits which at times have been up to several microns thick (as in the case of a Mir solar array after 10 years in space). The contamination species typically consist of silicon, oxygen and carbon. which in the synergistic environment of atomic oxygen and UV radiation leads to increased solar absorptance and reduced solar transmittance. A comparison of the results of atomic oxygen interaction with silicones and silicone contamination will be presented based on the LDEF, EOIM-111, Offeq-3 spacecraft and Mir solar array in-space results. The design of a contamination pin-hole camera space experiment which uses atomic oxygen to produce an image of the sources of silicone contamination will also be presented.

Oxygen evolution on a SrFeO3 anode - Mechanistic considerations from molecular orbital theory

NASA Technical Reports Server (NTRS)

Mehandru, S. P.; Anderson, Alfred B.

1989-01-01

Various pathways proposed in the literature for the evolution of O2 in electrochemical oxidations are explored using the atom superposition and electron delocalization molecular orbital (ASED-MO) theory and the cluster models of the SrFeO3 surface as a prototype material. Calculations indicate that oxygen atoms can be easily formed on the (100) surface as well as on the edge cation sites of a SrFeO3 anode by the discharge of OH(-), followed by its deprotonation and electron transfer to the electrode. The O atoms can form O2 on the edge and corner sites, where the Fe(4+) is coordinated to four and three bulk oxygen anions, respectively. The calculations strongly disfavor mechanisms involving coupling of oxygen atoms adsorbed on different cations as well as a mechanism featuring an ozone intermediate.

High intensity 5 eV O-atom exposure facility for material degradation studies

NASA Technical Reports Server (NTRS)

Cross, J. B.; Spangler, L. H.; Hoffbauer, M. A.; Archuleta, F. A.; Leger, Lubert; Visentine, James; Hunton, Don E.; Cross, J. B.

1986-01-01

An atomic oxygen exposure facility was developed for studies of material degradation. The goal of these studies is to provide design criteria and information for the manufacture of long life (20 to 30 years) construction materials for use in low Earth orbit. The studies that are being undertaken will provide: (1) absolute reaction cross sections for the engineering design problems, (2) formulations of reaction mechanisms for use in the selection of suitable existing materials and the design of new more resistant ones, and (3) the calibration of flight hardware (mass spectrometers, etc.) in order to directly relate experiments performed in low Earth orbit to ground based investigations. The facility consists of a CW laser sustained discharge source of O-atoms, an atomic beam formation and diagnostics system, a spinning rotor viscometer, and provision for using the system for calibration of actual flight instruments.

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.

Proceedings of the NASA Workshop on Atomic Oxygen Effects. [low earth orbital environment

NASA Technical Reports Server (NTRS)

Brinza, David E. (Editor)

1987-01-01

A workshop was held to address the scientific issues concerning the effects of atomic oxygen on materials in the low Earth orbital (LEO) environment. The program included 18 invited speakers plus contributed posters covering topics such as LEO spaceflight experiments, interaction mechanisms, and atomic oxygen source development. Discussion sessions were also held to organize a test program to evaluate atomic oxygen exposure facilities. The key issues raised in the workshop were: (1) the need to develop a reliable predictive model of the effects of long-term exposure of materials to the LEO environment; (2) the ability of ground-based exposure facilities to provide useful data for development of durable materials; and (3) accurate determination of the composition of the LEO environment. These proceedings include the invited papers, the abstracts for the contributed posters, and an account of the test program discussion sessions.

The effect of d and f states of ytterbium on the electronic and magnetic properties of Al1‑xYbxN: DFT+U study

NASA Astrophysics Data System (ADS)

Belhachi, S.

2018-04-01

Using density functional theory combined LSDA+U method, the structural, electronic and magnetic behaviors of ytterbium implanted in wurtzite AlN were investigated. Low formation energy shows that Yb atom favors to substitute for Al site and to confirm this stability, the adsorption energy has been calculated. It is found that Al0.9375Yb0.0625N possesses a semiconductor behavior. The magnetic moment 0.9891 μB per molecule principally comes from Yb ion with small contribution from the Al and N atoms. We predict that Yb ions order ferromagnetically in AlN. The hybridization between the f orbital of the Yb atom and the p orbital of the N atom is also observed. We see that AlN:Yb will be among the good candidates for spintronic applications.

Reaction and Protection of Electrical Wire Insulators in Atomic-oxygen Environments

NASA Technical Reports Server (NTRS)

Hung, Ching-Cheh; Cantrell, Gidget

1994-01-01

Atomic-oxygen erosion on spacecraft in low Earth orbit is an issue which is becoming increasingly important because of the growing number of spacecraft that will fly in the orbits which have high concentrations of atomic oxygen. In this investigation, the atomic-oxygen durability of three types of electrical wire insulation (carbon-based, fluoropolymer, and polysiloxane elastomer) were evaluated. These insulation materials were exposed to thermal-energy atomic oxygen, which was obtained by RF excitation of air at a pressure of 11-20 Pa. The effects of atomic-oxygen exposure on insulation materials indicate that all carbon-based materials erode at about the same rate as polyamide Kapton and, therefore, are not atomic-oxygen durable. However, the durability of fluoropolymers needs to be evaluated on a case by case basis because the erosion rates of fluoropolymers vary widely. For example, experimental data suggest the formation of atomic fluorine during atomic-oxygen amorphous-fluorocarbon reactions. Dimethyl polysiloxanes (silicone) do not lose mass during atomic-oxygen exposure, but develop silica surfaces which are under tension and frequently crack as a result of loss of methyl groups. However, if the silicone sample surfaces were properly pretreated to provide a certain roughness, atomic oxygen exposure resulted in a sturdy, non-cracked atomic-oxygen durable SiO2 layer. Since the surface does not crack during such silicone-atomic oxygen reaction, the crack-induced contamination by silicone can be reduced or completely stopped. Therefore, with proper pretreatment, silicone can be either a wire insulation material or a coating on wire insulation materials to provide atomic-oxygen durability.

Steering Quantum States Towards Classical Bohr-Like Orbits

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

Dunning, F. B.; Reinhold, Carlos O; Yoshida, S.

2010-01-01

This article furnishes an introduction to the properties of time-dependent electronic wavefunctions in atoms and to physics at the interface between the quantum and classical worlds. We describe how, almost 100 years after the introduction of the Bohr model of the atom, it is now possible using pulsed electric fields to create in the laboratory localized wavepackets in high-n (n ~ 300) Rydberg atoms that travel in near-circular Bohr-like orbits mimicking the behavior of a classical electron. The control protocols employed are explained with the aid of quantum and classical dynamics. Remarkably, while many aspects of the underlying behavior canmore » be described using classical arguments, even at n ~ 300 purely quantum effects such as revivals can be seen.« less

Near Hartree-Fock quality GTO basis sets for the second-row atoms

NASA Technical Reports Server (NTRS)

Partridge, Harry

1987-01-01

Energy optimized, near Hartree-Fock quality Gaussian basis sets ranging in size from (17s12p) to (20s15p) are presented for the ground states of the second-row atoms for Na(2P), Na(+), Na(-), Mg(3P), P(-), S(-), and Cl(-). In addition, optimized supplementary functions are given for the ground state basis sets to describe the negative ions, and the excited Na(2P) and Mg(3P) atomic states. The ratios of successive orbital exponents describing the inner part of the 1s and 2p orbitals are found to be nearly independent of both nuclear charge and basis set size. This provides a method of obtaining good starting estimates for other basis set optimizations.

Ultracold Chemical Reactions of a Single Rydberg Atom in a Dense Gas

DOE PAGES

Schlagmüller, Michael; Liebisch, Tara Cubel; Engel, Felix; ...

2016-08-10

Within a dense environment (ρ ≈ 10 14 atoms/cm 3) at ultracold temperatures (T < 1 μK), a single atom excited to a Rydberg state acts as a reaction center for surrounding neutral atoms. At these temperatures, almost all neutral atoms within the Rydberg orbit are bound to the Rydberg core and interact with the Rydberg atom. We have studied the reaction rate and products for nS 87Rb Rydberg states, and we mainly observe a state change of the Rydberg electron to a high orbital angular momentum l, with the released energy being converted into kinetic energy of the Rydberg atom. Unexpectedly, the measurements show a threshold behavior at n ≈ 100 for the inelastic collision time leading to increased lifetimes of the Rydberg state independent of the densities investigated. Even at very high densities (ρ ≈ 4.8 x 10 14 cm -3), the lifetime of a Rydberg atom exceeds 10 μs at n > 140 compared to 1 μs at n = 90. In addition, a second observed reaction mechanism, namely, Rbmore » $$+\\atop{2}$$ molecule formation, was studied. Both reaction products are equally probable for n = 40, but the fraction of Rb + 2 created drops to below 10% for n ≥ 90.« less

Low Earth Orbital Atomic Oxygen Interactions With Materials

NASA Technical Reports Server (NTRS)

Banks, Bruce A.; Miller, Sharon K.; deGroh, Kim K.

2004-01-01

Atomic oxygen is formed in the low Earth orbital environment (LEO) by photo dissociation of diatomic oxygen by short wavelength (< 243 nm) solar radiation which has sufficient energy to break the 5.12 eV O2 diatomic bond in an environment where the mean free path is sufficiently long ( 108 meters) that the probability of reassociation or the formation of ozone (O3) is small. As a consequence, between the altitudes of 180 and 650 km, atomic oxygen is the most abundant species. Spacecraft impact the atomic oxygen resident in LEO with sufficient energy to break hydrocarbon polymer bonds, causing oxidation and thinning of the polymers due to loss of volatile oxidation products. Mitigation techniques, such as the development of materials with improved durability to atomic oxygen attack, as well as atomic oxygen protective coatings, have been employed with varying degrees of success to improve durability of polymers in the LEO environment. Atomic oxygen can also oxidize silicones and silicone contamination to produce non-volatile silica deposits. Such contaminants are present on most LEO missions and can be a threat to performance of optical surfaces. The LEO atomic oxygen environment, its interactions with materials, results of space testing, computational modeling, mitigation techniques, and ground laboratory simulation procedures and issues are presented.

Atomic oxygen effects on materials

NASA Technical Reports Server (NTRS)

Banks, Bruce A.; Rutledge, Sharon K.; Brady, Joyce A.; Merrow, James E.

1989-01-01

Understanding of the basic processes of atomic oxygen interaction is currently at a very elementary level. However, measurement of erosion yields, surface morphology, and optical properties for low fluences have brought about much progress in the past decade. Understanding the mechanisms and those factors that are important for proper simulation of low Earth orbit is at a much lower level of understanding. The ability to use laboratory simulations with confidence to quantifiably address the functional performance and durability of materials in low Earth orbit will be necessary to assure long-term survivability to the natural space environment.

Measuring qutrit-qutrit entanglement of orbital angular momentum states of an atomic ensemble and a photon.

PubMed

Inoue, R; Yonehara, T; Miyamoto, Y; Koashi, M; Kozuma, M

2009-09-11

Three-dimensional entanglement of orbital angular momentum states of an atomic qutrit and a single photon qutrit has been observed. Their full state was reconstructed using quantum state tomography. The fidelity to the maximally entangled state of Schmidt rank 3 exceeds the threshold 2/3. This result confirms that the density matrix cannot be decomposed into an ensemble of pure states of Schmidt rank 1 or 2. That is, the Schmidt number of the density matrix must be equal to or greater than 3.

Relativistic Radiative and Auger Rates for Fe XXIV

NASA Technical Reports Server (NTRS)

Bautista, M. A.; Mendoza, C.; Kallman, T. R.; Palmeri, P.; White, Nicholas E. (Technical Monitor)

2002-01-01

As part of a project to compute improved atomic data for the spectral modeling of iron K lines, we report extensive calculations and comparisons of radiative and Auger rates for transitions involving the K-vacancy states in Fe XXIV. By making use of several computational codes, a detailed study is carried out of orbital representation, configuration interaction, relativistic corrections, cancellation effects, and fine tuning. It is shown that a formal treatment of the Breit interaction is essential to render the important magnetic correlations that take part in the decay pathways of this ion. As a result, the accuracy of the present A-values is firmly ranked at better than 10% while that of the Auger rates at only 15%.

Atomistic analysis of valley-orbit hybrid states and inter-dot tunnel rates in a Si double quantum dot

NASA Astrophysics Data System (ADS)

Ferdous, Rifat; Rahman, Rajib; Klimeck, Gerhard

2014-03-01

Silicon quantum dots are promising candidates for solid-state quantum computing due to the long spin coherence times in silicon, arising from small spin-orbit interaction and a nearly spin free host lattice. However, the conduction band valley degeneracy adds an additional degree of freedom to the electronic structure, complicating the encoding and operation of qubits. Although the valley and the orbital indices can be uniquely identified in an ideal silicon quantum dot, atomic-scale disorder mixes valley and orbital states in realistic dots. Such valley-orbit hybridization, strongly influences the inter-dot tunnel rates.Using a full-band atomistic tight-binding method, we analyze the effect of atomic-scale interface disorder in a silicon double quantum dot. Fourier transform of the tight-binding wavefunctions helps to analyze the effect of disorder on valley-orbit hybridization. We also calculate and compare inter-dot inter-valley and intra-valley tunneling, in the presence of realistic disorder, such as interface tilt, surface roughness, alloy disorder, and interface charges. The method provides a useful way to compute electronic states in realistically disordered systems without any posteriori fitting parameters.

Communication: Localized molecular orbital analysis of the effect of electron correlation on the anomalous isotope effect in the NMR spin-spin coupling constant in methane

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

Zarycz, M. Natalia C., E-mail: mnzarycz@gmail.com; Provasi, Patricio F., E-mail: patricio@unne.edu.ar; Sauer, Stephan P. A., E-mail: sauer@kiku.dk

2014-10-21

We discuss the effect of electron correlation on the unexpected differential sensitivity (UDS) in the {sup 1}J(C–H) coupling constant of CH{sub 4} using a decomposition into contributions from localized molecular orbitals and compare with the {sup 1}J(N–H) coupling constant in NH{sub 3}. In particular, we discuss the well known fact that uncorrelated coupled Hartree-Fock (CHF) calculations are not able to reproduce the UDS in methane. For this purpose we have implemented for the first time a localized molecular orbital analysis for the second order polarization propagator approximation with coupled cluster singles and doubles amplitudes—SOPPA(CCSD) in the DALTON program. Comparing themore » changes in the localized orbital contributions at the correlated SOPPA and SOPPA(CCSD) levels and at the uncorrelated CHF level, we find that the latter overestimates the effect of stretching the bond between the coupled atoms on the contribution to the coupling from the localized bonding orbital between these atoms. This disturbs the subtle balance between the molecular orbital contributions, which lead to the UDS in methane.« less

Techniques for Measuring Low Earth Orbital Atomic Oxygen Erosion of Polymers

NASA Technical Reports Server (NTRS)

deGroh, Kim K.; Banks, Bruce A.; Demko, Rikako

2002-01-01

Polymers such as polyimide Kapton and Teflon FEP (fluorinated ethylene propylene) are commonly used spacecraft materials due to their desirable properties such as flexibility, low density, and in the case of FEP, a low solar absorptance and high thermal emittance. Polymers on the exterior of spacecraft in the low Earth orbit (LEO) environment are exposed to energetic atomic oxygen. Atomic oxygen reaction with polymers causes erosion, which is a threat to spacecraft durability. It is therefore important to understand the atomic oxygen erosion yield (E, the volume loss per incident oxygen atom) of polymers being considered in spacecraft design. The most common technique for determining E is through mass loss measurements. For limited duration exposure experiments, such as shuttle experiments, where the atomic oxygen fluence is often so low that mass loss measurements can not produce acceptable uncertainties, recession measurements based on atomic force microscopy analyses can be used. Equally necessary to knowing the mass loss or recession depth for determining the erosion yield of polymers is the knowledge of the atomic oxygen fluence that the polymers were exposed to in space. This paper discusses the procedures and relevant issues for mass loss and recession depth measurements for passive atomic oxygen erosion yield characterization of polymers, along with techniques for active atomic oxygen fluence and erosion characterization. One active atomic oxygen erosion technique discussed is a new technique based on optical measurements. Details including the use of both semi-transparent and opaque polymers for active erosion measurement are reviewed.

Quantitative evaluation of orbital hybridization in carbon nanotubes under radial deformation using π-orbital axis vector

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

Ohnishi, Masato, E-mail: masato.ohnishi@rift.mech.tohoku.ac.jp; Suzuki, Ken; Miura, Hideo, E-mail: hmiura@rift.mech.tohoku.ac.jp

2015-04-15

When a radial strain is applied to a carbon nanotube (CNT), the increase in local curvature induces orbital hybridization. The effect of the curvature-induced orbital hybridization on the electronic properties of CNTs, however, has not been evaluated quantitatively. In this study, the strength of orbital hybridization in CNTs under homogeneous radial strain was evaluated quantitatively. Our analyses revealed the detailed procedure of the change in electronic structure of CNTs. In addition, the dihedral angle, the angle between π-orbital axis vectors of adjacent atoms, was found to effectively predict the strength of local orbital hybridization in deformed CNTs.

An accurate, compact and computationally efficient representation of orbitals for quantum Monte Carlo calculations

NASA Astrophysics Data System (ADS)

Luo, Ye; Esler, Kenneth; Kent, Paul; Shulenburger, Luke

Quantum Monte Carlo (QMC) calculations of giant molecules, surface and defect properties of solids have been feasible recently due to drastically expanding computational resources. However, with the most computationally efficient basis set, B-splines, these calculations are severely restricted by the memory capacity of compute nodes. The B-spline coefficients are shared on a node but not distributed among nodes, to ensure fast evaluation. A hybrid representation which incorporates atomic orbitals near the ions and B-spline ones in the interstitial regions offers a more accurate and less memory demanding description of the orbitals because they are naturally more atomic like near ions and much smoother in between, thus allowing coarser B-spline grids. We will demonstrate the advantage of hybrid representation over pure B-spline and Gaussian basis sets and also show significant speed-up like computing the non-local pseudopotentials with our new scheme. Moreover, we discuss a new algorithm for atomic orbital initialization which used to require an extra workflow step taking a few days. With this work, the highly efficient hybrid representation paves the way to simulate large size even in-homogeneous systems using QMC. This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Computational Materials Sciences Program.

Orbital occupancy evolution across spin- and charge-ordering transitions in YBaFe2O5

NASA Astrophysics Data System (ADS)

Lindén, J.; Lindroos, F.; Karen, P.

2017-08-01

Thermal evolution of the Fe2+-Fe3+ valence mixing in YBaFe2O5 is investigated using Mössbauer spectroscopy. In this high-spin double-cell perovskite, the d6 and d5 Fe states differ by the single minority-spin electron which then controls all the spin- and charge-ordering transitions. Orbital occupancies can be extracted from the spectra in terms of the dxz , dz2 and either dx2-y2 (Main Article) or dxy (Supplement) populations of this electron upon conserving its angular momentum. At low temperatures, the minority-spin electrons fill up the ordered dxz orbitals of Fe2+, in agreement with the considerable orthorhombic distortion of the structure. Heating through the Verwey transition supplies 93% of the mixing entropy, at which point the predominantly mixing electron occupies mainly the dx2-y2 /dxy orbitals weakly bonding the two Fe atoms that face each other across the bases of their coordination pyramids. This might stabilize a weak coulombic checkerboard order suggested by McQueeney et alii in Phys. Rev. B 87(2013)045127. When the remaining 7% of entropy is supplied at a subsequent transition, the mixing electron couples the two Fe atoms predominantly via their dz2 orbitals. The valence mixing concerns more than 95% of the Fe atoms present in the crystalline solid; the rest is semi-quantitatively interpreted as domain walls and antiphase boundaries formed upon cooling through the Néel and Verwey-transition temperatures, respectively.

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.

Atomic Oxygen Effects

NASA Technical Reports Server (NTRS)

Miller, Sharon K. R.

2014-01-01

Atomic oxygen, which is the most predominant species in low Earth orbit, is highly reactive and can break chemical bonds on the surface of a wide variety of materials leading to volatilization or surface oxidation which can result in failure of spacecraft materials and components. This presentation will give an overview of how atomic oxygen reacts with spacecraft materials, results of space exposure testing of a variety of materials, and examples of failures caused by atomic oxygen.

Direct mapping between exchange potentials of Hartree-Fock and Kohn-Sham schemes as origin of orbital proximity

NASA Astrophysics Data System (ADS)

Cinal, M.

2010-01-01

It is found that for closed-l-shell atoms, the exact local exchange potential vx(r) calculated in the exchange-only Kohn-Sham (KS) scheme of the density functional theory (DFT) is very well represented within the region of every atomic shell by each of the suitably shifted potentials obtained with the nonlocal Fock exchange operator for the individual Hartree-Fock (HF) orbitals belonging to this shell. This newly revealed property is not related to the well-known steplike shell structure in the response part of vx(r), but it results from specific relations satisfied by the HF orbital exchange potentials. These relations explain the outstanding proximity of the occupied HF and exchange-only KS orbitals as well as the high quality of the Krieger-Li-Iafrate and localized HF (or, equivalently, common-energy-denominator) approximations to the DFT exchange potential vx(r). Another highly accurate representation of vx(r) is given by the continuous piecewise function built of shell-specific exchange potentials, each defined as the weighted average of the shifted orbital exchange potentials corresponding to a given shell. The constant shifts added to the HF orbital exchange potentials, to map them onto vx(r), are nearly equal to the differences between the energies of the corresponding KS and HF orbitals. It is discussed why these differences are positive and grow when the respective orbital energies become lower for inner orbitals.

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

Quantum chemical approach for positron annihilation spectra of atoms and molecules beyond plane-wave approximation

NASA Astrophysics Data System (ADS)

Ikabata, Yasuhiro; Aiba, Risa; Iwanade, Toru; Nishizawa, Hiroaki; Wang, Feng; Nakai, Hiromi

2018-05-01

We report theoretical calculations of positron-electron annihilation spectra of noble gas atoms and small molecules using the nuclear orbital plus molecular orbital method. Instead of a nuclear wavefunction, the positronic wavefunction is obtained as the solution of the coupled Hartree-Fock or Kohn-Sham equation for a positron and the electrons. The molecular field is included in the positronic Fock operator, which allows an appropriate treatment of the positron-molecule repulsion. The present treatment succeeds in reproducing the Doppler shift, i.e., full width at half maximum (FWHM) of experimentally measured annihilation (γ-ray) spectra for molecules with a mean absolute error less than 10%. The numerical results indicate that the interpretation of the FWHM in terms of a specific molecular orbital is not appropriate.

Ultracold Atoms in a Square Lattice with Spin-Orbit Coupling: Charge Order, Superfluidity, and Topological Signatures

NASA Astrophysics Data System (ADS)

Rosenberg, Peter; Shi, Hao; Zhang, Shiwei

2017-12-01

We present an ab initio, numerically exact study of attractive fermions in square lattices with Rashba spin-orbit coupling. The ground state of this system is a supersolid, with coexisting charge and superfluid order. The superfluid is composed of both singlet and triplet pairs induced by spin-orbit coupling. We perform large-scale calculations using the auxiliary-field quantum Monte Carlo method to provide the first full, quantitative description of the charge, spin, and pairing properties of the system. In addition to characterizing the exotic physics, our results will serve as essential high-accuracy benchmarks for the intense theoretical and especially experimental efforts in ultracold atoms to realize and understand an expanding variety of quantum Hall and topological superconductor systems.

Orbital Energy Levels in Molecular Hydrogen. A Simple Approach.

ERIC Educational Resources Information Center

Willis, Christopher J.

1988-01-01

Described are the energetics involved in the formation of molecular hydrogen using concepts that should be familiar to students beginning the study of molecular orbital theory. Emphasized are experimental data on ionization energies. Included are two-electron atomic and molecular systems. (CW)

Herbert P. Broida Prize Talk: A single Rydberg electron in a Bose-Einstein condensate: from two to few to many-body physics

NASA Astrophysics Data System (ADS)

Pfau, Tilman

2017-04-01

Modern quantum scattering theory was developed in the context of Rydberg spectroscopy in 1934 by Enrico Fermi. He showed that for slow electrons the scattering from polarizable atoms via a 1/r4 potential is purely s-wave and can be described by a Fermi pseudopotential and a scattering length. To study this interaction Rydberg electrons are well suited as they are slow and trapped by the charged nucleus. In a high pressure discharge Amaldi and Segre, observed a line shift proportional to the scattering length. At ultracold temperatures one can ask the opposite question: What does a Rydberg electron do to the neutral atom sitting in the electronic orbit? We found that one, two or many ground state atoms can be trapped in the mean-field potential created by the Rydberg electron, leading to so called ultra-long range Rydberg molecules. I will explain this novel molecular binding mechanism and the properties of these exotic molecules. At higher Rydberg states the spatial extent of the Rydberg electron orbit is increasing. For principal quantum numbers n in the range of 100-200 up to several ten thousand ultracold ground state atoms can be located inside one Rydberg atom, When we excite a single Rydberg electron in a Bose-Einstein Condensate, the orbital size of which becomes comparable to the size of the BEC we observe the coupling between the electron and phonons in the BEC.

(T2L2) Time Transfer by Laser Link

NASA Technical Reports Server (NTRS)

Veillet, Christian; Fridelance, Patricia

1995-01-01

T2L2 (Time Transfer by Laser Link) is a new generation time transfer experiment based on the principles of LASSO (Laser Synchronization from Synchronous Orbit) and used with an operational procedure developed at OCA (Observatoire de la Cote d'Azur) during the active intercontinental phase of LASSO. The hardware improvements could lead to a precision better than 10 ps for time transfer (flying clock monitoring or ground based clock comparison). Such a package could fly on any spacecraft with a stable clock. It has been developed in France in the frame of the PHARAO project (cooled atom clock in orbit) involving CNES and different laboratories. But T2L2 could fly on any spacecraft carrying a stable oscillator. A GPS satellite would be a good candidate, as T2L2 could allow to link the flying clock directly to ground clocks using light, aiming to important accuracy checks, both for time and for geodesy. Radioastron (a flying VLBI antenna with a H-maser) is also envisioned, waiting for a PHARAO flight. The ultimate goal of T2L2 is to be part of more ambitious missions, as SORT (Solar Orbit Relativity Test), aiming to examine aspects of the gravitation in the vicinity of the Sun.

Laplace-transformed atomic orbital-based Møller–Plesset perturbation theory for relativistic two-component Hamiltonians

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

Helmich-Paris, Benjamin, E-mail: b.helmichparis@vu.nl; Visscher, Lucas, E-mail: l.visscher@vu.nl; Repisky, Michal, E-mail: michal.repisky@uit.no

2016-07-07

We present a formulation of Laplace-transformed atomic orbital-based second-order Møller–Plesset perturbation theory (MP2) energies for two-component Hamiltonians in the Kramers-restricted formalism. This low-order scaling technique can be used to enable correlated relativistic calculations for large molecular systems. We show that the working equations to compute the relativistic MP2 energy differ by merely a change of algebra (quaternion instead of real) from their non-relativistic counterparts. With a proof-of-principle implementation we study the effect of the nuclear charge on the magnitude of half-transformed integrals and show that for light elements spin-free and spin-orbit MP2 energies are almost identical. Furthermore, we investigate themore » effect of separation of charge distributions on the Coulomb and exchange energy contributions, which show the same long-range decay with the inter-electronic/atomic distance as for non-relativistic MP2. A linearly scaling implementation is possible if the proper distance behavior is introduced to the quaternion Schwarz-type estimates as for non-relativistic MP2.« less

Introduction to Density Functional Theory: Calculations by Hand on the Helium Atom

ERIC Educational Resources Information Center

Baseden, Kyle A.; Tye, Jesse W.

2014-01-01

Density functional theory (DFT) is a type of electronic structure calculation that has rapidly gained popularity. In this article, we provide a step-by-step demonstration of a DFT calculation by hand on the helium atom using Slater's X-Alpha exchange functional on a single Gaussian-type orbital to represent the atomic wave function. This DFT…

Atomic oxygen interaction at defect sights in protective coatings on polymers flown on LDEF

NASA Technical Reports Server (NTRS)

Banks, Bruce A.; Degroh, Kim K.; Auer, Bruce M.; Gebauer, Linda; Lamoreaux, Cynthia

1993-01-01

Although the Long Duration Exposure Facility (LDEF) has exposed materials with a fixed orientation relative to the ambient low-Earth-orbital environment, arrival of atomic oxygen is angularly distributed as a result of the atomic oxygen's high temperature Maxwellian velocity distribution and the LDEF's orbital inclination. Thus, atomic oxygen entering defects in protective coatings on polymeric surfaces can cause wider undercut cavities than the size of the defect in the protective coating. Because only a small fraction of atomic oxygen reacts upon first impact with most polymeric materials, secondary reactions with lower energy thermally accommodated atomic oxygen can occur. The secondary reactions of scattered and/or thermally accommodated atomic oxygen also contribute to widening the undercut cavity beneath the protective coating defect. As the undercut cavity enlarges, exposing more polymer, the probability of atomic oxygen reacting with underlying polymeric material increases because of multiple opportunities for reaction. Thus, the effective atomic oxygen erosion yield for atoms entering defects increases above that of the unprotected material. Based on the results of analytical modeling and computational modeling, aluminized Kapton multilayer insulation exposed to atomic oxygen on row 9 lost the entire externally exposed layer of polyimide Kapton, yet based on the results of this investigation, the bottom surface aluminum film must have remained in place, but crazed. Atomic oxygen undercutting at defect sites in protective coatings on graphite epoxy composites indicates that between 40 to 100 percent of the atomic oxygen thermally accommodates upon impact, and that the reaction probability of thermally accommodated atomic oxygen may range from 7.7 x 10(exp -6) to 2.1 x 10(exp -3), depending upon the degree of thermal accommodation upon each impact.

Relativistic Confinement Resonances

NASA Astrophysics Data System (ADS)

Keating, David; Manson, Steven; Deshmukh, Pranawa

2017-04-01

Photoionization of confined atoms in a C60 fullerene have been under intense investigation in the recent years, in particular the confinement induced resonances, termed confinement resonances. The effects of the C60 potential are modeled by a static spherical well, with (in atomic units) inner radius r0 = 5.8, width Δ = 1.9, and depth U0 = -0.302, which is reasonable in the energy region well above the C60 plasmons. At very high Z, relativistic interactions become important contributors to even the qualitative nature of atomic properties; this is true for confined atomic properties as well. To explore the extent of these interactions, a theoretical study of several heavy atoms has been performed using the relativistic random phase approximation (RRPA) methodology. In order to determine which features in the photoionization cross section are due to relativity, calculations using the (nonrelativistic) random phase approximation with exchange method (RPAE) are performed for comparison. The existence of the second subshell of the spin-orbit-split doublets can induce new confinement resonances in the total cross section, which is the sum of the spin-orbit-split doublets, due to the shift in the doublet's threshold. Several examples for confined high-Z atoms are presented. Work supported by DOE and NSF.

A facility to produce an energetic, ground state atomic oxygen beam for the simulation of the Low-Earth Orbit environment

NASA Technical Reports Server (NTRS)

Ketsdever, Andrew D.; Weaver, David P.; Muntz, E. P.

1994-01-01

Because of the continuing commitment to activity in low-Earth orbit (LEO), a facility is under development to produce energetic atmospheric species, particularly atomic oxygen, with energies ranging from 5 to 80 eV. This relatively high flux facility incorporates an ion engine to produce the corresponding specie ion which is charge exchanged to produce a neutral atomic beam. Ion fluxes of around 10(exp 15) sec(exp -1) with energies of 20-70 eV have been achieved. A geometrically augmented inertially tethered charge exchanger (GAITCE) was designed to provide a large column depth of charge exchange gas while reducing the gas load to the low pressure portion of the atomic beam facility. This is accomplished using opposed containment jets which act as collisional barriers to the escape of the dense gas region formed between the jets. Leak rate gains to the pumping system on the order of 10 were achieved for moderate jet mass flows. This system provides an attractive means for the charge exchange of atomic ions with a variety of gases to produce energetic atomic beams.

Investigation of Teflon FEP Embrittlement on Spacecraft in Low-Earth Orbit

NASA Technical Reports Server (NTRS)

deGroh, Kim K.; Banks, Bruce A.

1997-01-01

Teflon fluorinated ethylene propylene (FEP) (DuPont) is commonly used on exterior spacecraft surfaces for thermal control in the low-Earth orbit environment. Silverized or aluminized Teflon FEP is used for the outer layers of the thermal control blanket because of its high reflectance, low solar absorptance, and high thermal emittance. Teflon FEP is also desirable because, compared with other spacecraft polymers (such as Kapton), it has relatively high resistance to atomic oxygen erosion. Because of its comparably low atomic oxygen erosion yield, Teflon FEP has been used unprotected in the space environment. Samples of Teflon FEP from the Long Duration Exposure Facility (LDEF) and the Hubble Space Telescope (retrieved during its first servicing mission) were evaluated for solar-induced embrittlement and for synergistic effects of solar degradation and atomic oxygen.

Fermi orbital derivatives in self-interaction corrected density functional theory: Applications to closed shell atoms

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

Pederson, Mark R., E-mail: mark.pederson@science.doe.gov

2015-02-14

A recent modification of the Perdew-Zunger self-interaction-correction to the density-functional formalism has provided a framework for explicitly restoring unitary invariance to the expression for the total energy. The formalism depends upon construction of Löwdin orthonormalized Fermi-orbitals which parametrically depend on variational quasi-classical electronic positions. Derivatives of these quasi-classical electronic positions, required for efficient minimization of the self-interaction corrected energy, are derived and tested, here, on atoms. Total energies and ionization energies in closed-shell singlet atoms, where correlation is less important, using the Perdew-Wang 1992 Local Density Approximation (PW92) functional, are in good agreement with experiment and non-relativistic quantum-Monte-Carlo results albeitmore » slightly too low.« less

Realization of two-dimensional spin-orbit coupling for Bose-Einstein condensates.

PubMed

Wu, Zhan; Zhang, Long; Sun, Wei; Xu, Xiao-Tian; Wang, Bao-Zong; Ji, Si-Cong; Deng, Youjin; Chen, Shuai; Liu, Xiong-Jun; Pan, Jian-Wei

2016-10-07

Cold atoms with laser-induced spin-orbit (SO) interactions provide a platform to explore quantum physics beyond natural conditions of solids. Here we propose and experimentally realize two-dimensional (2D) SO coupling and topological bands for a rubidium-87 degenerate gas through an optical Raman lattice, without phase-locking or fine-tuning of optical potentials. A controllable crossover between 2D and 1D SO couplings is studied, and the SO effects and nontrivial band topology are observed by measuring the atomic cloud distribution and spin texture in momentum space. Our realization of 2D SO coupling with advantages of small heating and topological stability opens a broad avenue in cold atoms to study exotic quantum phases, including topological superfluids. Copyright © 2016, American Association for the Advancement of Science.

Effects of single atom doping on the ultrafast electron dynamics of M1Au24(SR)18 (M = Pd, Pt) nanoclusters

NASA Astrophysics Data System (ADS)

Zhou, Meng; Qian, Huifeng; Sfeir, Matthew Y.; Nobusada, Katsuyuki; Jin, Rongchao

2016-03-01

Atomically precise, doped metal clusters are receiving wide research interest due to their synergistic properties dependent on the metal composition. To understand the electronic properties of doped clusters, it is highly desirable to probe the excited state behavior. Here, we report the ultrafast relaxation dynamics of doped M1@Au24(SR)18 (M = Pd, Pt; R = CH2CH2Ph) clusters using femtosecond visible and near infrared transient absorption spectroscopy. Three relaxation components are identified for both mono-doped clusters: (1) sub-picosecond relaxation within the M1Au12 core states; (2) core to shell relaxation in a few picoseconds; and (3) relaxation back to the ground state in more than one nanosecond. Despite similar relaxation pathways for the two doped nanoclusters, the coupling between the metal core and surface ligands is accelerated by over 30% in the case of the Pt dopant compared with the Pd dopant. Compared to Pd doping, the case of Pt doping leads to much more drastic changes in the steady state and transient absorption of the clusters, which indicates that the 5d orbitals of the Pt atom are more strongly mixed with Au 5d and 6s orbitals than the 4d orbitals of the Pd dopant. These results demonstrate that a single foreign atom can lead to entirely different excited state spectral features of the whole cluster compared to the parent Au25(SR)18 cluster. The detailed excited state dynamics of atomically precise Pd/Pt doped gold clusters help further understand their properties and benefit the development of energy-related applications.Atomically precise, doped metal clusters are receiving wide research interest due to their synergistic properties dependent on the metal composition. To understand the electronic properties of doped clusters, it is highly desirable to probe the excited state behavior. Here, we report the ultrafast relaxation dynamics of doped M1@Au24(SR)18 (M = Pd, Pt; R = CH2CH2Ph) clusters using femtosecond visible and near infrared transient absorption spectroscopy. Three relaxation components are identified for both mono-doped clusters: (1) sub-picosecond relaxation within the M1Au12 core states; (2) core to shell relaxation in a few picoseconds; and (3) relaxation back to the ground state in more than one nanosecond. Despite similar relaxation pathways for the two doped nanoclusters, the coupling between the metal core and surface ligands is accelerated by over 30% in the case of the Pt dopant compared with the Pd dopant. Compared to Pd doping, the case of Pt doping leads to much more drastic changes in the steady state and transient absorption of the clusters, which indicates that the 5d orbitals of the Pt atom are more strongly mixed with Au 5d and 6s orbitals than the 4d orbitals of the Pd dopant. These results demonstrate that a single foreign atom can lead to entirely different excited state spectral features of the whole cluster compared to the parent Au25(SR)18 cluster. The detailed excited state dynamics of atomically precise Pd/Pt doped gold clusters help further understand their properties and benefit the development of energy-related applications. Electronic supplementary information (ESI) available: The pump dependent transient absorption spectra and the corresponding global analysis results. See DOI: 10.1039/c6nr01008c

Fluorescence detection of white-beam X-ray absorption anisotropy: towards element-sensitive projections of local atomic structure

PubMed Central

Korecki, P.; Tolkiehn, M.; Dąbrowski, K. M.; Novikov, D. V.

2011-01-01

Projections of the atomic structure around Nb atoms in a LiNbO3 single crystal were obtained from a white-beam X-ray absorption anisotropy (XAA) pattern detected using Nb K fluorescence. This kind of anisotropy results from the interference of X-rays inside a sample and, owing to the short coherence length of a white beam, is visible only at small angles around interatomic directions. Consequently, the main features of the recorded XAA corresponded to distorted real-space projections of dense-packed atomic planes and atomic rows. A quantitative analysis of XAA was carried out using a wavelet transform and allowed well resolved projections of Nb atoms to be obtained up to distances of 10 Å. The signal of nearest O atoms was detected indirectly by a comparison with model calculations. The measurement of white-beam XAA using characteristic radiation indicates the possibility of obtaining element-sensitive projections of the local atomic structure in more complex samples. PMID:21997909

Low Earth Orbital Atomic Oxygen Interactions With Spacecraft Materials

NASA Technical Reports Server (NTRS)

Banks, Bruce A.; deGroh, Kim K.; Miller, Sharon K.

2004-01-01

Atomic oxygen, formed in Earth s thermosphere, interacts readily with many materials on spacecraft flying in low Earth orbit (LEO). All hydrocarbon based polymers and graphite are easily oxidized upon the impact of approx.4.5 eV atomic oxygen as the spacecraft ram into the residual atmosphere. The resulting interactions can change the morphology and reduce the thickness of these materials. Directed atomic oxygen erosion will result in the development of textured surfaces on all materials with volatile oxidation products. Examples from space flight samples are provided. As a result of the erosive properties of atomic oxygen on polymers and composites, protective coatings have been developed and are used to increase the functional life of polymer films and composites that are exposed to the LEO environment. The atomic oxygen erosion yields for actual and predicted LEO exposure of numerous materials are presented. Results of in-space exposure of vacuum deposited aluminum protective coatings on polyimide Kapton indicate high rates of degradation are associated with aluminum coatings on both surfaces of the Kapton. Computational modeling predictions indicate that less trapping of the atomic oxygen occurs, with less resulting damage, if only the space-exposed surface is coated with vapor deposited aluminum rather than having both surfaces coated.

Two-component relativistic coupled-cluster methods using mean-field spin-orbit integrals

NASA Astrophysics Data System (ADS)

Liu, Junzi; Shen, Yue; Asthana, Ayush; Cheng, Lan

2018-01-01

A novel implementation of the two-component spin-orbit (SO) coupled-cluster singles and doubles (CCSD) method and the CCSD augmented with the perturbative inclusion of triple excitations [CCSD(T)] method using mean-field SO integrals is reported. The new formulation of SO-CCSD(T) features an atomic-orbital-based algorithm for the particle-particle ladder term in the CCSD equation, which not only removes the computational bottleneck associated with the large molecular-orbital integral file but also accelerates the evaluation of the particle-particle ladder term by around a factor of 4 by taking advantage of the spin-free nature of the instantaneous electron-electron Coulomb interaction. Benchmark calculations of the SO splittings for the thallium atom and a set of diatomic 2Π radicals as well as of the bond lengths and harmonic frequencies for a set of closed-shell diatomic molecules are presented. The basis-set and core-correlation effects in the calculations of these properties have been carefully analyzed.

Ultrastructural investigation of intact orbital implant surfaces using atomic force microscopy.

PubMed

Choi, Samjin; Lee, Seung Jun; Shin, Jae-Ho; Cheong, Youjin; Lee, Hui-Jae; Paek, Joo Hee; Kim, Jae Sik; Jin, Kyung-Hyun; Park, Hun-Kuk

2011-01-01

This study examined the surface nanostructures of three orbital implants: nonporous poly(methyl methacrylate) (PMMA), porous aluminum oxide and porous polyethylene. The morphological characteristics of the orbital implants surfaces were observed by atomic force microscopy (AFM). The AFM topography, phase shift and deflection images of the intact implant samples were obtained. The surface of the nonporous PMMA implant showed severe scratches and debris. The surface of the aluminum oxide implant showed a porous structure with varying densities and sizes. The PMMA implant showed nodule nanostructures, 215.56 ± 52.34 nm in size, and the aluminum oxide implant showed crystal structures, 730.22 ± 341.02 nm in size. The nonporous PMMA implant showed the lowest roughness compared with other implant biomaterials, followed by the porous aluminum oxide implant. The porous polyethylene implant showed the highest roughness and severe surface irregularities. Overall, the surface roughness of orbital implants might be associated with the rate of complications and cell adhesion. Copyright © 2011 Wiley Periodicals, Inc.

Unconventional Bose—Einstein Condensations from Spin-Orbit Coupling

NASA Astrophysics Data System (ADS)

Wu, Cong-Jun; Ian, Mondragon-Shem; Zhou, Xiang-Fa

2011-09-01

According to the “no-node" theorem, the many-body ground state wavefunctions of conventional Bose—Einstein condensations (BEC) are positive-definite, thus time-reversal symmetry cannot be spontaneously broken. We find that multi-component bosons with spin-orbit coupling provide an unconventional type of BECs beyond this paradigm. We focus on a subtle case of isotropic Rashba spin-orbit coupling and the spin-independent interaction. In the limit of the weak confining potential, the condensate wavefunctions are frustrated at the Hartree—Fock level due to the degeneracy of the Rashba ring. Quantum zero-point energy selects the spin-spiral type condensate through the “order-from-disorder" mechanism. In a strong harmonic confining trap, the condensate spontaneously generates a half-quantum vortex combined with the skyrmion type of spin texture. In both cases, time-reversal symmetry is spontaneously broken. These phenomena can be realized in both cold atom systems with artificial spin-orbit couplings generated from atom-laser interactions and exciton condensates in semi-conductor systems.

Chiral sp-orbital paired superfluid of fermionic atoms in a 2D spin-dependent optical lattice

NASA Astrophysics Data System (ADS)

Liu, Bo; Li, Xiaopeng; Wu, Biao; Liu, W. Vincent

2014-03-01

Recent progress in realizing synthetic quantum orbital materials in chequerboard and hexagonal optical lattices opens an avenue towards exploiting unconventional quantum states, advancing our understanding of correlated quantum matter. Here, we unveil a chiral sp -orbital paired superfluid state for an interacting two-component Fermi gas in a 2D spin-dependent optical lattice. Surprisingly, this novel state is found to exist in a wide regime of experimentally tunable interaction strengths. The coexistence of this chiral superfluid and the ferro-orbital order is reminiscent of that of magnetism and superconductivity which is a long-standing issue in condensed matter physics. The topological properties are demonstrated by the existence of gapless chiral fermions in the presence of domain wall defects, reminiscent of quantum Hall edge states. Such properties can be measured by radio frequency spectroscopy in cold atomic experiments. Work supported in part by U.S. ARO, AFOSR, and DARPA-OLE-ARO, Kaufman Foundation, and NSF of China.

Fully relativistic pseudopotential formalism under an atomic orbital basis: spin-orbit splittings and magnetic anisotropies.

PubMed

Cuadrado, R; Cerdá, J I

2012-02-29

We present an efficient implementation of the spin-orbit coupling within the density functional theory based SIESTA code (2002 J. Phys.: Condens. Matter 14 2745) using the fully relativistic and totally separable pseudopotential formalism of Hemstreet et al (1993 Phys. Rev. B 47 4238). First, we obtain the spin-orbit splittings for several systems ranging from isolated atoms to bulk metals and semiconductors as well as the Au(111) surface state. Next, and after extensive tests on the accuracy of the formalism, we also demonstrate its capability to yield reliable values for the magnetic anisotropy energy in magnetic systems. In particular, we focus on the L1(0) binary alloys and on two large molecules: Mn(6)O(2)(H -sao)(6)(O(2)CH)(2)(CH(3)OH)(4) and Co(4)(hmp)(4)(CH(3)OH)(4)Cl(4). In all cases our calculated anisotropies are in good agreement with those obtained with full-potential methods, despite the latter being, in general, computationally more demanding.

Implementation of an approximate self-energy correction scheme in the orthogonalized linear combination of atomic orbitals method of band-structure calculations

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

Gu, Z.; Ching, W.Y.

Based on the Sterne-Inkson model for the self-energy correction to the single-particle energy in the local-density approximation (LDA), we have implemented an approximate energy-dependent and [bold k]-dependent [ital GW] correction scheme to the orthogonalized linear combination of atomic orbital-based local-density calculation for insulators. In contrast to the approach of Jenkins, Srivastava, and Inkson, we evaluate the on-site exchange integrals using the LDA Bloch functions throughout the Brillouin zone. By using a [bold k]-weighted band gap [ital E][sub [ital g

Tight-binding model for borophene and borophane

NASA Astrophysics Data System (ADS)

Nakhaee, M.; Ketabi, S. A.; Peeters, F. M.

2018-03-01

Starting from the simplified linear combination of atomic orbitals method in combination with first-principles calculations, we construct a tight-binding (TB) model in the two-centre approximation for borophene and hydrogenated borophene (borophane). The Slater and Koster approach is applied to calculate the TB Hamiltonian of these systems. We obtain expressions for the Hamiltonian and overlap matrix elements between different orbitals for the different atoms and present the SK coefficients in a nonorthogonal basis set. An anisotropic Dirac cone is found in the band structure of borophane. We derive a Dirac low-energy Hamiltonian and compare the Fermi velocities with that of graphene.

Faraday diamagnetism under slowly oscillating magnetic fields

NASA Astrophysics Data System (ADS)

Kimura, Tsunehisa; Kimura, Fumiko; Kimura, Yosuke

2018-04-01

Diamagnetism is a universal phenomenon of materials arising from the orbital motion of electrons bound to atoms, which is commonly known as Langevin diamagnetism. The orbital motion also occurs according to the Faraday's law of induction when the applied magnetic field is oscillating. However, the influence of this dynamic effect on the magnetism of materials has seldom been studied. Here, we propose a new type diamagnetism coined Faraday diamagnetism. The magnitude of this diamagnetism evaluated by an atomic electric circuit model was as large as that of Langevin diamagnetism. The predicted scale of Faraday diamagnetism was supported by experiments.

Interplay between the spin-selection rule and frontier orbital theory in O2 activation and CO oxidation by single-atom-sized catalysts on TiO2(110).

PubMed

Li, Shunfang; Zhao, Xingju; Shi, Jinlei; Jia, Yu; Guo, Zhengxiao; Cho, Jun-Hyung; Gao, Yanfei; Zhang, Zhenyu

2016-09-28

Exploration of the catalytic activity of low-dimensional transition metal (TM) or noble metal catalysts is a vital subject of modern materials science because of their instrumental role in numerous industrial applications. Recent experimental advances have demonstrated the utilization of single atoms on different substrates as effective catalysts, which exhibit amazing catalytic properties such as more efficient catalytic performance and higher selectivity in chemical reactions as compared to their nanostructured counterparts; however, the underlying microscopic mechanisms operative in these single atom catalysts still remain elusive. Based on first-principles calculations, herein, we present a comparative study of the key kinetic rate processes involved in CO oxidation using a monomer or dimer of two representative TMs (Pd and Ni) on defective TiO2(110) substrates (TMn@TiO2(110), n = 1, 2) to elucidate the underlying mechanism of single-atom catalysis. We reveal that the O2 activation rates of the single atom TM catalysts deposited on TiO2(110) are governed cooperatively by the classic spin-selection rule and the well-known frontier orbital theory (or generalized d-band picture) that emphasizes the energy gap between the frontier orbitals of the TM catalysts and O2 molecule. We further illuminate that the subsequent CO oxidation reactions proceed via the Langmuir-Hinshelwood mechanism with contrasting reaction barriers for the Pd monomer and dimer catalysts. These findings not only provide an explanation for existing observations of distinctly different catalytic activities of Pd@TiO2(110) and Pd2@TiO2(110) [Kaden et al., Science, 2009, 326, 826-829] but also shed new insights into future utilization and optimization of single-atom catalysis.

Polymerization of a divalent/tetravalent metal-storing atom-mimicking dendrimer.

PubMed

Albrecht, Ken; Hirabayashi, Yuki; Otake, Masaya; Mendori, Shin; Tobari, Yuta; Azuma, Yasuo; Majima, Yutaka; Yamamoto, Kimihisa

2016-12-01

The phenylazomethine dendrimer (DPA) has a layer-by-layer electron density gradient that is an analog of the Bohr atom (atom mimicry). In combination with electron pair mimicry, the polymerization of this atom-mimicking dendrimer was achieved. The valency of the mimicked atom was controlled by changing the chemical structure of the dendrimer. By mimicking a divalent atom, a one-dimensional (1D) polymer was obtained, and by using a planar tetravalent atom mimic, a 2D polymer was obtained. These poly(dendrimer) polymers could store Lewis acids (SnCl 2 ) in their unoccupied orbitals, thus indicating that these poly(dendrimer) polymers consist of a series of nanocontainers.

Creating Rydberg electron wave packets using terahertz pulses

NASA Astrophysics Data System (ADS)

Bromage, Jake

1999-10-01

In this thesis I present experiments in which we excited classical-limit states of an atom using terahertz pulses. In a classical-limit state, an atom's outer electron is confined to a wave packet that orbits the core along a classical trajectory. Researchers have excited states with classical traits, but wave packets localized in all three dimensions have proved elusive. Theoretical studies have shown such states can be created using terahertz pulses. Using these techniques, we created a linear-orbit wave packet (LOWP), that is three-dimensionally localized and orbits along a line on one side of the atom's core. Terahertz pulses are sub-picosecond bursts of far- infrared radiation. Unlike ultrashort optical pulses, the electric field of terahertz pulses barely completes a single cycle. Our simulations of the atom-pulse interaction show that this electric field profile is critical in determining the quality of the wave packet. To characterize our terahertz pulses, we invented dithered-edge sampling which time- resolves the electric field using a photoconductive receiver and a triggered attenuator. We also studied how pulses are distorted after propagating through metallic structures, and used our findings to design our atomic experiments. We excited wave packets in atomic sodium using a two-step process. First, we used tunable, nanosecond dye lasers to excite an extreme Stark state. Next, we used a terahertz pump pulse to coherently redistribute population among extreme Stark states in neighboring manifolds. Interference between the final states produces a localized, dynamic LOWP. To analyze the LOWP, we ionized it with a stronger terahertz probe pulse, varying the pump-probe delay to map out its motion. We observed two strong LOWP signatures. Changing the static electric field produced small changes (2%) in the orbital period that agreed with our theoretical predictions. Secondly, because the LOWP scatters off the core, the pump-probe signal depended on the direction of the kick the LOWP received from the robe pulse. These observations, combined with our detailed simulations that used sodium parameters and the actual shape of the terahertz pulse, lead us to conclude that we excited a LOWP.

Super-reduced polyoxometalates: excellent molecular cluster battery components and semipermeable molecular capacitors.

PubMed

Nishimoto, Yoshio; Yokogawa, Daisuke; Yoshikawa, Hirofumi; Awaga, Kunio; Irle, Stephan

2014-06-25

Theoretical investigations are presented on the molecular and electronic structure changes that occur as α-Keggin-type polyoxometalate (POM(3-)) clusters [PM12O40](3-) (M = Mo, W) are converted toward their super-reduced POM(27-) state during the discharging process in lithium-based molecular cluster batteries. Density functional theory was employed in geometry optimization, and first-principles molecular dynamics simulations were used to explore local minima on the potential energy surface of neutral POM clusters adorned with randomly placed Li atoms as electron donors around the cluster surface. On the basis of structural, electron density, and molecular orbital studies, we present evidence that the super-reduction is accompanied by metal-metal bond formation, beginning from the 12th to 14th excess electron transferred to the cluster. Afterward, the number of metal-metal bonds increases nearly linearly with the number of additionally transferred excess electrons. In α-Keggin-type POMs, metal triangles are a prominently emerging structural feature. The origin of the metal triangle formation during super-reduction stems from the formation of characteristic three-center two-electron bonds in triangular metal atom sites, created under preservation of the POM skeleton via "squeezing out" of oxygen atoms bridging two metal atoms when the underlying metal atoms form covalent bonds. The driving force for this unusual geometrical and electronic structure change is a local Jahn-Teller distortion at individual transition-metal octahedral sites, where the triply degenerate t2 d orbitals become partially filled during reduction and gain energy by distortion of the octahedron in such a way that metal-metal bonds are formed. The bonding orbitals show strong contributions from mixing with metal-oxygen antibonding orbitals, thereby "shuffling away" excess electrons from the cluster center to the outside of the cage. The high density of negatively charged yet largely separated oxygen atoms on the surface of the super-reduced POM(27-) polyanion allows the huge Coulombic repulsion due to the presence of the excess electrons to be counterbalanced by the presence of Li countercations, which partially penetrate into the outer oxygen shell. This "semiporous molecular capacitor" structure is likely the reason for the effective electron uptake in POMs.

Physics of higher orbital bands in optical lattices: a review.

PubMed

Li, Xiaopeng; Liu, W Vincent

2016-11-01

The orbital degree of freedom plays a fundamental role in understanding the unconventional properties in solid state materials. Experimental progress in quantum atomic gases has demonstrated that high orbitals in optical lattices can be used to construct quantum emulators of exotic models beyond natural crystals, where novel many-body states such as complex Bose-Einstein condensates and topological semimetals emerge. A brief introduction of orbital degrees of freedom in optical lattices is given and a summary of exotic orbital models and resulting many-body phases is provided. Experimental consequences of the novel phases are also discussed.

Computer Series, 89.

ERIC Educational Resources Information Center

Moore, John W., Ed.

1988-01-01

Describes five computer software packages; four for MS-DOS Systems and one for Apple II. Included are SPEC20, an interactive simulation of a Bausch and Lomb Spectronic-20; a database for laboratory chemicals and programs for visualizing Boltzmann-like distributions, orbital plot for the hydrogen atom and molecular orbital theory. (CW)

Orbital Battleship: A Guessing Game to Reinforce Atomic Structure

ERIC Educational Resources Information Center

Kurushkin, Mikhail; Mikhaylenko, Maria

2016-01-01

A competitive educational guessing game "Orbital Battleship" which reinforces Madelung's and Hund's rules, values of quantum numbers, and understanding of periodicity was designed. The game develops strategic thinking, is not time-consuming, requires minimal preparation and supervision, and is an efficient and fun alternative to more…

Strongly-correlated crystal-field approach to heavy-fermion compounds and to 3d oxides

NASA Astrophysics Data System (ADS)

Radwanski, Ryszard; Ropka, Zofia

2005-03-01

The description of electronic and magnetic properties of real compounds like LaMnO3, LaCoO3, Na2V3O7, FeO, NdAl2 and ErNi5 as well as heavy-fermion superconductor UPd2Al3 and heavy-fermion metal YbRh2Si2, both zero-temperature ground state properties and thermodynamics, will be presented pointing out the existence of a discrete atomic-like low-energy, in the meV scale, electronic structure. This low-energy many-electron discrete atomic-like electronic structure is governed by very strong electron correlations, predominantly on-site, by the intra-atomic spin-orbit coupling and by details of the local surrounding (crystal-field interactions), but later is modified by inter-site interactions. Our studies indicate that there is the highest time to ``unquench'' the orbital moment in solid state physics in description of 3d-/4f-/5f-atom containing compounds and that heavy-fermion phenomena are of the relativistic origin.

Neutral sodium atoms extraction by micrometeoroid impacts on the surface of Mercury

NASA Astrophysics Data System (ADS)

Cremonese, G.; Orsini, S.; Capria, M. T.; Milillo, A.; Mura, A.; Mangano, V.; Carbognani, A.

2003-04-01

The Mercury's exosphere is more dependent on the micrometeoroid impacts than the lunar exosphere and we have applied an order-to-magnitude calculation on the physical conditions of the sodium atoms during these events. This calculation shows the different ionization degree of sodium atoms depending on the meteoroid impact velocity and the related emission enhancements we may have observing the exosphere. We have applied the same calculation to the visible and UV doublets showing the large difference, a factor 5, between the two emission intensities only taking into account the same micrometeoroids contribution. Furthermore we provide a rough estimate for the impact magnitude in sodium light if we observe the night side of the Mercury's surface from the orbit of the ESA mission BepiColombo. Assuming a specific energy distribution of the emitted neutrals, we simulate the characteristics of the low-energy neutral atom fluxes as observable by the SERENA/ELENA instrument proposed on board the ESA BepiColombo Planetary Orbiter.

Laser supported detonation wave source of atomic oxygen for aerospace material testing

NASA Technical Reports Server (NTRS)

Krech, Robert H.; Caledonia, George E.

1990-01-01

A pulsed high-flux source of nearly monoenergetic atomic oxygen was developed to perform accelerated erosion testing of spacecraft materials in a simulated low-earth orbit (LEO) environment. Molecular oxygen is introduced into an evacuated conical expansion nozzle at several atmospheres pressure through a pulsed molecular beam valve. A laser-induced breakdown is generated in the nozzle throat by a pulsed CO2 TEA laser. The resulting plasma is heated by the ensuing laser-supported detonation wave, and then it rapidly expands and cools. An atomic oxygen beam is generated with fluxes above 10 to the 18th atoms per pulse at 8 + or - 1.6 km/s with an ion content below 1 percent for LEO testing. Materials testing yielded the same surface oxygen enrichment in polyethylene samples as observed on the STS mission, and scanning electron micrographs of the irradiated polymer surfaces showed an erosion morphology similar to that obtained on low earth orbit.

An electrically conductive thermal control surface for spacecraft encountering Low-Earth Orbit (LEO) atomic oxygen indium tin oxide-coated thermal blankets

NASA Technical Reports Server (NTRS)

Bauer, J. L.

1987-01-01

An organic black thermal blanket material was coated with indium tin oxide (ITO) to prevent blanket degradation in the low Earth orbit (LEO) atomic oxygen environment. The blankets were designed for the Galileo spacecraft. Galileo was initially intended for space shuttle launch and would, therefore, have been exposed to atomic oxygen in LEO for between 10 and 25 hours. Two processes for depositing ITO are described. Thermooptical, electrical, and chemical properties of the ITO film are presented as a function of the deposition process. Results of exposure of the ITO film to atomic oxygen (from a shuttle flight) and radiation exposure (simulated Jovian environment) are also presented. It is shown that the ITO-protected thermal blankets would resist the anticipated LEO oxygen and Jovian radiation yet provide adequate thermooptical and electrical resistance. Reference is made to the ESA Ulysses spacecraft, which also used ITO protection on thermal control surfaces.

Spin-Orbit Interactions and Quantum Spin Dynamics in Cold Ion-Atom Collisions

NASA Astrophysics Data System (ADS)

Tscherbul, Timur V.; Brumer, Paul; Buchachenko, Alexei A.

2016-09-01

We present accurate ab initio and quantum scattering calculations on a prototypical hybrid ion-atom system Yb+ -Rb, recently suggested as a promising candidate for the experimental study of open quantum systems, quantum information processing, and quantum simulation. We identify the second-order spin-orbit (SO) interaction as the dominant source of hyperfine relaxation in cold Yb+ -Rb collisions. Our results are in good agreement with recent experimental observations [L. Ratschbacher et al., Phys. Rev. Lett. 110, 160402 (2013)] of hyperfine relaxation rates of trapped Yb+ immersed in an ultracold Rb gas. The calculated rates are 4 times smaller than is predicted by the Langevin capture theory and display a weak T-0.3 temperature dependence, indicating significant deviations from statistical behavior. Our analysis underscores the deleterious nature of the SO interaction and implies that light ion-atom combinations such as Yb+ -Li should be used to minimize hyperfine relaxation and decoherence of trapped ions in ultracold atomic gases.

Mono-Mercury Doping of Au25 and the HOMO/LUMO Energies Evaluation Employing Differential Pulse Voltammetry.

PubMed

Liao, Lingwen; Zhou, Shiming; Dai, Yafei; Liu, Liren; Yao, Chuanhao; Fu, Cenfeng; Yang, Jinlong; Wu, Zhikun

2015-08-05

Controlling the bimetal nanoparticle with atomic monodispersity is still challenging. Herein, a monodisperse bimetal nanoparticle is synthesized in 25% yield (on gold atom basis) by an unusual replacement method. The formula of the nanoparticle is determined to be Au24Hg1(PET)18 (PET: phenylethanethiolate) by high-resolution ESI-MS spectrometry in conjunction with multiple analyses including X-ray photoelectron spectroscopy (XPS) and thermogravimetric analysis (TGA). X-ray single-crystal diffraction reveals that the structure of Au24Hg1(PET)18 remains the structural framework of Au25(PET)18 with one of the outer-shell gold atoms replaced by one Hg atom, which is further supported by theoretical calculations and experimental results as well. Importantly, differential pulse voltammetry (DPV) is first employed to estimate the highest occupied molecular orbit (HOMO) and the lowest unoccupied molecular orbit (LUMO) energies of Au24Hg1(PET)18 based on previous calculations.

Observation of anisotropic interactions between metastable atoms and target molecules by two-dimensional collisional ionization electron spectroscopy

NASA Astrophysics Data System (ADS)

Kishimoto, Naoki; Ohno, Koichi

Excited metastable atoms colliding with target molecules can sensitively probe outer properties of molecules by chemi-ionization (Penning ionization) from molecular orbitals in the outer region, since metastable atoms cannot penetrate into the repulsive interaction wall around the molecules. By means of two-dimensional measurements using kinetic energy analysis of electrons combined with a velocity-resolved metastable beam, one can obtain information on the anisotropic interaction between the colliding particles without any control of orientation or alignment of target molecules. We have developed a classical trajectory method to calculate the collision energy dependence of partial ionization cross-sections (CEDPICS) on the anisotropic interaction potential energy surface, which has enabled us to study stereodynamics between metastable atoms and target molecules as well as the spatial distribution of molecular orbitals and electron ejection functions which have a relation with entrance and exit channels of the reaction. Based on the individual CEDPICS, the electronic structure of molecules can also be elucidated.

Atomic Cholesky decompositions: a route to unbiased auxiliary basis sets for density fitting approximation with tunable accuracy and efficiency.

PubMed

Aquilante, Francesco; Gagliardi, Laura; Pedersen, Thomas Bondo; Lindh, Roland

2009-04-21

Cholesky decomposition of the atomic two-electron integral matrix has recently been proposed as a procedure for automated generation of auxiliary basis sets for the density fitting approximation [F. Aquilante et al., J. Chem. Phys. 127, 114107 (2007)]. In order to increase computational performance while maintaining accuracy, we propose here to reduce the number of primitive Gaussian functions of the contracted auxiliary basis functions by means of a second Cholesky decomposition. Test calculations show that this procedure is most beneficial in conjunction with highly contracted atomic orbital basis sets such as atomic natural orbitals, and that the error resulting from the second decomposition is negligible. We also demonstrate theoretically as well as computationally that the locality of the fitting coefficients can be controlled by means of the decomposition threshold even with the long-ranged Coulomb metric. Cholesky decomposition-based auxiliary basis sets are thus ideally suited for local density fitting approximations.

Atomic Cholesky decompositions: A route to unbiased auxiliary basis sets for density fitting approximation with tunable accuracy and efficiency

NASA Astrophysics Data System (ADS)

Aquilante, Francesco; Gagliardi, Laura; Pedersen, Thomas Bondo; Lindh, Roland

2009-04-01

Cholesky decomposition of the atomic two-electron integral matrix has recently been proposed as a procedure for automated generation of auxiliary basis sets for the density fitting approximation [F. Aquilante et al., J. Chem. Phys. 127, 114107 (2007)]. In order to increase computational performance while maintaining accuracy, we propose here to reduce the number of primitive Gaussian functions of the contracted auxiliary basis functions by means of a second Cholesky decomposition. Test calculations show that this procedure is most beneficial in conjunction with highly contracted atomic orbital basis sets such as atomic natural orbitals, and that the error resulting from the second decomposition is negligible. We also demonstrate theoretically as well as computationally that the locality of the fitting coefficients can be controlled by means of the decomposition threshold even with the long-ranged Coulomb metric. Cholesky decomposition-based auxiliary basis sets are thus ideally suited for local density fitting approximations.

Structure assignment, electronic properties, and magnetism quenching of endohedrally doped neutral silicon clusters, Si(n)Co (n = 10-12).

PubMed

Li, Yejun; Tam, Nguyen Minh; Claes, Pieterjan; Woodham, Alex P; Lyon, Jonathan T; Ngan, Vu Thi; Nguyen, Minh Tho; Lievens, Peter; Fielicke, André; Janssens, Ewald

2014-09-18

The structures of neutral cobalt-doped silicon clusters have been assigned by a combined experimental and theoretical study. Size-selective infrared spectra of neutral Si(n)Co (n = 10-12) clusters are measured using a tunable IR-UV two-color ionization scheme. The experimental infrared spectra are compared with calculated spectra of low-energy structures predicted at the B3P86 level of theory. It is shown that the Si(n)Co (n = 10-12) clusters have endohedral caged structures, where the silicon frameworks prefer double-layered structures encapsulating the Co atom. Electronic structure analysis indicates that the clusters are stabilized by an ionic interaction between the Co dopant atom and the silicon cage due to the charge transfer from the silicon valence sp orbitals to the cobalt 3d orbitals. Strong hybridization between the Co dopant atom and the silicon host quenches the local magnetic moment on the encapsulated Co atom.

Effects of anisotropic electron-ion interactions in atomic photoelectron angular distributions

NASA Technical Reports Server (NTRS)

Dill, D.; Starace, A. F.; Manson, S. T.

1974-01-01

The photoelectron asymmetry parameter beta in LS-coupling is obtained as an expansion into contributions from alternative angular momentum transfers j sub t. The physical significance of this expansion of beta is shown to be that: (1) the electric dipole interaction transfers to the atom a charcteristic single angular momentum j sub t = sub o, where sub o is the photoelectron's initial orbital momentum; and (2) angular momentum transfers indicate the presence of anisotropic interaction of the outgoing photoelectron with the residual ion. For open shell atoms the photoelectron-ion interaction is generally anisotropic; photoelectron phase shifts and electric dipole matrix elements depend on both the multiplet term of the residual ion and the total orbital momentum of the ion-photoelectron final state channel. Consequently beta depends on the term levels of the residual ion and contains contributions from all allowed values of j sub t. Numerical calculations of the asymmetry parameters and partial cross sections for photoionization of atomic sulfur are presented.

Spin-orbit coupling effect on structural and magnetic properties of ConRh13-n (n = 0-13) clusters

NASA Astrophysics Data System (ADS)

Bai, Xi; Lv, Jin; Zhang, Fu-Qiang; Jia, Jian-Feng; Wu, Hai-Shun

2018-04-01

The effect of spin-orbit interaction on the structures and magnetism of ConRh13-n (n = 0-13) clusters have been systematically investigated by using the spin-orbit coupling (SOC) implementation of the density functional theory (DFT). The results calculated without SOC (NSOC) show that Rh13 prefers the double simple-cubic configuration, and icosahedron is the favorable structure for n = 1-9, while n ≥ 10, clusters favor the hexagonal bilayer structure. The inclusion of SOC in calculation does not change the geometries of clusters. Compared with that in NSOC calculation, although the binding energy per atom in clusters with same composition decreases in SOC calculation, the relative stability of clusters with different compositions does not change. An interesting result is that the spin moments of clusters for n = 1-9 are almost constant (21 μB). Spin-orbit interaction recovers orbital moment and its anisotropy by removing crystal-field effect in calculation. The destruction of bonding symmetry and relaxation of bonding account for high anisotropies of orbital moments in Co11Rh2 and CoRh12 clusters. With atomic composition (Co/Rh) around 4/9-5/8 and 9/4, the Co-Rh clusters exhibit high magnetic anisotropy energies.

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

Ünlü, Hilmi, E-mail: hunlu@itu.edu.tr

We propose a non-orthogonal sp{sup 3} hybrid bond orbital model to determine the electronic properties of semiconductor heterostructures. The model considers the non-orthogonality of sp{sup 3} hybrid states of nearest neighboring adjacent atoms using the intra-atomic Coulomb interactions corrected Hartree-Fock atomic energies and metallic contribution to calculate the valence band width energies of group IV elemental and group III-V and II-VI compound semiconductors without any adjustable parameter.

Atomic Data for the K-vacancy States of Fe XXIV

NASA Technical Reports Server (NTRS)

Bautista, M. A.; Mendoza, C.; Kallman, T. R.; Palmeri, P.

2003-01-01

As part of a project to compute improved atomic data for the spectral modeling of iron K lines, we report extensive calculations and comparisons of atomic data for K-vacancy states in Fe XXIV. The data sets include: (i) energy levels, line wavelengths, radiative and Auger rates; (ii) inner-shell electron impact excitation rates and (iii) fine structure inner-shell photoionization cross sections. The calculations of energy levels and radiative and Auger rates have involved a detailed study of orbital representations, core relaxation, configuration interaction, relativistic corrections, cancellation effects and semi-empirical corrections. It is shown that a formal treatment of the Breit interaction is essential to render the important magnetic correlations that take part in the decay pathways of this ion. As a result, the accuracy of the present A-values is firmly ranked at better than 10% while that of the Auger rates at only 15%. The calculations of collisional excitation and photoionization cross sections take into account the effects of radiation and spectator Auger dampings. In the former, these effects cause significant attenuation of resonances leading to a good agreement with a simpler method where resonances are excluded. In the latter, resonances converging to the K threshold display symmetric profiles of constant width that causes edge smearing.

Atomic Data for the K-Vacancy States of Fe XXIV

NASA Technical Reports Server (NTRS)

Bautista, M. A.; Mendoza, C.; Kallman, T. R.; Palmeri, P.

2002-01-01

As part of a project to compute improved atomic data for the spectral modeling of iron K lines, we report extensive calculations and comparisons of atomic data for K-vacancy states in Fe XXIV. The data sets include: (i) energy levels, line wavelengths, radiative and Auger rates; (ii) inner-shell electron impact excitation rates and (iii) fine structure inner-shell photoionization cross sections. The calculations of energy levels and radiative and Auger rates have involved a detailed study of orbital representations, core relaxation, configuration interaction, relativistic corrections, cancellation effects and semi-empirical corrections. It is shown that a formal treatment of the Breit interaction is essential to render the important magnetic correlations that take part in the decay pathways of this ion. As a result, the accuracy of the present A-values is firmly ranked at better than 10% while that of the Auger rates at only 15%. The calculations of collisional excitation and photoionization cross sections take into account the effects of radiation and spectator Auger dampings. In the former, these effects cause significant attenuation of resonances leading to a good agreement with a simpler method where resonances are excluded. In the latter, resonances converging to the K threshold display symmetric profiles of constant width that causes edge smearing.

Influence of Atomic Oxygen Exposure on Friction Behavior of 321 Stainless Steel

NASA Astrophysics Data System (ADS)

Liu, Y.; Yang, J.; Ye, Z.; Dong, S.; Zhang, L.; Zhang, Z.

Atomic oxygen (AO) exposure testing has been conducted on a 321 stainless steel rolled 1 mm thick sheet to simulate the effect of AO environment on steel in low Earth orbit (LEO). An atomic oxygen exposure facility was employed to carry out AO experiments with the fluence up to ~1021 atom/cm2. The AO exposed specimens were evaluated in air at room temperature using a nanoindenter and a tribological system. The exposed surfaces were analyzed usign XPS technique.

Advancing Navigation, Timing, and Science with the Deep Space Atomic Clock

NASA Technical Reports Server (NTRS)

Ely, Todd A.; Seubert, Jill; Bell, Julia

2014-01-01

NASA's Deep Space Atomic Clock mission is developing a small, highly stable mercury ion atomic clock with an Allan deviation of at most 1e-14 at one day, and with current estimates near 3e-15. This stability enables one-way radiometric tracking data with accuracy equivalent to and, in certain conditions, better than current two-way deep space tracking data; allowing a shift to a more efficient and flexible one-way deep space navigation architecture. DSAC-enabled one-way tracking will benefit navigation and radio science by increasing the quantity and quality of tracking data. Additionally, DSAC would be a key component to fully-autonomous onboard radio navigation useful for time-sensitive situations. Potential deep space applications of DSAC are presented, including orbit determination of a Mars orbiter and gravity science on a Europa flyby mission.

Atomic oxygen effects on spacecraft materials: The state of the art of our knowledge

NASA Technical Reports Server (NTRS)

Koontz, Steven L.

1989-01-01

In the flight materials exposure data base extensive quantitative data is available from limited exposures in a narrow range of orbital environments. More data is needed in a wider range of environments as well as longer exposure times. Synergistic effects with other environmental factors; polar orbit and higher altitude environments; and real time materials degradation data is needed to understand degradation kinetics and mechanism. Almost no laboratory data exists from high fidelity simulations of the LEO environment. Simulation and test system are under development, and the data base is scanty. Theoretical understanding of hyperthermal atom surface reactions in the LEO environment is not good enough to support development of reliable accelerated test methods. The laser sustained discharge, atom beam sources are the most promising high fidelity simulation-test systems at this time.

"Doping" pentacene with sp(2)-phosphorus atoms: towards high performance ambipolar semiconductors.

PubMed

Long, Guankui; Yang, Xuan; Chen, Wangqiao; Zhang, Mingtao; Zhao, Yang; Chen, Yongsheng; Zhang, Qichun

2016-01-28

Recent research progress in black phosphorus sheets strongly encourages us to employ pentacene as a parent system to systematically investigate how the "doping" of sp(2)-phosphorus atoms onto the backbone of pentacene influences its optical and charge transport properties. Our theoretical investigations proved that increasing the contribution of the pz atomic orbital of the sp(2)-phosphorus to the frontier molecular orbital of phosphapentacenes could significantly decrease both hole and electron reorganization energies and dramatically red-shift the absorption of pentacene. The record smallest hole and electron reorganization energies of 69.80 and 95.74 meV for heteropentacene derivatives were obtained. These results suggest that phosphapentacenes (or phosphaacenes) could be potential promising candidates to achieve both higher and balanced mobilities in organic field effect transistors and realize a better power conversion efficiency in organic photovoltaics.

Students' Levels of Explanations, Models, and Misconceptions in Basic Quantum Chemistry: A Phenomenographic Study

ERIC Educational Resources Information Center

Stefani, Christina; Tsaparlis, Georgios

2009-01-01

We investigated students' knowledge constructions of basic quantum chemistry concepts, namely atomic orbitals, the Schrodinger equation, molecular orbitals, hybridization, and chemical bonding. Ausubel's theory of meaningful learning provided the theoretical framework and phenomenography the method of analysis. The semi-structured interview with…

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…

Towards a global model of spin-orbit coupling in the halocarbenes

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

Nyambo, Silver; Karshenas, Cyrus; Reid, Scott A., E-mail: scott.reid@marquette.edu, E-mail: dawesr@mst.edu

We report a global analysis of spin-orbit coupling in the mono-halocarbenes, CH(D)X, where X = Cl, Br, and I. These are model systems for examining carbene singlet-triplet energy gaps and spin-orbit coupling. Over the past decade, rich data sets collected using single vibronic level emission spectroscopy and stimulated emission pumping spectroscopy have yielded much information on the ground vibrational level structure and clearly demonstrated the presence of perturbations involving the low-lying triplet state. To model these interactions globally, we compare two approaches. First, we employ a diabatic treatment of the spin-orbit coupling, where the coupling matrix elements are written inmore » terms of a purely electronic spin-orbit matrix element which is independent of nuclear coordinates, and an integral representing the overlap of the singlet and triplet vibrational wavefunctions. In this way, the structures, harmonic frequencies, and normal mode displacements from ab initio calculations were used to calculate the vibrational overlaps of the singlet and triplet state levels, including the full effects of Duschinsky mixing. These calculations have allowed many new assignments to be made, particularly for CHI, and provided spin-orbit coupling parameters and values for the singlet-triplet gaps. In a second approach, we have computed and fit full geometry dependent spin-orbit coupling surfaces and used them to compute matrix elements without the product form approximation. Those matrix elements were used in similar fits varying the anharmonic constants and singlet-triplet gap to reproduce the experimental levels. The derived spin-orbit parameters for carbenes CHX (X = Cl, Br, and I) show an excellent linear correlation with the atomic spin-orbit constant of the corresponding halogen, indicating that the spin-orbit coupling in the carbenes is consistently around 14% of the atomic value.« less

Simulation of charge transfer and orbital rehybridization in molecular and condensed matter systems

NASA Astrophysics Data System (ADS)

Nistor, Razvan A.

The mixing and shifting of electronic orbitals in molecules, or between atoms in bulk systems, is crucially important to the overall structure and physical properties of materials. Understanding and accurately modeling these orbital interactions is of both scientific and industrial relevance. Electronic orbitals can be perturbed in several ways. Doping, adding or removing electrons from systems, can change the bond-order and the physical properties of certain materials. Orbital rehybridization, driven by either thermal or pressure excitation, alters the short-range structure of materials and changes their long-range transport properties. Macroscopically, during bond formation, the shifting of electronic orbitals can be interpreted as a charge transfer phenomenon, as electron density may pile up around, and hence, alter the effective charge of, a given atom in the changing chemical environment. Several levels of theory exist to elucidate the mechanisms behind these orbital interactions. Electronic structure calculations solve the time-independent Schrodinger equation to high chemical accuracy, but are computationally expensive and limited to small system sizes and simulation times. Less fundamental atomistic calculations use simpler parameterized functional expressions called force-fields to model atomic interactions. Atomistic simulations can describe systems and time-scales larger and longer than electronic-structure methods, but at the cost of chemical accuracy. In this thesis, both first-principles and phenomenological methods are addressed in the study of several encompassing problems dealing with charge transfer and orbital rehybridization. Firstly, a new charge-equilibration method is developed that improves upon existing models to allow next-generation force-fields to describe the electrostatics of changing chemical environments. Secondly, electronic structure calculations are used to investigate the doping dependent energy landscapes of several high-temperature superconducting materials in order to parameterize the apparently large nonlinear electron-phonon coupling. Thirdly, ab initio simulations are used to investigate the role of pressure-driven structural re-organization in the crystalline-to-amorphous (or, metallic-to-insulating) transition of a common binary phase-change material composed of Ge and Sb. Practical applications of each topic will be discussed. Keywords. Charge-equilibration methods, molecular dynamics, electronic structure calculations, ab initio simulations, high-temperature superconductors, phase-change materials.

The Materials Chemistry of Atomic Oxygen with Applications to Anisotropic Etching of Submicron Structures in Microelectronics and the Surface Chemistry Engineering of Porous Solids

NASA Technical Reports Server (NTRS)

Koontz, Steve L.; Leger, Lubert J.; Wu, Corina; Cross, Jon B.; Jurgensen, Charles W.

1994-01-01

Neutral atomic oxygen is the most abundant component of the ionospheric plasma in the low Earth orbit environment (LEO; 200 to 700 kilometers altitude) and can produce significant degradation of some spacecraft materials. In order to produce a more complete understanding of the materials chemistry of atomic oxygen, the chemistry and physics of O-atom interactions with materials were determined in three radically different environments: (1) The Space Shuttle cargo bay in low Earth orbit (the EOIM-3 space flight experiment), (2) a high-velocity neutral atom beam system (HVAB) at Los Alamos National Laboratory (LANL), and (3) a microwave-plasma flowing-discharge system at JSC. The Space Shuttle and the high velocity atom beam systems produce atom-surface collision energies ranging from 0.1 to 7 eV (hyperthermal atoms) under high-vacuum conditions, while the flowing discharge system produces a 0.065 eV surface collision energy at a total pressure of 2 Torr. Data obtained in the three different O-atom environments referred to above show that the rate of O-atom reaction with polymeric materials is strongly dependent on atom kinetic energy, obeying a reactive scattering law which suggests that atom kinetic energy is directly available for overcoming activation barriers in the reaction. General relationships between polymer reactivity with O atoms and polymer composition and molecular structure have been determined. In addition, vacuum ultraviolet photochemical effects have been shown to dominate the reaction of O atoms with fluorocarbon polymers. Finally, studies of the materials chemistry of O atoms have produced results which may be of interest to technologists outside the aerospace industry. Atomic oxygen 'spin-off' or 'dual use' technologies in the areas of anisotropic etching in microelectronic materials and device processing, as well as surface chemistry engineering of porous solid materials are described.

2001 Mars Odyssey Project report

NASA Technical Reports Server (NTRS)

Spencer, D. A.; Gibbs, R. G.; Mase, R. A.; Plaut, J. J.; Saunders, R. S.

2002-01-01

The Mars Odyssey orbiter was launched on April 7, 2001, and arrived at Mars on October 24, 2001. The orbiter carries scientific instruments that will determine surface elemental composition, mineralogy and morphology, and measure the Mars radiation environment from orbit. In addition, the orbiter will serve as a data relay for future surface missions. This paper will present an overview of the Odyssey project, including the key elements of the spacecraft design, mission design and navigation, mission operations, and the science approach. The project's risk management process will be described. Initial findings of the science team will be summarized.

Quasi-relativistic modeltotential approach. Spin-orbit effects on energies and geometries of several di- and tri-atomic molecules

NASA Astrophysics Data System (ADS)

Hafner, P.; Habitz, P.; Ishikawa, Y.; Wechsel-Trakowski, E.; Schwarz, W. H. E.

1981-06-01

Calculations on ground and valence-excited states of Au +2, Tl 2 and Pb 2, and on the ground states of HgCl 2, PbCl 2 and PbH 2 have teen performed within the Kramers-restricteu self-consistent-field approach using a quasi-relativitistic model-potential hamiltonian. The influence of spin—orbit coupling on molecular orbitals, bond energies and geometries is discussed.

NanoLaunch

NASA Technical Reports Server (NTRS)

Jones, Jonathan; Harris, Lawanna

2015-01-01

NASA's NanoLaunch effort will provide the framework to mature both Earth-to-orbit and on-orbit propulsion and avionics technologies while also providing affordable, dedicated access to low-Earth orbit for CubeSat-class payloads. The project will also serve as an early career personnel training opportunity with mentors to gain hands-on project experience.

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

Thayer, K.J.

The past year has seen several of the Physics Division`s new research projects reach major milestones with first successful experiments and results: the atomic physics station in the Basic Energy Sciences Research Center at the Argonne Advanced Photon Source was used in first high-energy, high-brilliance x-ray studies in atomic and molecular physics; the Short Orbit Spectrometer in Hall C at the Thomas Jefferson National Accelerator (TJNAF) Facility that the Argonne medium energy nuclear physics group was responsible for, was used extensively in the first round of experiments at TJNAF; at ATLAS, several new beams of radioactive isotopes were developed andmore » used in studies of nuclear physics and nuclear astrophysics; the new ECR ion source at ATLAS was completed and first commissioning tests indicate excellent performance characteristics; Quantum Monte Carlo calculations of mass-8 nuclei were performed for the first time with realistic nucleon-nucleon interactions using state-of-the-art computers, including Argonne`s massively parallel IBM SP. At the same time other future projects are well under way: preparations for the move of Gammasphere to ATLAS in September 1997 have progressed as planned. These new efforts are imbedded in, or flowing from, the vibrant ongoing research program described in some detail in this report: nuclear structure and reactions with heavy ions; measurements of reactions of astrophysical interest; studies of nucleon and sub-nucleon structures using leptonic probes at intermediate and high energies; atomic and molecular structure with high-energy x-rays. The experimental efforts are being complemented with efforts in theory, from QCD to nucleon-meson systems to structure and reactions of nuclei. Finally, the operation of ATLAS as a national users facility has achieved a new milestone, with 5,800 hours beam on target for experiments during the past fiscal year.« less

Texturing Carbon-carbon Composite Radiator Surfaces Utilizing Atomic Oxygen

NASA Technical Reports Server (NTRS)

Raack, Taylor

2004-01-01

Future space nuclear power systems will require radiator technology to dissipate excess heat created by a nuclear reactor. Large radiator fins with circulating coolant are in development for this purpose and an investigation of how to make them most efficient is underway. Maximizing the surface area while minimizing the mass of such radiator fins is critical for obtaining the highest efficiency in dissipating heat. Processes to develop surface roughness are under investigation to maximize the effective surface area of a radiator fin. Surface roughness is created through several methods including oxidation and texturing. The effects of atomic oxygen impingement on carbon-carbon surfaces are currently being investigated for texturing a radiator surface. Early studies of atomic oxygen impingement in low Earth orbit indicate significant texturing due to ram atomic oxygen. The surface morphology of the affected surfaces shows many microscopic cones and valleys which have been experimentally shown to increase radiation emittance. Further study of this morphology proceeded in the Long Duration Exposure Facility (LDEF). Atomic oxygen experiments on the LDEF successfully duplicated the results obtained from materials in spaceflight by subjecting samples to 4.5 eV atomic oxygen from a fixed ram angle. These experiments replicated the conical valley morphology that was seen on samples subjected to low Earth orbit.

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.

Intelsat solar array coupon atomic oxygen flight experiment

NASA Technical Reports Server (NTRS)

Koontz, S.; King, G.; Dunnet, A.; Kirkendahl, T.; Linton, R.; Vaughn, J.

1994-01-01

A Hughes communications satellite (INTELSAT series) belonging to the INTELSAT Organization was marooned in low-Earth orbit (LEO) on March 14, 1990, following failure of the Titan launch vehicle third stage to separate properly. The satellite, INTELSAT 6, was designed for service in geosynchronous orbit and contains several materials that are potentially susceptible to attack by atomic oxygen. Analysis showed that direct exposure of the silver interconnects in the satellite photovoltaic array to atomic oxygen in LEO was the key materials issue. Available data on atomic oxygen degradation of silver are limited and show high variance, so solar array configurations of the INTELSAT 6 type and individual interconnects were tested in ground-based facilities and during STS-41 (Space Shuttle Discovery, October 1990) as part of the ISAC flight experiment. Several materials for which little or no flight data exist were also tested for atomic oxygen reactivity. Dry lubricants, elastomers, and polymeric and inorganic materials were exposed to an oxygen atom fluence of 1.1 x 10(exp 20) atoms cm(exp 2). Many of the samples were selected to support Space Station Freedom design and decision making. This paper provides an overview of the ISAC flight experiment and a brief summary of results. In addition to new data on materials not before flown, ISAC provided data supporting the decision to rescue INTELSAT 6, which was successfully undertaken in May 1992.

Quantum-projection-noise-limited interferometry with coherent atoms in a Ramsey-type setup

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

Doering, D.; McDonald, G.; Debs, J. E.

2010-04-15

Every measurement of the population in an uncorrelated ensemble of two-level systems is limited by what is known as the quantum projection noise limit. Here, we present quantum-projection-noise-limited performance of a Ramsey-type interferometer using freely propagating coherent atoms. The experimental setup is based on an electro-optic modulator in an inherently stable Sagnac interferometer, optically coupling the two interfering atomic states via a two-photon Raman transition. Going beyond the quantum projection noise limit requires the use of reduced quantum uncertainty (squeezed) states. The experiment described demonstrates atom interferometry at the fundamental noise level and allows the observation of possible squeezing effectsmore » in an atom laser, potentially leading to improved sensitivity in atom interferometers.« less

A Simple Relativistic Bohr Atom

ERIC Educational Resources Information Center

Terzis, Andreas F.

2008-01-01

A simple concise relativistic modification of the standard Bohr model for hydrogen-like atoms with circular orbits is presented. As the derivation requires basic knowledge of classical and relativistic mechanics, it can be taught in standard courses in modern physics and introductory quantum mechanics. In addition, it can be shown in a class that…

Photoelectron spectroscopy of heavy atoms and molecules

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

White, M.G.

1979-07-01

The importance of relativistic interactions in the photoionization of heavy atoms and molecules has been investigated by the technique of photoelectron spectroscopy. In particular, experiments are reported which illustrate the effects of the spin-orbit interaction in the neutral ground state, final ionic states and continuum states of the photoionization target.

Band gap modulation of graphene by metal substrate: A first principles study

NASA Astrophysics Data System (ADS)

Sahoo, Mihir Ranjan; Sahu, Sivabrata; Kushwaha, Anoop Kumar; Nayak, S. K.

2018-04-01

Due to high in-plane charge carrier mobility with high electron velocity and long spin diffusion length, graphene guarantees as a completely unique material for devices with various applications. Unaffected 2pz orbitals of carbon atoms in graphene can be highly influenced by substrates and leads to tuning in electronic properties. We report here a density functional calculation of graphene monolayer based on metallic substrate like nickel surfaces. Band-gap of graphene near K points opens due to interactions between 2pz and d-orbitals of nickel atoms and the gap modulation can be done with the increasing number of layers of substrates.

Hydrogen doping in HfO{sub 2} resistance change random access memory

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

Duncan, D.; Magyari-Köpe, B.; Nishi, Y.

2016-01-25

The structures and energies of hydrogen-doped monoclinic hafnium dioxide were calculated using density-functional theory. The electronic interactions are described within the LDA + U formalism, where on-site Coulomb corrections are applied to the 5d orbital electrons of Hf atoms and 2p orbital electrons of the O atoms. The effects of charge state, defect-defect interactions, and hydrogenation are investigated and compared with experiment. It is found that hydrogenation of HfO{sub 2} resistance-change random access memory devices energetically stabilizes the formation of oxygen vacancies and conductive vacancy filaments through multiple mechanisms, leading to improved switching characteristic and device yield.

Creating Spin-One Fermions in the Presence of Artificial Spin-Orbit Fields: Emergent Spinor Physics and Spectroscopic Properties

NASA Astrophysics Data System (ADS)

Kurkcuoglu, Doga Murat; de Melo, C. A. R. Sá

2018-05-01

We propose the creation and investigation of a system of spin-one fermions in the presence of artificial spin-orbit coupling, via the interaction of three hyperfine states of fermionic atoms to Raman laser fields. We explore the emergence of spinor physics in the Hamiltonian described by the interaction between light and atoms, and analyze spectroscopic properties such as dispersion relation, Fermi surfaces, spectral functions, spin-dependent momentum distributions and density of states. Connections to spin-one bosons and SU(3) systems is made, as well relations to the Lifshitz transition and Pomeranchuk instability are presented.

Photoionization of sodium atoms and electron scattering from ionized sodium

NASA Technical Reports Server (NTRS)

Dasgupta, A.; Bhatia, A. K.

1985-01-01

The polarized-orbital method of Temkin (1957) is applied using polarized orbitals determined from Sternheimer's equation to compute the photoionization cross sections of Na atoms from threshold to about 60 eV. The approximations involved in the analysis are explained in detail; the explicit forms of the integrals and matrix expressions are given in appendices; and the results are presented in tables and graphs. Good agreement is found with the results of Chang and Kelly (1975), and the possibility that small amounts of molecular vapor in Na-photoionization experiments are responsible for the discrepancies between calculated and measured cross sections is considered.

Spatial intensity distribution of controlled-NOT gate carrying orbital angular momentum via photonic band gap structure

NASA Astrophysics Data System (ADS)

Zhang, Yan; Wang, Xiaorui; Zhe Zhang, Yun

2018-07-01

By employing the different topological charges of a Laguerre–Gaussian beam as a qubit, we experimentally demonstrate a controlled-NOT (CNOT) gate with light beams carrying orbital angular momentum via a photonic band gap structure in a hot atomic ensemble. Through a degenerate four-wave mixing process, the spatial distribution of the CNOT gate including splitting and spatial shift can be affected by the Kerr nonlinear effect in multilevel atomic systems. Moreover, the intensity variations of the CNOT gate can be controlled by the relative phase modulation. This research can be useful for applications in quantum information processing.

Rydberg Atoms in Strong Fields: a Testing Ground for Quantum Chaos.

NASA Astrophysics Data System (ADS)

Courtney, Michael

1995-01-01

Rydberg atoms in strong static electric and magnetic fields provide experimentally accessible systems for studying the connections between classical chaos and quantum mechanics in the semiclassical limit. This experimental accessibility has motivated the development of reliable quantum mechanical solutions. This thesis uses both experimental and computed quantum spectra to test the central approaches to quantum chaos. These central approaches consist mainly of developing methods to compute the spectra of quantum systems in non -perturbative regimes, correlating statistical descriptions of eigenvalues with the classical behavior of the same Hamiltonian, and the development of semiclassical methods such as periodic-orbit theory. Particular emphasis is given to identifying the spectral signature of recurrences --quantum wave packets which follow classical orbits. The new findings include: the breakdown of the connection between energy-level statistics and classical chaos in odd-parity diamagnetic lithium, the discovery of the signature of very long period orbits in atomic spectra, quantitative evidence for the scattering of recurrences by the alkali -metal core, quantitative description of the behavior of recurrences near bifurcations, and a semiclassical interpretation of the evolution of continuum Stark spectra. (Copies available exclusively from MIT Libraries, Rm. 14-0551, Cambridge, MA 02139-4307. Ph. 617-253-5668; Fax 617-253-1690.).

Correlated motion of electrons in the He atom irradiated with coherent light

NASA Astrophysics Data System (ADS)

Someda, Kiyohiko

2018-05-01

Correlated motion of electrons in the He atom irradiated with linearly polarised light is discussed. Mixing of the 2pz orbital into the 1s orbital is interpreted as motion of an electron along the z-axis. The transitions to the configurations (1s)(2pz) and (2pz)(2pz) from (1s)(1s) are described by using 1s-2pz hybridised orbitals with variable coefficients of hybridisation, in other words, by using the Thouless parameters. The quasi-eigenstates of the atom in stationary light are obtained on the basis of the Floquet formalism, and the behaviour of the Thouless parameters is analysed. Trajectories of time evolution of the Thouless parameters are found to be useful to grasp the motion of electrons. Shapes of the trajectories are classified into four modes: (1) two electrons try to stay away from each other due to Coulomb repulsion, (2) one of the electrons is solely driven to run, (3) two electrons are driven to travel together and (4) two electrons run anti-parallel with each other. The conditions of intensity and frequency of light causing these four modes are clarified and summarised in a kind of phase diagram.

New hybrid lead iodides: From one-dimensional chain to two-dimensional layered perovskite structure

NASA Astrophysics Data System (ADS)

Xiong, Kecai; Liu, Wei; Teat, Simon J.; An, Litao; Wang, Hao; Emge, Thomas J.; Li, Jing

2015-10-01

Two new hybrid lead halides (H2BDA)[PbI4] (1) (H2BDA=1,4-butanediammonium dication) and (HNPEIM)[PbI3] (2) (HNPEIM=N-​phenyl-ethanimidamidine cation) have been synthesized and structurally characterized. X-ray diffraction analyses reveal that compound 1 features a two-dimensional corner-sharing perovskite layer whereas compound 2 contains one-dimensional edge-sharing double chains. The N-​phenyl-ethanimidamidine cation within compound 2 was generated in-situ under solvothermal conditions. The optical absorption spectra collected at room temperature suggest that both compounds are semiconductors having direct band gaps, with estimated values of 2.64 and 2.73 eV for 1 and 2, respectively. Results from the density functional theory (DFT) calculations are consistent with the experimental data. Density of states (DOS) analysis reveals that in both compounds 1 and 2, the energy states in the valence band maximum region are iodine 5p atomic orbitals with a small contribution from lead 6s, while in the region of conduction band minimum, the major contributions are from the inorganic (Pb 6p atomic orbitals) and organic components (C and N 2p atomic orbitals) in compound 1 and 2, respectively.

Ultra-fast computation of electronic spectra for large systems by tight-binding based simplified Tamm-Dancoff approximation (sTDA-xTB)

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

Grimme, Stefan, E-mail: grimme@thch.uni-bonn.de; Bannwarth, Christoph

2016-08-07

The computational bottleneck of the extremely fast simplified Tamm-Dancoff approximated (sTDA) time-dependent density functional theory procedure [S. Grimme, J. Chem. Phys. 138, 244104 (2013)] for the computation of electronic spectra for large systems is the determination of the ground state Kohn-Sham orbitals and eigenvalues. This limits such treatments to single structures with a few hundred atoms and hence, e.g., sampling along molecular dynamics trajectories for flexible systems or the calculation of chromophore aggregates is often not possible. The aim of this work is to solve this problem by a specifically designed semi-empirical tight binding (TB) procedure similar to the wellmore » established self-consistent-charge density functional TB scheme. The new special purpose method provides orbitals and orbital energies of hybrid density functional character for a subsequent and basically unmodified sTDA procedure. Compared to many previous semi-empirical excited state methods, an advantage of the ansatz is that a general eigenvalue problem in a non-orthogonal, extended atomic orbital basis is solved and therefore correct occupied/virtual orbital energy splittings as well as Rydberg levels are obtained. A key idea for the success of the new model is that the determination of atomic charges (describing an effective electron-electron interaction) and the one-particle spectrum is decoupled and treated by two differently parametrized Hamiltonians/basis sets. The three-diagonalization-step composite procedure can routinely compute broad range electronic spectra (0-8 eV) within minutes of computation time for systems composed of 500-1000 atoms with an accuracy typical of standard time-dependent density functional theory (0.3-0.5 eV average error). An easily extendable parametrization based on coupled-cluster and density functional computed reference data for the elements H–Zn including transition metals is described. The accuracy of the method termed sTDA-xTB is first benchmarked for vertical excitation energies of open- and closed-shell systems in comparison to other semi-empirical methods and applied to exemplary problems in electronic spectroscopy. As side products of the development, a robust and efficient valence electron TB method for the accurate determination of atomic charges as well as a more accurate calculation scheme of dipole rotatory strengths within the Tamm-Dancoff approximation is proposed.« less

Resonance of an unshared electron pair between two atoms connected by a single bond

PubMed Central

Pauling, Linus

1983-01-01

The reported structure of the dimer of a compound of bicovalent tin indicates that the tin-tin bond is of a new type. It can be described as involving resonance between two structures in which there is transfer of an electron pair from one tin atom to the other. The tin atoms are connected by a single covalent bond (each also forms two covalent bonds with carbon atoms), and an unshared electron pair resonates between the fourth sp3 orbitals of the two atoms. Similar structures probably occur in digermene and distannene. PMID:16593329

Simple iterative construction of the optimized effective potential for orbital functionals, including exact exchange.

PubMed

Kümmel, Stephan; Perdew, John P

2003-01-31

For exchange-correlation functionals that depend explicitly on the Kohn-Sham orbitals, the potential V(xcsigma)(r) must be obtained as the solution of the optimized effective potential (OEP) integral equation. This is very demanding and has limited the use of orbital functionals. We demonstrate that instead the OEP can be obtained iteratively by solving the partial differential equations for the orbital shifts that exactify the Krieger-Li-Iafrate approximation. Unoccupied orbitals do not need to be calculated. Accuracy and efficiency of the method are shown for atoms and clusters using the exact-exchange energy. Counterintuitive asymptotic limits of the exact OEP are presented.

Persistent three- and four-atom orbital molecules in the spinel Al V2O4

NASA Astrophysics Data System (ADS)

Browne, Alexander J.; Kimber, Simon A. J.; Attfield, J. Paul

2017-10-01

Electronic instabilities in transition-metal compounds may lead to ground states containing orbital molecules when direct metal-metal orbital interactions occur. The spinel Al V2O4 was reported to contain V717 + orbital heptamers that emerge below a 700 K charge ordering transition. Our x-ray total scattering analysis of Al V2O4 between 300 and 1100 K reveals a very different picture as the postulated heptamers are found to be pairs of spin-singlet V39 + trimers and V48 + tetramers, and these orbital molecules persist to at least 1100 K in a disordered high-temperature cubic phase.

Three orbital transfer vehicles

NASA Technical Reports Server (NTRS)

1990-01-01

Aerospace engineering students at the Virginia Polytechnic Institute and State University undertook three design projects under the sponsorship of the NASA/USRA Advanced Space Design Program. All three projects addressed cargo and/or crew transportation between low Earth orbit and geosynchronous Earth orbit. Project SPARC presents a preliminary design of a fully reusable, chemically powered aeroassisted vehicle for a transfer of a crew of five and a 6000 to 20000 pound payload. The ASTV project outlines a chemically powered aeroassisted configuration that uses disposable tanks and a relatively small aerobrake to realize propellant savings. The third project, LOCOST, involves a reusable, hybrid laser/chemical vehicle designed for large cargo (up to 88,200 pounds) transportation.

First-principles investigation of graphitic carbon nitride monolayer with embedded Fe atom

NASA Astrophysics Data System (ADS)

Abdullahi, Yusuf Zuntu; Yoon, Tiem Leong; Halim, Mohd Mahadi; Hashim, Md. Roslan; Lim, Thong Leng

2018-01-01

Density-functional theory (DFT) calculations with spin-polarized generalized gradient approximation and Hubbard U correction are carried out to investigate the mechanical, structural, electronic and magnetic properties of graphitic heptazine with embedded Fe atom under bi-axial tensile strain and applied perpendicular electric field. It was found that the binding energy of heptazine with embedded Fe atom system decreases as larger tensile strain is applied, while it increases as larger electric field strength is applied. Our calculations also predict a band gap at a peak value of 5% tensile strain but at expense of the structural stability of the system. The band gap open up at 5% tensile strain is due to distortion in the structure caused by the repulsive effect in the cavity between the lone pairs of the edge nitrogen atoms and dxy /dx2 -y2 orbital of Fe atom, forcing the unoccupied pz- orbital is forced to shift toward higher energy. The electronic and magnetic properties of the heptazine with embedded Fe system under perpendicular electric field up to a peak value of 8 V/nm is also well preserved despite an obvious buckled structure. Such properties are desirable for diluted magnetic semiconductors, spintronics, and sensing devices.

Electronic Structure of I-M8Ga16Sn30 (M = Ba, Sr, Yb) by First-Principles Calculation

NASA Astrophysics Data System (ADS)

Wang, Jin-song; Liu, Hong-xia; Deng, Shuping; Li, De-cong; Shen, Lan-xian; Cheng, Feng; Deng, Shu-kang

2017-05-01

Sn-based clathrates possess excellent thermoelectric properties ascribed to their higher Seebeck coefficient and lower thermal conductivity. Guest atoms significantly modulate the thermoelectric properties of Sn-based calculates because of their diverse atomic radius and interactions with framework atoms. Thus, we explored the electronic structure of I-M8Ga16Sn30 (M = Ba, Sr, Yb) by first-principles calculation. Results revealed significant differences between Yb8Ga16Sn30 and M8Ga16Sn30 (M = Ba, Sr,). In particular, the Yb-filled compound substitution possesses lowest formation energy and the off-center distance of the Yb atom is the largest compared with the other structures. I-M8Ga16Sn30 (M = Ba, Sr, Yb) is an indirect band gap semiconductor, and the enhanced hybridization effect between the guest and framework atoms' orbits exists because the Yb f orbit results in a decrease in band gap. Ba- and Sr-filled clathrates have similar valence bands but slightly different conduction bands; however, Yb8Ga16Sn30 possess the spiculate density of states near the Fermi level that reveals excellent thermoelectric properties.

Orbital atomic oxygen effects on materials: An overview of MSFC experiments on the STS-46 EOIM-3

NASA Astrophysics Data System (ADS)

Linton, Roger C.; Vaughn, Jason A.; Finckenor, Miria M.; Kamenetzky, Rachel R.; Dehaye, Robert F.; Whitaker, Ann F.

1995-02-01

The third Evaluation of Oxygen Interaction with Materials experiment was flown on Space Shuttle Mission STS-46 (July 31 - August 8, 1992), representing a joint effort of several NASA centers, universities, and contractors. This array of active instrumentation and material exposure sub-assemblies was integrated as a Shuttle cargo bay pallet experiment for investigating the effects of orbital atomic oxygen on candidate space materials. Marshall Space Flight Center contributed several passive exposure trays of material specimens, uniform stress and static stress material exposure fixtures, the Atomic Oxygen Resistance Monitor (AORM), and specimens of thermal coatings for the EOIM-3 variable exposure mechanisms. As a result of 42 hours of spacecraft velocity vector-oriented exposure during the later phases of the STS-46 mission in LEO, EOIM-3 materials were exposed to an atomic oxygen fluence of 2.2 x 10(exp 20) atoms/sq cm. In this paper, an overview is presented of the technical approaches and results from analyses of the MSFC flight specimens, fixtures, and the AORM. More detailed results from earlier EOIM missions, the LDEF, and from laboratory testing are included in associated papers of this conference session.

Dirac-, Rashba-, and Weyl-type spin-orbit couplings: Toward experimental realization in ultracold atoms

NASA Astrophysics Data System (ADS)

Wang, Bao-Zong; Lu, Yue-Hui; Sun, Wei; Chen, Shuai; Deng, Youjin; Liu, Xiong-Jun

2018-01-01

We propose a hierarchy set of minimal optical Raman lattice schemes to pave the way for experimental realization of high-dimensional spin-orbit (SO) couplings for ultracold atoms, including two-dimensional (2D) Dirac type, 2D Rashba type, and three-dimensional (3D) Weyl type. The proposed Dirac-type SO coupling exhibits precisely controllable high symmetry, for which a large topological phase region is predicted. The generation of 2D Rashba and 3D Weyl types requires that two sources of laser beams have distinct frequencies of factor 2 difference. Surprisingly, we find that 133Cs atoms provide an ideal candidate for the realization. A common and essential feature is of high controllability and absent of any fine-tuning in the realization, and the resulting SO coupled ultracold atoms have a long lifetime. In particular, a long-lived topological Bose gas of 2D Dirac SO coupling has been proved in the follow-up experiment. These schemes essentially improve over the current experimental accessibility and controllability, and open a realistic way to explore novel high-dimensional SO physics, particularly quantum many-body physics and quantum far-from-equilibrium dynamics with novel topology for ultracold atoms.

Quantum defect theory for the orbital Feshbach resonance

NASA Astrophysics Data System (ADS)

Cheng, Yanting; Zhang, Ren; Zhang, Peng

2017-01-01

In the ultracold gases of alkali-earth-metal-like atoms, a new type of Feshbach resonance, i.e., the orbital Feshbach resonance (OFR), has been proposed and experimentally observed in ultracold 173Yb atoms [R. Zhang et al., Phys. Rev. Lett. 115, 135301 (2015), 10.1103/PhysRevLett.115.135301]. When the OFR of the 173Yb atoms occurs, the energy gap between the open and closed channels is smaller by two orders of magnitude than the van der Waals energy. As a result, quantitative accurate results for the low-energy two-body problems can be obtained via multichannel quantum defect theory (MQDT), which is based on the exact solution of the Schrödinger equation with the van der Waals potential. In this paper we use MQDT to calculate the two-atom scattering length, effective range, and binding energy of two-body bound states for the systems with OFR. With these results we further study the clock-transition spectrum for the two-body bound states, which can be used to experimentally measure the binding energy. Our results are helpful for the quantitative theoretical and experimental research for the ultracold gases of alkali-earth-metal-like atoms with OFR.

A simple scheme for magnetic balance in four-component relativistic Kohn-Sham calculations of nuclear magnetic resonance shielding constants in a Gaussian basis.

PubMed

Olejniczak, Małgorzata; Bast, Radovan; Saue, Trond; Pecul, Magdalena

2012-01-07

We report the implementation of nuclear magnetic resonance (NMR) shielding tensors within the four-component relativistic Kohn-Sham density functional theory including non-collinear spin magnetization and employing London atomic orbitals to ensure gauge origin independent results, together with a new and efficient scheme for assuring correct balance between the large and small components of a molecular four-component spinor in the presence of an external magnetic field (simple magnetic balance). To test our formalism we have carried out calculations of NMR shielding tensors for the HX series (X = F, Cl, Br, I, At), the Xe atom, and the Xe dimer. The advantage of simple magnetic balance scheme combined with the use of London atomic orbitals is the fast convergence of results (when compared with restricted kinetic balance) and elimination of linear dependencies in the basis set (when compared to unrestricted kinetic balance). The effect of including spin magnetization in the description of NMR shielding tensor has been found important for hydrogen atoms in heavy HX molecules, causing an increase of isotropic values of 10%, but negligible for heavy atoms.

Orbital atomic oxygen effects on materials: An overview of MSFC experiments on the STS-46 EOIM-3

NASA Technical Reports Server (NTRS)

Linton, Roger C.; Vaughn, Jason A.; Finckenor, Miria M.; Kamenetzky, Rachel R.; Dehaye, Robert F.; Whitaker, Ann F.

1995-01-01

The third Evaluation of Oxygen Interaction with Materials experiment was flown on Space Shuttle Mission STS-46 (July 31 - August 8, 1992), representing a joint effort of several NASA centers, universities, and contractors. This array of active instrumentation and material exposure sub-assemblies was integrated as a Shuttle cargo bay pallet experiment for investigating the effects of orbital atomic oxygen on candidate space materials. Marshall Space Flight Center contributed several passive exposure trays of material specimens, uniform stress and static stress material exposure fixtures, the Atomic Oxygen Resistance Monitor (AORM), and specimens of thermal coatings for the EOIM-3 variable exposure mechanisms. As a result of 42 hours of spacecraft velocity vector-oriented exposure during the later phases of the STS-46 mission in LEO, EOIM-3 materials were exposed to an atomic oxygen fluence of 2.2 x 10(exp 20) atoms/sq cm. In this paper, an overview is presented of the technical approaches and results from analyses of the MSFC flight specimens, fixtures, and the AORM. More detailed results from earlier EOIM missions, the LDEF, and from laboratory testing are included in associated papers of this conference session.

Atomic Gaussian type orbitals and their Fourier transforms via the Rayleigh expansion

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

Yükçü, Niyazi

Gaussian type orbitals (GTOs), which are one of the types of exponential type orbitals (ETOs), are used usually as basis functions in the multi-center atomic and molecular integrals to better understand physical and chemical properties of matter. In the Fourier transform method (FTM), basis functions have not simplicity to make mathematical operations, but their Fourier transforms are easier to use. In this work, with the help of FTM, Rayleigh expansion and some properties of unnormalized GTOs, we present new mathematical results for the Fourier transform of GTOs in terms of Laguerre polynomials, hypergeometric and Whittaker functions. Physical and analytical propertiesmore » of GTOs are discussed and some numerical results have been given in a table. Finally, we compare our mathematical results with the other known literature results by using a computer program and details of evaluation are presented.« less

Mid- and long-term debris environment projections using the EVOLVE and CHAIN models

NASA Astrophysics Data System (ADS)

Eichler, Peter; Reynolds, Robert C.

1995-06-01

Results of debris environment projections are of great importance for the evaluation of the necessity and effectiveness of debris mitigation measures. EVOLVE and CHAIN are two models for debris environment projections that have been developed independently using different conceptual approaches. A comparison of results from these two models therefore provides a means of validating debris environment projections which they have made. EVOLVE is a model that requires mission model projections to describe future space operation; these projections include launch date, mission orbit altitude and inclimation, mission duration, vehicle size and mass, and classification as an object capable of experiencing breakup from on-board stored energy. EVOLVE describes the orbital debris environment by the orbital elements of the objects in the environment. CHAIN is an analytic model that bins the debris environemnt in size and altitude rather than following the orbit evolution of individual debris fragments. The altitude/size bins are coupled by the initial spreading of fragments by collisions and the following orbital decay behavior. A set of test cases covering a variety of space usage scenarios have been defined for the two models. In this paper, a comparison of the results will be presented and sources of disagreement identified and discussed. One major finding is that despite differences in the results of the two models, the basic tendencies of the environment projections are independent of modeled uncertainties, leading to the demand of debris mitigation measures--explosion suppression and de-orbit of rocket bodies and payloads after mission completion.

Doping the alkali atom: an effective strategy to improve the electronic and nonlinear optical properties of the inorganic Al12N12 nanocage.

PubMed

Niu, Min; Yu, Guangtao; Yang, Guanghui; Chen, Wei; Zhao, Xingang; Huang, Xuri

2014-01-06

Under ab initio computations, several new inorganic electride compounds with high stability, M@x-Al12N12 (M = Li, Na, and K; x = b66, b64, and r6), were achieved for the first time by doping the alkali metal atom M on the fullerene-like Al12N12 nanocage, where the alkali atom is located over the Al-N bond (b66/b64 site) or six-membered ring (r6 site). It is revealed that independent of the doping position and atomic number, doping the alkali atom can significantly narrow the wide gap between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) (EH-L = 6.12 eV) of the pure Al12N12 nanocage in the range of 0.49-0.71 eV, and these doped AlN nanocages can exhibit the intriguing n-type characteristic, where a high energy level containing the excess electron is introduced as the new HOMO orbital in the original gap of pure Al12N12. Further, the diffuse excess electron also brings these doped AlN nanostructures the considerable first hyperpolarizabilities (β0), which are 1.09 × 10(4) au for Li@b66-Al12N12, 1.10 × 10(4), 1.62 × 10(4), 7.58 × 10(4) au for M@b64-Al12N12 (M = Li, Na, and K), and 8.89 × 10(5), 1.36 × 10(5), 5.48 × 10(4) au for M@r6-Al12N12 (M = Li, Na, and K), respectively. Clearly, doping the heavier Na/K atom over the Al-N bond can get the larger β0 value, while the reverse trend can be observed for the series with the alkali atom over the six-membered ring, where doping the lighter Li atom can achieve the larger β0 value. These fascinating findings will be advantageous for promoting the potential applications of the inorganic AlN-based nanosystems in the new type of electronic nanodevices and high-performance nonlinear optical (NLO) materials.

Transfer of a weakly bound electron in collisions of Rydberg atoms with neutral particles. II. Ion-pair formation and resonant quenching of the Rb(nl) and Ne(nl) States by Ca, Sr, and Ba atoms

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

Narits, A. A.; Mironchuk, E. S.; Lebedev, V. S., E-mail: vlebedev@sci.lebedev.ru

2013-10-15

Electron-transfer processes are studied in thermal collisions of Rydberg atoms with alkaline-earth Ca(4s{sup 2}), Sr(5s{sup 2}), and Ba(6s{sup 2}) atoms capable of forming negative ions with a weakly bound outermost p-electron. We consider the ion-pair formation and resonant quenching of highly excited atomic states caused by transitions between Rydberg covalent and ionic terms of a quasi-molecule produced in collisions of particles. The contributions of these reaction channels to the total depopulation cross section of Rydberg states of Rb(nl) and Ne(nl) atoms as functions of the principal quantum number n are compared for selectively excited nl-levels with l Much-Less-Than n andmore » for states with large orbital quantum numbers l = n - 1, n - 2. It is shown that the contribution from resonant quenching dominates at small values of n, and the ion-pair formation process begins to dominate with increasing n. The values and positions of the maxima of cross sections for both processes strongly depend on the electron affinity of an alkaline-earth atom and on the orbital angular momentum l of a highly excited atom. It is shown that in the case of Rydberg atoms in states with large l {approx} n - 1, the rate constants of ion-pair formation and collisional quenching are considerably lower than those for nl-levels with l Much-Less-Than n.« less

There may be Fermi Energy levels in the hollow interiors of Nanotubes that would allow for a type of Quantum

NASA Astrophysics Data System (ADS)

Kriske, Richard

2011-04-01

There may be Fermi Energy levels that would allow for easy travel by Atoms, Molecules and Particles, in the hollow interior of Nanotubes. This may result in a Quantum Mechanical explaination of Capillary Action, and it may result in devices could take advantage of the idea that it takes no energy to rise in a Capillary tube, only in leaving it. This no-energy conjecture of Capillarity sounds very much like the idea that Electrons in obitals lose no Energy staying in orbit, only in changing orbits.It is this conjecture that may reveal that a Fermi Energy state is essentially in a weak orbital. This weak orbital could be exploited to store Anti-matter for instance. More profoundly it clearly shows how the Quantum Mechanical states meld smoothly into Classical Physics. It also reveals how extremely efficient Classical Machines could be constructed to take advantage of this spontaneous action. Say a tube could be designed to nudge electrons out of a weak obital in one place, sent down the tube (which is another weak orbital) and deposited in a weak orbital of another very distant Atom, apparently with little or perhaps no work being done, as long as the orbitals are the same energy. This may already exist in some Biological systems. Although more experimentation is needed, this would be the breakthrough that is needed to unify Classical and Quantum Mechanics.

Application of the multireference equation of motion coupled cluster method, including spin-orbit coupling, to the atomic spectra of Cr, Mn, Fe and Co

NASA Astrophysics Data System (ADS)

Liu, Zhebing; Huntington, Lee M. J.; Nooijen, Marcel

2015-10-01

The recently introduced multireference equation of motion (MR-EOM) approach is combined with a simple treatment of spin-orbit coupling, as implemented in the ORCA program. The resulting multireference equation of motion spin-orbit coupling (MR-EOM-SOC) approach is applied to the first-row transition metal atoms Cr, Mn, Fe and Co, for which experimental data are readily available. Using the MR-EOM-SOC approach, the splittings in each L-S multiplet can be accurately assessed (root mean square (RMS) errors of about 70 cm-1). The RMS errors for J-specific excitation energies range from 414 to 783 cm-1 and are comparable to previously reported J-averaged MR-EOM results using the ACESII program. The MR-EOM approach is highly efficient. A typical MR-EOM calculation of a full spin-orbit spectrum takes about 2 CPU hours on a single processor of a 12-core node, consisting of Intel XEON 2.93 GHz CPUs with 12.3 MB of shared cache memory.

The Deep Space Atomic Clock Mission

NASA Technical Reports Server (NTRS)

Ely, Todd A.; Koch, Timothy; Kuang, Da; Lee, Karen; Murphy, David; Prestage, John; Tjoelker, Robert; Seubert, Jill

2012-01-01

The Deep Space Atomic Clock (DSAC) mission will demonstrate the space flight performance of a small, low-mass, high-stability mercury-ion atomic clock with long term stability and accuracy on par with that of the Deep Space Network. The timing stability introduced by DSAC allows for a 1-Way radiometric tracking paradigm for deep space navigation, with benefits including increased tracking via utilization of the DSN's Multiple Spacecraft Per Aperture (MSPA) capability and full ground station-spacecraft view periods, more accurate radio occultation signals, decreased single-frequency measurement noise, and the possibility for fully autonomous on-board navigation. Specific examples of navigation and radio science benefits to deep space missions are highlighted through simulations of Mars orbiter and Europa flyby missions. Additionally, this paper provides an overview of the mercury-ion trap technology behind DSAC, details of and options for the upcoming 2015/2016 space demonstration, and expected on-orbit clock performance.

Depopulation of Single-Phthalocyanine Molecular Orbitals upon Pyrrolic-Hydrogen Abstraction on Graphene.

PubMed

Néel, Nicolas; Lattelais, Marie; Bocquet, Marie-Laure; Kröger, Jörg

2016-02-23

Single-molecule chemistry with a scanning tunneling microscope has preponderantly been performed on metal surfaces. The molecule-metal hybridization, however, is often detrimental to genuine molecular properties and obscures their changes upon chemical reactions. We used graphene on Ir(111) to reduce the coupling between Ir(111) and adsorbed phthalocyanine molecules. By local electron injection from the tip of a scanning tunneling microscope the two pyrrolic H atoms were removed from single phthalocyanines. The detachment of the H atom pair induced a strong modification of the molecular electronic structure, albeit with no change in the adsorption geometry. Spectra and maps of the differential conductance combined with density functional calculations unveiled the entire depopulation of the highest occupied molecular orbital upon H abstraction. Occupied π states of intact molecules are proposed to be emptied via intramolecular electron transfer to dangling σ states of H-free N atoms.

Electron capture in collisions of S4+ with atomic hydrogen

NASA Astrophysics Data System (ADS)

Stancil, P. C.; Turner, A. R.; Cooper, D. L.; Schultz, D. R.; Rakovic, M. J.; Fritsch, W.; Zygelman, B.

2001-06-01

Charge transfer processes due to collisions of ground state S4+(3s2 1S) ions with atomic hydrogen are investigated for energies between 1 meV u-1 and 10 MeV u-1 using the quantum mechanical molecular-orbital close-coupling (MOCC), atomic-orbital close-coupling, classical trajectory Monte Carlo (CTMC) and continuum distorted wave methods. The MOCC calculations utilize ab initio adiabatic potentials and nonadiabatic radial coupling matrix elements obtained with the spin-coupled valence-bond approach. A number of variants of the CTMC approach were explored, including different momentum and radial distributions for the initial state, as well as effective charge and quantum-defect models to determine the corresponding quantum state after capture into final partially stripped S3+ excited classical states. Hydrogen target isotope effects are explored and rate coefficients for temperatures between 100 and 106 K are also presented.

New forms of spin-orbit coupling in a strontium optical lattice clock

NASA Astrophysics Data System (ADS)

Perlin, Michael; Safavi-Naini, Arghavan; Ozeri, Roee; Rey, Ana Maria

2017-04-01

Ultracold atomic systems allow for the simulation of a variety of condensed matter phenomena, including spin-orbit coupling (SOC), a key ingredient behind recently discovered topological insulators and a path for the realization of topological superfluids. While many experimental efforts have used alkali atoms to engineer SOC via Raman transitions, undesirable heating mechanisms have limited the observation of many-body phenomena manifest at long timescales. Alkaline earth atoms (AEA) have been recently shown to be a potentially better platform for the implementation of SOC due to their reduced sensitivity to spontaneous emission. While previous work has used electronic clock states as a pseudo-spin degree of freedom, we consider the effects of clock side-band transitions. We discuss the richer SOC dynamics which emerges as a result of this extension, and present methods to probe these dynamics in current AEA optical lattice clocks. AFOSR, NSF-PFC and DARPA.

Angularly resolved X-ray photoelectron spectroscopy investigation of PTFE after prolonged space exposure

NASA Technical Reports Server (NTRS)

Dalins, I.; Karimi, M.

1992-01-01

Monochromatized angularly resolved X-ray photoelectron spectroscopy (ARXPS) was used to study PTFE (Teflon) that had been exposed to an earth orbital environment for approximately six years. The primary interest of the research is on a very reactive component of this environment (atomic oxygen) which, because of the typical orbital velocities of a spacecraft, impinge on exposed surfaces with 5 eV energy. This presentation deals with the method of analysis, the findings as they pertain to a rather complex carbon, oxygen, and fluorine XPS peak analysis, and the character of the valence bands. An improved bias referencing method, based on ARXPS, is also demonstrated for evaluating specimen charging effects. It was found that the polymer molecule tends to resist the atomic oxygen attack by reorienting itself, so that the most electronegative CF3 groups are facing the incoming hyperthermal oxygen atoms. The implications of these findings to ground-based laboratory studies are discussed.

Comparison of Hyperthermal Ground Laboratory Atomic Oxygen Erosion Yields With Those in Low Earth Orbit

NASA Technical Reports Server (NTRS)

Banks, Bruce A.; Dill, Grace C.; Loftus, Ryan J.; deGroh, Kim K.; Miller, Sharon K.

2013-01-01

The atomic oxygen erosion yields of 26 materials (all polymers except for pyrolytic graphite) were measured in two directed hyperthermal radio frequency (RF) plasma ashers operating at 30 or 35 kHz with air. The hyperthermal asher results were compared with thermal energy asher results and low Earth orbital (LEO) results from the Materials International Space Station Experiment 2 and 7 (MISSE 2 and 7) flight experiments. The hyperthermal testing was conducted to a significant portion of the atomic oxygen fluence similar polymers were exposed to during the MISSE 2 and 7 missions. Comparison of the hyperthermal asher prediction of LEO erosion yields with thermal energy asher erosion yields indicates that except for the fluorocarbon polymers of PTFE and FEP, the hyperthermal energy ashers are a much more reliable predictor of LEO erosion yield than thermal energy asher testing, by a factor of four.

Open-orbit theory of photoionization microscopy on nonhydrogenic atoms

NASA Astrophysics Data System (ADS)

Liu, F. L.; Zhao, L. B.

2017-04-01

Semiclassical open-orbit theory (OOT), previously developed to study photoionization of hydrogenic atoms in a uniform electric field [L. B. Zhao and J. B. Delos, Phys. Rev. A 81, 053417 (2010), 10.1103/PhysRevA.81.053417], has been generalized to describe the propagation of outgoing electron waves to macroscopic distances from a nonhydrogenic atomic source. The generalized OOT has been applied to calculate spatial distributions of electron probability densities and current densities, produced due to photoionization for lithium in a uniform electric field. The obtained results are compared with those from the fully quantum-mechanical coupled-channel theory (CCT). The excellent agreement between the CCT and OOT confirms the reliability of the generalized OOT. Comparison is also made with theoretical calculations from the wave-packet propagation technique and the recent photoionization microscopy experiment. The existing difference between theory and experiment is discussed.

Dirac State in the FeB2 Monolayer with Graphene-Like Boron Sheet.

PubMed

Zhang, Haijun; Li, Yafei; Hou, Jianhou; Du, Aijun; Chen, Zhongfang

2016-10-12

By introducing the commonly utilized Fe atoms into a two-dimensional (2D) honeycomb boron network, we theoretically designed a new Dirac material of FeB 2 monolayer with a Fermi velocity in the same order of graphene. The electron transfer from Fe atoms to B networks not only effectively stabilizes the FeB 2 networks but also leads to the strong interaction between the Fe and B atoms. The Dirac state in FeB 2 system primarily arises from the Fe d orbitals and hybridized orbital from Fe-d and B-p states. The newly predicted FeB 2 monolayer has excellent dynamic and thermal stabilities and is also the global minimum of 2D FeB 2 system, implying its experimental feasibility. Our results are beneficial to further uncovering the mechanism of the Dirac cones and providing a feasible strategy for Dirac materials design.

Spin-orbit coupled systems in the atomic limit: rhenates, osmates, iridates

NASA Astrophysics Data System (ADS)

Paramekanti, Arun; Singh, David J.; Yuan, Bo; Casa, Diego; Said, Ayman; Kim, Young-June; Christianson, A. D.

2018-06-01

Motivated by RIXS experiments on a wide range of complex heavy oxides, including rhenates, osmates, and iridates, we discuss the theory of RIXS for site-localized t2 g orbital systems with strong spin-orbit coupling. For such systems, we present exact diagonalization results for the spectrum at different electron fillings, showing that it accesses "single-particle" and "multiparticle" excitations. This leads to a simple picture for the energies and intensities of the RIXS spectra in Mott insulators such as double perovskites which feature highly localized electrons, and yields estimates of the spin-orbit coupling and Hund's coupling in correlated 5 d oxides. We present new higher resolution RIXS data at the Re L3 edge in Ba2YReO6 which finds a previously unresolved peak splitting, providing further confirmation of our theoretical predictions. Using ab initio electronic structure calculations on Ba2M ReO6 (with M =Re , Os, Ir) we show that while the atomic limit yields a reasonable effective Hamiltonian description of the experimental observations, effects such as t2 g-eg interactions and hybridization with oxygen are important. Our ab initio estimate for the strength of the intersite exchange coupling shows that, compared to the d3 systems, the exchange is one or two orders of magnitude weaker in the d2 and d4 materials, which may partly explain the suppression of long-range magnetic order in the latter compounds. As a way to interpolate between the site-localized picture and our electronic structure band calculations, we discuss the spin-orbital levels of the M O6 cluster. This suggests a possible role for intracluster excitons in Ba2YIrO6 which may lead to a weak breakdown of the atomic Jeff=0 picture and to small magnetic moments.

Dynamic localization in optical and Zeeman lattices in the presence of spin-orbit coupling

NASA Astrophysics Data System (ADS)

Kartashov, Yaroslav V.; Konotop, Vladimir V.; Zezyulin, Dmitry A.; Torner, Lluis

2016-12-01

The dynamic localization of a two-level atom in a periodic potential under the action of spin-orbit coupling and a weak harmonically varying linear force is studied. We consider optical and Zeeman potentials that are either in phase or out of phase in two spinor components, respectively. The expectation value for the position of the atom after one oscillation period of the linear force is recovered in authentic resonances or in pseudoresonances. The frequencies of the linear force corresponding to authentic resonances are determined by the band structure of the periodic potential and are affected by the spin-orbit coupling. The width or dispersion of the wave packet in authentic resonances is usually minimal. The frequencies corresponding to pseudoresonances do not depend on the type of potential and on the strength of the spin-orbit coupling, while the evolution of excitations at the corresponding frequencies is usually accompanied by significant dispersion. Pseudoresonances are determined by the initial phase of the linear force and by the quasimomentum of the wave packet. Due to the spinor nature of the system, the motion of the atom is accompanied by periodic, but not harmonic, spin oscillations. Under the action of spin-orbit coupling the oscillations of the wave packet can be nearly completely suppressed in optical lattices. Dynamic localization in Zeeman lattices is characterized by doubling of the resonant oscillation periods due to band crossing at the boundary of the Brillouin zone. We also show that higher harmonics in the Fourier expansion of the energy band lead to effective dispersion, which can be strong enough to prevent dynamic localization of the Bloch wave packet.

Band structure and orbital character of monolayer MoS2 with eleven-band tight-binding model

NASA Astrophysics Data System (ADS)

Shahriari, Majid; Ghalambor Dezfuli, Abdolmohammad; Sabaeian, Mohammad

2018-02-01

In this paper, based on a tight-binding (TB) model, first we present the calculations of eigenvalues as band structure and then present the eigenvectors as probability amplitude for finding electron in atomic orbitals for monolayer MoS2 in the first Brillouin zone. In these calculations we are considering hopping processes between the nearest-neighbor Mo-S, the next nearest-neighbor in-plan Mo-Mo, and the next nearest-neighbor in-plan and out-of-plan S-S atoms in a three-atom based unit cell of two-dimensional rhombic MoS2. The hopping integrals have been solved in terms of Slater-Koster and crystal field parameters. These parameters are calculated by comparing TB model with the density function theory (DFT) in the high-symmetry k-points (i.e. the K- and Γ-points). In our TB model all the 4d Mo orbitals and the 3p S orbitals are considered and detailed analysis of the orbital character of each energy level at the main high-symmetry points of the Brillouin zone is described. In comparison with DFT calculations, our results of TB model show a very good agreement for bands near the Fermi level. However for other bands which are far from the Fermi level, some discrepancies between our TB model and DFT calculations are observed. Upon the accuracy of Slater-Koster and crystal field parameters, on the contrary of DFT, our model provide enough accuracy to calculate all allowed transitions between energy bands that are very crucial for investigating the linear and nonlinear optical properties of monolayer MoS2.

Coupled potential energy surface for the F(2P)+CH4→HF+CH3 entrance channel and quantum dynamics of the CH4·F- photodetachment.

PubMed

Westermann, Till; Eisfeld, Wolfgang; Manthe, Uwe

2013-07-07

An approach to construct vibronically and spin-orbit coupled diabatic potential energy surfaces (PESs) which describe all three relevant electronic states in the entrance channels of the X(P) + CH4 →HX + CH3 reactions (with X=F((2)P), Cl((2)P), or O((3)P)) is introduced. The diabatization relies on the permutational symmetry present in the methane molecule and results in diabatic states which transform as the three p orbitals of the X atom. Spin-orbit coupling is easily and accurately included using the atomic spin-orbit coupling matrix of the isolated X atom. The method is applied to the F + CH4 system obtaining an accurate PES for the entrance channel based on ab initio multi-reference configuration interaction (MRCI) calculations. Comparing the resulting PESs with spin-orbit MRCI calculations, excellent agreement is found for the excited electronic states at all relevant geometries. The photodetachment spectrum of CH4·F(-) is investigated via full-dimensional (12D) quantum dynamics calculations on the coupled PESs using the multi-layer multi-configurational time-dependent Hartree approach. Extending previous work [J. Palma and U. Manthe, J. Chem. Phys. 137, 044306 (2012)], which was restricted to the dynamics on a single adiabatic PES, the contributions of the electronically excited states to the photodetachment spectrum are calculated and compared to experiment. Considering different experimental setups, good agreement between experiment and theory is found. Addressing questions raised in the previous work, the present dynamical calculations show that the main contribution to the second peak in the photodetachment spectrum results from electron detachment into the electronically excited states of the CH4F complex.

Vibrational spectroscopic and DFT calculation studies of 2-amino-7-bromo-5-oxo-[1]benzopyrano [2,3-b]pyridine-3 carbonitrile

NASA Astrophysics Data System (ADS)

Premkumar, S.; Jawahar, A.; Mathavan, T.; Kumara Dhas, M.; Milton Franklin Benial, A.

2015-03-01

The vibrational spectra of 2-amino-7-bromo-5-oxo-[1]benzopyrano [2,3-b]pyridine-3 carbonitrile were recorded using fourier transform-infrared and fourier transform-Raman spectrometer. The optimized structural parameters, vibrational frequencies, Mulliken atomic charge distribution, frontier molecular orbitals, thermodynamic properties, temperature dependence of thermodynamic parameters, first order hyperpolarizability and natural bond orbital calculations of the molecule were performed using the Gaussian 09 program. The vibrational frequencies were assigned on the basis of potential energy distribution calculation using the VEDA 4.0 program. The calculated first order hyperpolarizability of ABOBPC molecule was obtained as 6.908 × 10-30 issue, which was 10.5 times greater than urea. The nonlinear optical activity of the molecule was also confirmed by the frontier molecular orbitals and natural bond orbital analysis. The frontier molecular orbitals analysis shows that the lower energy gap of the molecule, which leads to the higher value of first order hyperpolarizability. The natural bond orbital analysis indicates that the nonlinear optical activity of the molecule arises due to the π → π∗ transitions. The Mulliken atomic charge distribution confirms the presence of intramolecular charge transfer within the molecule. The reactive site of the molecule was predicted from the molecular electrostatic potential contour map. The values of thermo dynamic parameters were increasing with increasing temperature.

Evaluating frontier orbital energy and HOMO/LUMO gap with descriptors from density functional reactivity theory.

PubMed

Huang, Ying; Rong, Chunying; Zhang, Ruiqin; Liu, Shubin

2017-01-01

Wave function theory (WFT) and density functional theory (DFT)-the two most popular solutions to electronic structure problems of atoms and molecules-share the same origin, dealing with the same subject yet using distinct methodologies. For example, molecular orbitals are artifacts in WFT, whereas in DFT, electron density plays the dominant role. One question that needs to be addressed when using these approaches to appreciate properties related to molecular structure and reactivity is if there is any link between the two. In this work, we present a piece of strong evidence addressing that very question. Using five polymeric systems as illustrative examples, we reveal that using quantities from DFT such as Shannon entropy, Fisher information, Ghosh-Berkowitz-Parr entropy, Onicescu information energy, Rényi entropy, etc., one is able to accurately evaluate orbital-related properties in WFT like frontier orbital energies and the HOMO (highest occupied molecular orbital)/LUMO (lowest unoccupied molecular orbital) gap. We verified these results at both the whole molecule level and the atoms-in-molecules level. These results provide compelling evidence suggesting that WFT and DFT are complementary to each other, both trying to comprehend the same properties of the electronic structure and molecular reactivity from different perspectives using their own characteristic vocabulary. Hence, there should be a bridge or bridges between the two approaches.

The Investigation Of Carbon Contamination And Sputtering Effects Of Xenon Ion Thrusters

NASA Technical Reports Server (NTRS)

Prak, Moline K.

2004-01-01

The Electro-Physics Branch of the NASA Glenn Research Center investigates the effect of atomic oxygen, environmental durability of high performance power materials and surfaces, and low earth orbit. One of its current projects involves the analysis of ion thrusters. Ion thrusters are devices that initiate a beam of ions to a target area. The type of ion thruster that I have been working with this Summer of 2004 emits positively charged Xenon (Xe(+)) atoms through two grids, the screen grid and the accelerator grid, after it enters an ionization chamber. Insulators are used to mechanically hold and separate these two grids. A propellant isolator, an instrument that closely resembles insulators, is placed in front of the ionization chamber. Both the insulator and isolator are made with a ceramic compound and filled with insulating beads. The main difference between the two devices is that the propellant isolator allows gas to flow through, in this case, the gas is Xe(+) and the insulators do not. In order to avoid carbon deposits and other contaminating chemicals to settle on the insulators and propellant isolator, a metal shadow shield is placed around them. These shadow shields function as a protectant and can be shaped in numerous configurations. Part of my job responsibility this summer is to investigate the effectiveness of different shadow shields that are utilized on three different ion engines: the NSTAR (NASA Solar Electric Propulsion Technology Application Readiness), JIMO (Jupiter Icy Moons Orbiter), and NEXIS (Nuclear Electric Xenon Ion System). Using calculus and other mathematical tactics, I was asked to find the total flux of carbon contamination that was able to pass the protectant shadow shield. I familiarized myself with the software program, MathCad2004, to help perform some mathematical computations such as complex integration. Another method of studying the probability of contamination is by experimental simulation. After attaining the precise parameters of the actual shadow shields, I created replicas of three types of shadow shielding to be used to undergo testing. It will be placed in a machine that produces carbon atoms at a high temperature of 200 C. or beam is aimed at a targeted material. As a result of this collision, atoms and other particles are ejected out of the target surface. Another part of my internship consisted of research on sputter ejection, or the angle distribution of sputtered material. This research entailed finding the past results of sputter ejection investigation as well as creating another type of mock simulation. Other minor projects include calculating the path of Xe(+) gas through the insulating beads of the isolators and assisting my mentor in collecting data for his paper for the Joint Propulsion Conference & Exhibit to be held July 11-14,2004 in Fort Lauderdale, Florida.

Role of orbital overlap in atomic manipulation

NASA Astrophysics Data System (ADS)

Jarvis, Sam; Sweetman, Adam; Bamidele, Joseph; Kantorovich, Lev; Moriarty, Philip

2012-06-01

We conduct ab initio simulations illustrating that the ability to achieve atomic manipulation using a dynamic force microscope depends on the precise orientation of the dangling bond(s) at the tip apex and their charge density with respect to those of surface atoms. Using the Si(100)-c(4×2) surface as a prototype, we demonstrate that it is possible to select tip apices capable of performing atomic manipulation tasks which are unachievable using another choice of apex. Specific tip apices can be identified via examination of F(z) curves taken at different lateral positions.

Atomic oxygen exposure of LDEF experiment trays

NASA Technical Reports Server (NTRS)

Bourassa, R. J.; Gillis, J. R.

1992-01-01

Atomic oxygen exposures were determined analytically for rows, longerons, and end bays of the Long Duration Exposure Facility (LDEF). The calculations are based on an analytical model that accounts for the effects of thermal molecular velocity, atmospheric temperature, number density, spacecraft velocity, incidence angle, and atmospheric rotation on atomic oxygen flux. Results incorporate variations in solar activity, geomagnetic index, and orbital parameters occurring over the 6-year flight of the spacecraft. To facilitate use of the data, both detailed tabulations and summary charts for atomic oxygen fluences are presented.

Covalent functionalization of MoS2 nanosheets synthesized by liquid phase exfoliation to construct electrochemical sensors for Cd (II) detection.

PubMed

Gan, Xiaorong; Zhao, Huimin; Wong, Kwok-Yin; Lei, Dang Yuan; Zhang, Yaobin; Quan, Xie

2018-05-15

Surface functionalization is an effective strategy in the precise control of electronic surface states of two-dimensional materials for promoting their applications. In this study, based on the strong coordination interaction between the transition-metal centers and N atoms, the surface functionalization of few-layer MoS 2 nanosheets was successfully prepared by liquid phase exfoliation method in N, N-dimethylformamide (DMF), 1-methyl-2-pyrrolidinone, and formamide. The cytotoxicity of surface-functionalized MoS 2 nanosheets was for the first time evaluated by the methylthiazolyldiphenyl-tetrazoliumbromide assays. An electrochemical sensor was constructed based on glass carbon electrode (GCE) modified by MoS 2 nanosheets obtained in DMF, which exhibits relatively higher sensitivity to Cd 2+ detection and lower cytotoxicity against MCF-7 cells. The mechanisms of surface functionalization and selectively detecting Cd 2+ were investigated by density functional theory calculations together with various spectroscopic measurements. It was found that surface-functionalized MoS 2 nanosheets could be generated through Mo-N covalent bonds due to the orbital hybridization between the 5 s orbitals of Mo atoms and the 2p orbitals of N atoms of the solvent molecules. The high selectivity of the sensor is attributed to the coordination reaction between Cd 2+ and O donor atoms of DMF adsorbed on MoS 2 nanosheets. The robust anti-interference is ascribed to the strong binding energy of Cd 2+ and O atoms of DMF. Under the optimum conditions, the electrochemical sensor exhibits highly sensitive and selective assaying of Cd 2+ with a measured detection limit of 0.2 nM and a linear range from 2 nM to 20 μM. Copyright © 2018 Elsevier B.V. All rights reserved.

Effects of single atom doping on the ultrafast electron dynamics of M1Au24(SR)18 (M = Pd, Pt) nanoclusters.

PubMed

Zhou, Meng; Qian, Huifeng; Sfeir, Matthew Y; Nobusada, Katsuyuki; Jin, Rongchao

2016-04-07

Atomically precise, doped metal clusters are receiving wide research interest due to their synergistic properties dependent on the metal composition. To understand the electronic properties of doped clusters, it is highly desirable to probe the excited state behavior. Here, we report the ultrafast relaxation dynamics of doped M1@Au24(SR)18 (M = Pd, Pt; R = CH2CH2Ph) clusters using femtosecond visible and near infrared transient absorption spectroscopy. Three relaxation components are identified for both mono-doped clusters: (1) sub-picosecond relaxation within the M1Au12 core states; (2) core to shell relaxation in a few picoseconds; and (3) relaxation back to the ground state in more than one nanosecond. Despite similar relaxation pathways for the two doped nanoclusters, the coupling between the metal core and surface ligands is accelerated by over 30% in the case of the Pt dopant compared with the Pd dopant. Compared to Pd doping, the case of Pt doping leads to much more drastic changes in the steady state and transient absorption of the clusters, which indicates that the 5d orbitals of the Pt atom are more strongly mixed with Au 5d and 6s orbitals than the 4d orbitals of the Pd dopant. These results demonstrate that a single foreign atom can lead to entirely different excited state spectral features of the whole cluster compared to the parent Au25(SR)18 cluster. The detailed excited state dynamics of atomically precise Pd/Pt doped gold clusters help further understand their properties and benefit the development of energy-related applications.

Effects of single atom doping on the ultrafast electron dynamics of M 1Au 24(SR) 18 (M = Pd, Pt) nanoclusters

DOE PAGES

Zhou, Meng; Qian, Huifeng; Sfeir, Matthew Y.; ...

2016-02-29

Atomically precise, doped metal clusters are receiving wide research interest due to their synergistic properties dependent on the metal composition. To understand the electronic properties of doped clusters, it is highly desirable to probe the excited state behavior. Here, we report the ultrafast relaxation dynamics of doped M 1@Au 24(SR) 18 (M = Pd, Pt; R = CH 2CH 2Ph) clusters using femtosecond visible and near infrared transient absorption spectroscopy. Three relaxation components are identified for both mono-doped clusters: (1) sub-picosecond relaxation within the M 1Au 12 core states; (2) core to shell relaxation in a few picoseconds; and (3)more » relaxation back to the ground state in more than one nanosecond. Despite similar relaxation pathways for the two doped nanoclusters, the coupling between the metal core and surface ligands is accelerated by over 30% in the case of the Pt dopant compared with the Pd dopant. Compared to Pd doping, the case of Pt doping leads to much more drastic changes in the steady state and transient absorption of the clusters, which indicates that the 5d orbitals of the Pt atom are more strongly mixed with Au 5d and 6s orbitals than the 4d orbitals of the Pd dopant. These results demonstrate that a single foreign atom can lead to entirely different excited state spectral features of the whole cluster compared to the parent Au 25(SR) 18 cluster. As a result, the detailed excited state dynamics of atomically precise Pd/Pt doped gold clusters help further understand their properties and benefit the development of energy-related applications.« less

A "Bit" of Quantum Mechanics

ERIC Educational Resources Information Center

Oss, Stefano; Rosi, Tommaso

2015-01-01

We have developed an app for iOS-based smart-phones/tablets that allows a 3-D, complex phase-based colorful visualization of hydrogen atom wave functions. Several important features of the quantum behavior of atomic orbitals can easily be made evident, thus making this app a useful companion in introductory modern physics classes. There are many…

Exploiting Universality in Atoms with Large Scattering Lengths

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

Braaten, Eric

2012-05-31

The focus of this research project was atoms with scattering lengths that are large compared to the range of their interactions and which therefore exhibit universal behavior at sufficiently low energies. Recent dramatic advances in cooling atoms and in manipulating their scattering lengths have made this phenomenon of practical importance for controlling ultracold atoms and molecules. This research project was aimed at developing a systematically improvable method for calculating few-body observables for atoms with large scattering lengths starting from the universal results as a first approximation. Significant progress towards this goal was made during the five years of the project.

Localizing gravitational wave sources with single-baseline atom interferometers

NASA Astrophysics Data System (ADS)

Graham, Peter W.; Jung, Sunghoon

2018-02-01

Localizing sources on the sky is crucial for realizing the full potential of gravitational waves for astronomy, astrophysics, and cosmology. We show that the midfrequency band, roughly 0.03 to 10 Hz, has significant potential for angular localization. The angular location is measured through the changing Doppler shift as the detector orbits the Sun. This band maximizes the effect since these are the highest frequencies in which sources live for several months. Atom interferometer detectors can observe in the midfrequency band, and even with just a single baseline they can exploit this effect for sensitive angular localization. The single-baseline orbits around the Earth and the Sun, causing it to reorient and change position significantly during the lifetime of the source, and making it similar to having multiple baselines/detectors. For example, atomic detectors could predict the location of upcoming black hole or neutron star merger events with sufficient accuracy to allow optical and other electromagnetic telescopes to observe these events simultaneously. Thus, midband atomic detectors are complementary to other gravitational wave detectors and will help complete the observation of a broad range of the gravitational spectrum.

Combinatorial Search for High-Activity Hydrogen Catalysts Based on Transition-Metal-Embedded Graphitic Carbons

DOE PAGES

Choi, Woon Ih; Wood, Brandon C.; Schwegler, Eric; ...

2015-09-22

Transition metal (TM) atoms in porphyrin–like complexes play important roles in many protein and enzymetic systems, where crystal–field effects are used to modify d–orbital levels. Inspired by the tunable electronic structure of these motifs, a high–throughput computational search for synthetic hydrogen catalysts is performed based on a similar motif of TM atoms embedded into the lattice of graphene. Based on an initial list of 300 possible embedding geometries, binders, and host atoms, descriptors for stability and catalytic activity are applied to extract ten promising candidates for hydrogen evolution, two of which are expected to exhibit high activity for hydrogen oxidation.more » In several instances, the active TM atoms are earth–abundant elements that show no activity in the bulk phase, highlighting the importance of the coordination environment in tuning the d–orbitals. In conclusion, it is found that the most active candidates involve a hitherto unreported surface reaction pathway that involves a Kubas–complex intermediate, which significantly lowers the kinetic barrier associated with hydrogen dissociation and association.« less

Clarification of the interaction between Au atoms and the anatase TiO2 (112) surface using density functional theory

NASA Astrophysics Data System (ADS)

Tada, Kohei; Koga, Hiroaki; Okumura, Mitsutaka; Tanaka, Shingo

2018-04-01

A model (112) surface slab of anatase TiO2 (112) was optimized, and the adsorption of Au atoms onto the (112) surface was investigated by first-principles calculations based on DFT (density functional theory) with the generalized gradient approximation (GGA). Furthermore, the results were compared with those of Au/anatase TiO2 (101) system. The (112) surface has a ridge and a groove (zig-zag structure). The Au atoms were strongly adsorbed in the grooves but became unstable as they climbed toward the ridges, and the promotion of electrons in the 5d orbitals to the 6s and 6p orbitals in the absorbed Au atom occurred. At the Au/anatase TiO2 interface, the Au-Ti4+ coordinate bond in the (112) system is stronger than that in the (101) system because the promotion of electrons is greater in the former interaction than the latter. The results suggest that Au/anatase TiO2 catalysts with a higher dispersion of Au nanoparticles could be prepared when the (112) surface is preferentially exposed.

KSC-2012-1857

NASA Image and Video Library

2012-02-17

Project Mercury: With Project Mercury, the United States gained its first experience in conducting human space missions that provided scientific and engineering knowledge of astronauts in space. Alan Shepard made history May 5, 1961, as America's first man in space. Less than a year later, John Glenn made the nation’s first orbital flight on Feb. 20, 1962. After two suborbital and three orbital missions, Project Mercury ended with a 22-orbit spaceflight on May 16, 1963. Poster designed by Kennedy Space Center Graphics Department/Greg Lee. Credit: NASA

KSC-2012-1858

NASA Image and Video Library

2012-02-17

Project Mercury: With Project Mercury, the United States gained its first experience in conducting human space missions that provided scientific and engineering knowledge of astronauts in space. Alan Shepard made history May 5, 1961, as America's first man in space. Less than a year later, John Glenn made the nation’s first orbital flight on Feb. 20, 1962. After two suborbital and three orbital missions, Project Mercury ended with a 22-orbit spaceflight on May 16, 1963. Poster designed by Kennedy Space Center Graphics Department/Greg Lee. Credit: NASA

DFT Studies on Interaction between Lanthanum and Hydroxyamide

NASA Astrophysics Data System (ADS)

Pati, Anindita; Kundu, T. K.; Pal, Snehanshu

2018-03-01

Extraction and separation of individual rare earth elements has been a challenge as they are chemically very similar. Solvent extraction is the most suitable way for extraction of rare earth elements. Acidic, basic, neutral, chelating are the major classes of extractants for solvent extraction of rare earth elements. The coordination complex of chelating extractants is very selective with positively charged metal ion. Hence they are widely used. Hydroxyamide is capable of forming chelates with metal cations. In this present study interactions of hydroxyamide ligand with lanthanum have been investigated using density functional theory (DFT). Two different functional such as raB97XD and B3LYP are applied along with 6-31+G(d,p) basis set for carbon, nitrogen, hydrogen and SDD basis set for lanthanum. Stability of formed complexes has been evaluated based on calculated interaction energies and solvation energies. Frontier orbital (highest occupied molecular orbital or HOMO and lowest unoccupied molecular orbital or LUMO) energies of the molecule have also been calculated. Electronegativity, chemical hardness, chemical softness and chemical potential are also determined for these complexes to get an idea about the reactivity. From the partial charge distribution it is seen that oxygen atoms in hydroxyamide have higher negative charge. The double bonded oxygen atom present in the hydroxyamide structure has higher electron density and so it forms bond with lanthanum but the singly bonded oxygen atom in the hydroxyamide structure is weaker donor atom and so it is less available for interaction with lanthanum.

Effect of local atomic and electronic structures on thermoelectric properties of chemically substituted CoSi

NASA Astrophysics Data System (ADS)

Hsu, C. C.; Pao, C. W.; Chen, J. L.; Chen, C. L.; Dong, C. L.; Liu, Y. S.; Lee, J. F.; Chan, T. S.; Chang, C. L.; Kuo, Y. K.; Lue, C. S.

2014-05-01

We report the effects of Ge partial substitution for Si on local atomic and electronic structures of thermoelectric materials in binary compound cobalt monosilicides (\\text{CoSi}_{1-x}\\text{Ge}_{x}\\text{:}\\ 0 \\le x \\le 0.15 ). Correlations between local atomic/electronic structure and thermoelectric properties are investigated by means of X-ray absorption spectroscopy. The spectroscopic results indicate that as Ge is partially substituted onto Si sites at x \\le 0.05 , Co in CoSi1-xGex gains a certain amount of charge in its 3d orbitals. Contrarily, upon further replacing Si with Ge at x \\ge 0.05 , the Co 3d orbitals start to lose some of their charge. Notably, thermopower is strongly correlated with charge redistribution in the Co 3d orbital, and the observed charge transfer between Ge and Co is responsible for the variation of Co 3d occupancy number. In addition to Seebeck coefficient, which can be modified by tailoring the Co 3d states, local lattice disorder may also be beneficial in enhancing the thermoelectric properties. Extended X-ray absorption fine structure spectrum results further demonstrate that the lattice phonons can be enhanced by Ge doping, which results in the formation of the disordered Co-Co pair. Improvements in the thermoelectric properties are interpreted based on the variation of local atomic and electronic structure induced by lattice distortion through chemical substitution.

Modeling Photodetachment from HO2- Using the pd Case of the Generalized Mixed Character Molecular Orbital Model

NASA Astrophysics Data System (ADS)

Blackstone, Christopher C.; Sanov, Andrei

2016-06-01

Using the generalized model for photodetachment of electrons from mixed-character molecular orbitals, we gain insight into the nature of the HOMO of HO2- by treating it as a coherent superpostion of one p- and one d-type atomic orbital. Fitting the pd model function to the ab initio calculated HOMO of HO2- yields a fractional d-character, γp, of 0.979. The modeled curve of the anisotropy parameter, β, as a function of electron kinetic energy for a pd-type mixed character orbital is matched to the experimental data.

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.

The influence of molecular symmetry and topological factors on the internal heavy atom effect in aromatic and heteroaromatic compounds

NASA Astrophysics Data System (ADS)

Nijegorodov, N.; Mabbs, R.

2001-06-01

The absorption and fluorescence properties of 26 specially selected aromatic and heteroaromatic compounds, from different classes, are studied quantum chemically and experimentally at room temperature (293 K). Seven of these compounds have not been studied before. The compounds are arranged in seven groups, which illustrate different cases of the internal heavy atom effect. The quantum yield of fluorescence, γ and fluorescence decay time, τf of deaerated and non-deaerated cyclohexane or ethanol solutions are measured. The oscillator strength, fe, fluorescence rate constant, kf, natural lifetime, τ0t, and intersystem crossing rate constant, kST, were calculated for each compound. The orbital nature of the lowest excited singlet state and direction of polarization of the S0→ S1 transitions are determined using the PPP-CI method for each molecule. The investigation shows that substitution of a heavy atom(s) (Cl, S, Br, I etc.) into an aromatic or heteroaromatic molecule may produce different changes in all the fluorescence parameters (sometimes dramatically) and not necessarily lead to the quenching of fluorescence. Substitution of a heavy atom(s) may increase the value of the spin-orbit operator, \\Hcirc SO, if the S0→ S1 excitation is localized to some extent on a carbon atom bonded to a heavy atom(s) or on the heavy atom itself (Ö or S). Such substitution may change the symmetry of a molecule and hence the values of the ΨS 1\\HcircsoΨT i' matrix elements would change (in molecules of higher symmetry groups not all Ti states are able to mix with the perturbing S1 state). Such substitution may change the arrangement of Ti states below the S1, state and hence, the Franck-Condon factors would change. Such substitution may also change the value of the ΨS 0M jΨS 1 matrix element and, consequently, the oscillator strength of the S0→ S1 transition would change. A combination of all these possible changes determines the value of kf and kST and, consequently, determines the value of γ and τf. It is observed that in many cases, the value of the spin-orbit operator is related to the dipole moment operator, e.g. if the introduction of a heavy atom increases kST then, as a rule, it decreases fe( 1A→ 1La).

Information origins of the chemical bond: Bond descriptors from molecular communication channels in orbital resolution

NASA Astrophysics Data System (ADS)

Nalewajski, Roman F.

The flow of information in the molecular communication networks in the (condensed) atomic orbital (AO) resolution is investigated and the plane-wave (momentum-space) interpretation of the average Fisher information in the molecular information system is given. It is argued using the quantum-mechanical superposition principle that, in the LCAO MO theory the squares of corresponding elements of the Charge and Bond-Order (CBO) matrix determine the conditional probabilities between AO, which generate the molecular communication system of the Orbital Communication Theory (OCT) of the chemical bond. The conditional-entropy ("noise," information-theoretic "covalency") and the mutual-information (information flow, information-theoretic "ionicity") descriptors of these molecular channels are related to Wiberg's covalency indices of chemical bonds. The illustrative application of OCT to the three-orbital model of the chemical bond X-Y, which is capable of describing the forward- and back-donations as well as the atom promotion accompanying the bond formation, is reported. It is demonstrated that the entropy/information characteristics of these separate bond-effects can be extracted by an appropriate reduction of the output of the molecular information channel, carried out by combining several exits into a single (condensed) one. The molecular channels in both the AO and hybrid orbital representations are examined for both the molecular and representative promolecular input probabilities.

Analytical energy gradient for the two-component normalized elimination of the small component method

NASA Astrophysics Data System (ADS)

Zou, Wenli; Filatov, Michael; Cremer, Dieter

2015-06-01

The analytical gradient for the two-component Normalized Elimination of the Small Component (2c-NESC) method is presented. The 2c-NESC is a Dirac-exact method that employs the exact two-component one-electron Hamiltonian and thus leads to exact Dirac spin-orbit (SO) splittings for one-electron atoms. For many-electron atoms and molecules, the effect of the two-electron SO interaction is modeled by a screened nucleus potential using effective nuclear charges as proposed by Boettger [Phys. Rev. B 62, 7809 (2000)]. The effect of spin-orbit coupling (SOC) on molecular geometries is analyzed utilizing the properties of the frontier orbitals and calculated SO couplings. It is shown that bond lengths can either be lengthened or shortened under the impact of SOC where in the first case the influence of low lying excited states with occupied antibonding orbitals plays a role and in the second case the jj-coupling between occupied antibonding and unoccupied bonding orbitals dominates. In general, the effect of SOC on bond lengths is relatively small (≤5% of the scalar relativistic changes in the bond length). However, large effects are found for van der Waals complexes Hg2 and Cn2, which are due to the admixture of more bonding character to the highest occupied spinors.

76 FR 17460 - South Texas Project Nuclear Operating Company; Establishment of Atomic Safety and Licensing Board

Federal Register 2010, 2011, 2012, 2013, 2014

2011-03-29

...] South Texas Project Nuclear Operating Company; Establishment of Atomic Safety and Licensing Board..., 2.318, and 2.321, notice is hereby given that an Atomic Safety and Licensing Board (Board) is being...: Ronald M. Spritzer, Chair, Atomic Safety and Licensing Board Panel, U.S. Nuclear Regulatory Commission...

New Active Optical Technique Developed for Measuring Low-Earth-Orbit Atomic Oxygen Erosion of Polymers

NASA Technical Reports Server (NTRS)

Banks, Bruce A.; deGroh, Kim K.; Demko, Rikako

2003-01-01

Polymers such as polyimide Kapton (DuPont) and Teflon FEP (DuPont, fluorinated ethylene propylene) are commonly used spacecraft materials because of desirable properties such as flexibility, low density, and in the case of FEP, a low solar absorptance and high thermal emittance. Polymers on the exterior of spacecraft in the low-Earth-orbit (LEO) environment are exposed to energetic atomic oxygen. Atomic oxygen reaction with polymers causes erosion, which is a threat to spacecraft performance and durability. It is, therefore, important to understand the atomic oxygen erosion yield E (the volume loss per incident oxygen atom) of polymers being considered in spacecraft design. The most common technique for determining E is a passive technique based on mass-loss measurements of samples exposed to LEO atomic oxygen during a space flight experiment. There are certain disadvantages to this technique. First, because it is passive, data are not obtained until after the flight is completed. Also, obtaining the preflight and postflight mass measurements is complicated by the fact that many polymers absorb water and, therefore, the mass change due to water absorption can affect the E data. This is particularly true for experiments that receive low atomic oxygen exposures or for samples that have a very low E. An active atomic oxygen erosion technique based on optical measurements has been developed that has certain advantages over the mass-loss technique. This in situ technique can simultaneously provide the erosion yield data on orbit and the atomic oxygen exposure fluence, which is needed for erosion yield determination. In the optical technique, either sunlight or artificial light can be used to measure the erosion of semitransparent or opaque polymers as a result of atomic oxygen attack. The technique is simple and adaptable to a rather wide range of polymers, providing that they have a sufficiently high optical absorption coefficient. If one covers a photodiode with a uniformly thick sheet of semitransparent polymer such as Kapton H polyimide, then as atomic oxygen erodes the polymer, the short-circuit current from the photodiode will increase in an exponential manner with fluence. This nonlinear response with fluence results in a lack of sensitivity for measuring low atomic oxygen fluences. However, if one uses a variable-thickness polymer or carbon sample, which is configured as shown in the preceding figure, then a linear response can be achieved for opaque materials using a parabolic well for a circular geometry detector or a V-shaped well for a rectangular-geometry detector. Variable-thickness samples can be fabricated using many thin polymer layers. For semitransparent polymers such as Kapton H polyimide, there is an initial short-circuit current that is greater than zero. This current has a slightly nonlinear dependence on atomic oxygen fluence in comparison to opaque materials such as black Kapton as shown in the graph. For this graph figure, the total thickness of Kapton H was assumed to be 0.03 cm. The photodiode short-circuit current shown in the graph was generated on the basis of preliminary measurements-a total reflectance rho of 0.0424 and an optical absorption coefficient a of 146.5 cm(sup -1). In addition to obtaining on-orbit data, the advantage of this active erosion and erosion yield measurement technique is its simplicity and reliance upon well-characterized fluence witness materials as well as a nearly linear photodiode short-circuit current dependence upon atomic oxygen fluence. The optical technique is useful for measuring either atomic oxygen fluence or erosion, depending on the information desired. To measure the atomic oxygen erosion yield of a test material, one would need to have two photodiode sensors, one for the test material and one that uses a known erosion yield material (such as Kapton) to measure the atomic oxygen fluence.

The QTP family of consistent functionals and potentials in Kohn-Sham density functional theory

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

Jin, Yifan; Bartlett, Rodney J., E-mail: bartlett@qtp.ufl.edu

This manuscript presents the second, consistent density functional in the QTP (Quantum Theory Project) family, that is, the CAM-QTP(01). It is a new range-separated exchange-correlation functional in which the non-local exchange contribution is 100% at large separation. It follows the same basic principles of this family that the Kohn-Sham eigenvalues of the occupied orbitals approximately equal the vertical ionization energies, which is not fulfilled by most of the traditional density functional methods. This new CAM-QTP(01) functional significantly improves the accuracy of the vertical excitation energies especially for the Rydberg states in the test set. It also reproduces many other propertiesmore » such as geometries, reaction barrier heights, and atomization energies.« less

Orbital Electron Capture Rates in Extreme Astrophysical Environments

NASA Astrophysics Data System (ADS)

Martin, Matthew; McDonald, William; Leach, Kyle

2017-09-01

In an attempt to better understand EC decay rates in hot environments, we have developed a program to examine and parse all evaluated atomic and nuclear data. Taking into account the effects of ionization on accessible decay states and electron capture probabilities, half lives across the nuclear chart can be investigated without the need for theoretical estimates. Part of the ongoing project will include isolating stable isotopes that become unstable due to ionization and estimating their stability in these new environments. In addition, we hope to account for a thermal population of excited states to better simulate these environments. This should aide in the complete understanding of nuclear processes in these extreme astrophysical environments. This work is supported in part by the U.S. Department of Energy, Office of Science, Office of Nuclear Physics.

LRO-LAMP observations of the LCROSS impact plume.

PubMed

Gladstone, G Randall; Hurley, Dana M; Retherford, Kurt D; Feldman, Paul D; Pryor, Wayne R; Chaufray, Jean-Yves; Versteeg, Maarten; Greathouse, Thomas K; Steffl, Andrew J; Throop, Henry; Parker, Joel Wm; Kaufmann, David E; Egan, Anthony F; Davis, Michael W; Slater, David C; Mukherjee, Joey; Miles, Paul F; Hendrix, Amanda R; Colaprete, Anthony; Stern, S Alan

2010-10-22

On 9 October 2009, the Lunar Crater Observation and Sensing Satellite (LCROSS) sent a kinetic impactor to strike Cabeus crater, on a mission to search for water ice and other volatiles expected to be trapped in lunar polar soils. The Lyman Alpha Mapping Project (LAMP) ultraviolet spectrograph onboard the Lunar Reconnaissance Orbiter (LRO) observed the plume generated by the LCROSS impact as far-ultraviolet emissions from the fluorescence of sunlight by molecular hydrogen and carbon monoxide, plus resonantly scattered sunlight from atomic mercury, with contributions from calcium and magnesium. The observed light curve is well simulated by the expansion of a vapor cloud at a temperature of ~1000 kelvin, containing ~570 kilograms (kg) of carbon monoxide, ~140 kg of molecular hydrogen, ~160 kg of calcium, ~120 kg of mercury, and ~40 kg of magnesium.

Quantum orbital angular momentum of elliptically symmetric light

NASA Astrophysics Data System (ADS)

Plick, William N.; Krenn, Mario; Fickler, Robert; Ramelow, Sven; Zeilinger, Anton

2013-03-01

We present a quantum-mechanical analysis of the orbital angular momentum of a class of recently discovered elliptically symmetric stable light fields—the so-called Ince-Gauss modes. We study, in a fully quantum formalism, how the orbital angular momentum of these beams varies with their ellipticity, and we discover several compelling features, including nonmonotonic behavior, stable beams with real continuous (noninteger) orbital angular momenta, and orthogonal modes with the same orbital angular momenta. We explore, and explain in detail, the reasons for this behavior. These features may have applications in quantum key distribution, atom trapping, and quantum informatics in general—as the ellipticity opens up an alternative way of navigating the spatial photonic Hilbert space.

Platinum atomic wire encapsulated in gold nanotubes: A first principle study

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

Nigam, Sandeep, E-mail: snigam@barc.gov.in; Majumder, Chiranjib; Sahoo, Suman K.

2014-04-24

The nanotubes of gold incorporated with platinum atomic wire have been investigated by means of firstprinciples density functional theory with plane wave pseudopotential approximation. The structure with zig-zag chain of Pt atoms in side gold is found to be 0.73 eV lower in energy in comparison to straight chain of platinum atoms. The Fermi level of the composite tube was consisting of d-orbitals of Pt atoms. Further interaction of oxygen with these tubes reveals that while tube with zig-zag Pt prefers dissociative adsorption of oxygen molecule, the gold tube with linear Pt wire favors molecular adsorption.

Long-range dispersion interactions between Li and rare-gas atoms

NASA Astrophysics Data System (ADS)

Zhang, Deng-Hong; Xu, Ya-Bin; Jiang, Jun; Jiang, Li; Xie, Lu-You; Dong, Chen-Zhong

2017-06-01

The energy levels, oscillator strength and dipole scalar polarizabilities of Li atoms are calculated by using the relativistic semiempirical-core-potential method (RCICP). The dispersion coefficients C6 between ground 2s1/2 2p1/2,2p3/2 states of Li atom and the ground state of rare gas atoms (Ne, Ar, Kr, Xe) are calculated in JJ coupled states, in which the spin-orbital interactions are included. Present results are in good agreement with other available results. 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.

Conceptual Integration of Hybridization by Algerian Students Intending to Teach Physical Sciences

ERIC Educational Resources Information Center

Salah, Hazzi; Dumon, Alain

2011-01-01

This work aims to assess the difficulties encountered by students of the Ecole Normale Superieure of Kouba (Algeria) intending to teach physical science in the integration of the hybridization of atomic orbitals. It is a concept that they should use in describing the formation of molecular orbitals ([sigma] and [pi]) in organic chemistry and gaps…

Introductory Molecular Orbital Theory: An Honors General Chemistry Computational Lab as Implemented Using Three-Dimensional Modeling Software

ERIC Educational Resources Information Center

Ruddick, Kristie R.; Parrill, Abby L.; Petersen, Richard L.

2012-01-01

In this study, a computational molecular orbital theory experiment was implemented in a first-semester honors general chemistry course. Students used the GAMESS (General Atomic and Molecular Electronic Structure System) quantum mechanical software (as implemented in ChemBio3D) to optimize the geometry for various small molecules. Extended Huckel…

Ultracold Fermions in the P-Orbital Band of an Optical Lattice

DTIC Science & Technology

2015-07-27

introduces (1) a new degree of freedom due to orbital degeneracy and (2) a tunneling anisotropy which depends on the orientation of the orbital wavefunction...demonstrated this new technique with a diode -pumped solid-state laser operating at 1342 nm that could be frequency doubled to provide 671 nm light for laser...Figure 3: Self-injection locked, diode -pumped solid-state laser for laser cooling of Li atoms. The solid-state Nd:YVO4 laser at the top consists of a

On the physics of the pressure and temperature gradients in the edge of tokamak plasmas

NASA Astrophysics Data System (ADS)

Stacey, Weston M.

2018-04-01

An extended plasma fluid theory including atomic physics, radiation, electromagnetic and themodynamic forces, external sources of particles, momentum and energy, and kinetic ion orbit loss is employed to derive theoretical expressions that display the role of the various factors involved in the determination of the pressure and temperature gradients in the edge of tokamak plasmas. Calculations for current experiments are presented to illustrate the magnitudes of various effects including strong radiative and atomic physics edge cooling effects and strong reduction in ion particle and energy fluxes due to ion orbit loss in the plasma edge. An important new insight is the strong relation between rotation and the edge pressure gradient.

Machine learning reveals orbital interaction in materials

NASA Astrophysics Data System (ADS)

Lam Pham, Tien; Kino, Hiori; Terakura, Kiyoyuki; Miyake, Takashi; Tsuda, Koji; Takigawa, Ichigaku; Chi Dam, Hieu

2017-12-01

We propose a novel representation of materials named an 'orbital-field matrix (OFM)', which is based on the distribution of valence shell electrons. We demonstrate that this new representation can be highly useful in mining material data. Experimental investigation shows that the formation energies of crystalline materials, atomization energies of molecular materials, and local magnetic moments of the constituent atoms in bimetal alloys of lanthanide metal and transition-metal can be predicted with high accuracy using the OFM. Knowledge regarding the role of the coordination numbers of the transition-metal and lanthanide elements in determining the local magnetic moments of the transition-metal sites can be acquired directly from decision tree regression analyses using the OFM.

Influence of the photon orbital angular momentum on electric dipole transitions: negative experimental evidence.

PubMed

Giammanco, F; Perona, A; Marsili, P; Conti, F; Fidecaro, F; Gozzini, S; Lucchesini, A

2017-01-15

We describe an experiment of atomic spectroscopy devoted to ascertaining whether the orbital angular momentum (OAM) of photons has the same property of interacting with atoms or molecules as occurs for the spin angular momentum (SAM). In our experiment, rubidium vapors are excited by means of laser radiation with different combinations of OAM and SAM, particularly selected to inhibit or enhance the fluorescence according to the selection rules for the electric dipole transitions between the fundamental state and the first excited doublet. Our results clearly show that an electric-dipole-type transition is insensitive to the OAM value, and provide an original validation of a problem long debated in theoretical works.

Electron correlation within the relativistic no-pair approximation

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

Almoukhalalati, Adel; Saue, Trond, E-mail: trond.saue@irsamc.ups-tlse.fr; Knecht, Stefan

This paper addresses the definition of correlation energy within 4-component relativistic atomic and molecular calculations. In the nonrelativistic domain the correlation energy is defined as the difference between the exact eigenvalue of the electronic Hamiltonian and the Hartree-Fock energy. In practice, what is reported is the basis set correlation energy, where the “exact” value is provided by a full Configuration Interaction (CI) calculation with some specified one-particle basis. The extension of this definition to the relativistic domain is not straightforward since the corresponding electronic Hamiltonian, the Dirac-Coulomb Hamiltonian, has no bound solutions. Present-day relativistic calculations are carried out within themore » no-pair approximation, where the Dirac-Coulomb Hamiltonian is embedded by projectors eliminating the troublesome negative-energy solutions. Hartree-Fock calculations are carried out with the implicit use of such projectors and only positive-energy orbitals are retained at the correlated level, meaning that the Hartree-Fock projectors are frozen at the correlated level. We argue that the projection operators should be optimized also at the correlated level and that this is possible by full Multiconfigurational Self-Consistent Field (MCSCF) calculations, that is, MCSCF calculations using a no-pair full CI expansion, but including orbital relaxation from the negative-energy orbitals. We show by variational perturbation theory that the MCSCF correlation energy is a pure MP2-like correlation expression, whereas the corresponding CI correlation energy contains an additional relaxation term. We explore numerically our theoretical analysis by carrying out variational and perturbative calculations on the two-electron rare gas atoms with specially tailored basis sets. In particular, we show that the correlation energy obtained by the suggested MCSCF procedure is smaller than the no-pair full CI correlation energy, in accordance with the underlying minmax principle and our theoretical analysis. We also show that the relativistic correlation energy, obtained from no-pair full MCSCF calculations, scales at worst as X{sup −2} with respect to the cardinal number X of our correlation-consistent basis sets optimized for the two-electron atoms. This is better than the X{sup −1} scaling suggested by previous studies, but worse than the X{sup −3} scaling observed in the nonrelativistic domain. The well-known 1/Z- expansion in nonrelativistic atomic theory follows from coordinate scaling. We point out that coordinate scaling for consistency should be accompanied by velocity scaling. In the nonrelativistic domain this comes about automatically, whereas in the relativistic domain an explicit scaling of the speed of light is required. This in turn explains why the relativistic correlation energy to the lowest order is not independent of nuclear charge, in contrast to nonrelativistic theory.« less

Atomic orbital-based SOS-MP2 with tensor hypercontraction. II. Local tensor hypercontraction

NASA Astrophysics Data System (ADS)

Song, Chenchen; Martínez, Todd J.

2017-01-01

In the first paper of the series [Paper I, C. Song and T. J. Martinez, J. Chem. Phys. 144, 174111 (2016)], we showed how tensor-hypercontracted (THC) SOS-MP2 could be accelerated by exploiting sparsity in the atomic orbitals and using graphical processing units (GPUs). This reduced the formal scaling of the SOS-MP2 energy calculation to cubic with respect to system size. The computational bottleneck then becomes the THC metric matrix inversion, which scales cubically with a large prefactor. In this work, the local THC approximation is proposed to reduce the computational cost of inverting the THC metric matrix to linear scaling with respect to molecular size. By doing so, we have removed the primary bottleneck to THC-SOS-MP2 calculations on large molecules with O(1000) atoms. The errors introduced by the local THC approximation are less than 0.6 kcal/mol for molecules with up to 200 atoms and 3300 basis functions. Together with the graphical processing unit techniques and locality-exploiting approaches introduced in previous work, the scaled opposite spin MP2 (SOS-MP2) calculations exhibit O(N2.5) scaling in practice up to 10 000 basis functions. The new algorithms make it feasible to carry out SOS-MP2 calculations on small proteins like ubiquitin (1231 atoms/10 294 atomic basis functions) on a single node in less than a day.

Atomic oxygen beam source for erosion simulation

NASA Technical Reports Server (NTRS)

Cuthbertson, J. W.; Langer, W. D.; Motley, R. W.; Vaughn, J. A.

1991-01-01

A device for the production of low energy (3 to 10 eV) neutral atomic beams for surface modification studies is described that reproduces the flux of atomic oxygen in low Earth orbit. The beam is produced by the acceleration of plasma ions onto a negatively biased plate of high-Z metal; the ions are neutralized and reflected by the surface, retaining some fraction of their incident kinetic energy, forming a beam of atoms. The plasma is generated by a coaxial RF exciter which produces a magnetically-confined (4 kG) plasma column. At the end of the column, ions fall through the sheath to the plate, whose bias relative to the plasma can be varied to adjust the beam energy. The source provides a neutral flux approximately equal to 5 x 10(exp 16)/sq cm at a distance of 9 cm and a fluence approximately equal to 10(exp 20)/sq cm in five hours. The composition and energy of inert gas beams was diagnosed using a mass spectometer/energy analyzer. The energy spectra of the beams demonstrate energies in the range 5 to 15 eV, and qualitatively show expected dependences upon incident and reflecting atom species and potential drop. Samples of carbon film, carbon-based paint, Kapton, mylar, and teflon exposed to atomic O beams show erosion quite similar to that observed in orbit on the space shuttle.

Preferred site occupation of 3 d atoms in NixF e4 -xN (x =1 and 3) films revealed by x-ray absorption spectroscopy and magnetic circular dichroism

NASA Astrophysics Data System (ADS)

Takata, Fumiya; Ito, Keita; Takeda, Yukiharu; Saitoh, Yuji; Takanashi, Koki; Kimura, Akio; Suemasu, Takashi

2018-02-01

X-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism measurements were performed at the Ni and Fe L2 ,3 absorption edges for N ixF e4 -xN (x =1 and 3) epitaxial films. Spectral line-shape analysis and element-specific magnetic moment evaluations are presented. Shoulders at approximately 2 eV above the Ni L2 ,3 main peaks in the XAS spectrum of N i3FeN were interpreted to originate from hybridization of orbitals between Ni 3 d at face-centered (II) sites and N 2 p at body-centered sites, while such features were missing in NiF e3N film. Similar shoulders were observed at Fe L2 ,3 edges in both films. These results indicate that the orbitals of Ni atoms did not hybridize with those of N atoms in the NiF e3N film. Hence, Ni atoms preferentially occupied corner (I) sites, where the hybridization was weak because of the relatively long distance between Ni at I sites and N atoms. The relatively large magnetic moment deduced from sum-rule analysis of NiF e3N also showed a good agreement with the presence of Ni atoms at I sites.

Atomic orbital-based SOS-MP2 with tensor hypercontraction. II. Local tensor hypercontraction.

PubMed

Song, Chenchen; Martínez, Todd J

2017-01-21

In the first paper of the series [Paper I, C. Song and T. J. Martinez, J. Chem. Phys. 144, 174111 (2016)], we showed how tensor-hypercontracted (THC) SOS-MP2 could be accelerated by exploiting sparsity in the atomic orbitals and using graphical processing units (GPUs). This reduced the formal scaling of the SOS-MP2 energy calculation to cubic with respect to system size. The computational bottleneck then becomes the THC metric matrix inversion, which scales cubically with a large prefactor. In this work, the local THC approximation is proposed to reduce the computational cost of inverting the THC metric matrix to linear scaling with respect to molecular size. By doing so, we have removed the primary bottleneck to THC-SOS-MP2 calculations on large molecules with O(1000) atoms. The errors introduced by the local THC approximation are less than 0.6 kcal/mol for molecules with up to 200 atoms and 3300 basis functions. Together with the graphical processing unit techniques and locality-exploiting approaches introduced in previous work, the scaled opposite spin MP2 (SOS-MP2) calculations exhibit O(N 2.5 ) scaling in practice up to 10 000 basis functions. The new algorithms make it feasible to carry out SOS-MP2 calculations on small proteins like ubiquitin (1231 atoms/10 294 atomic basis functions) on a single node in less than a day.

Orbital Debris Shape Characterization Project Abstract

NASA Technical Reports Server (NTRS)

Pease, Jessie

2016-01-01

I have been working on a project to further our understanding of orbital debris by helping create a new dataset previously too complex to be implemented in past orbital debris propagation models. I am doing this by creating documentation and 3D examples and illustrations of the shape categories. Earlier models assumed all orbital debris to be spherical aluminum fragments. My project will help expand our knowledge of shape populations to 6 categories: Straight Needle/Rod/Cylinder, Bent Needle/Rod/Cylinder, Flat Plate, Bent Plate, Nugget/Parallelepiped/Spheroid, and Flexible. The last category, Flexible, is still up for discussion and may be modified. These categories will be used to characterize fragments in the DebriSat experiment.

Atomic Oxygen Durability Testing of an International Space Station Solar Array Validation Coupon

NASA Technical Reports Server (NTRS)

Forkapa, Mark J.; Stidham, Curtis; Banks, Bruce A.; Rutledge, Sharon K.; Ma, David H.; Sechkar, Edward A.

1996-01-01

An International Space Station solar array validation coupon was exposed in a directed atomic oxygen beam for space environment durability testing at the NASA Lewis Research Center. Exposure to atomic oxygen and intermittent tensioning of the solar array were conducted to verify the solar array#s durability to low Earth orbital atomic oxygen and to the docking threat of plume loading both of which are anticipated over its expected mission life of fifteen years. The validation coupon was mounted on a specially designed rotisserie. The rotisserie mounting enabled the solar and anti-solar facing side of the array to be exposed to directed atomic oxygen in a sweeping arrival process replicating space exposure. The rotisserie mounting also enabled tensioning, in order to examine the durability of the array and its hinge to simulated plume loads. Flash testing to verify electrical performance of the solar array was performed with a solar simulator before and after the exposure to atomic oxygen and tensile loading. Results of the flash testing indicated little or no degradation in the solar array#s performance. Photographs were also taken of the array before and after the durability testing and are included along with comparisons and discussions in this report. The amount of atomic oxygen damage appeared minor with the exception of a very few isolated defects. There were also no indications that the simulated plume loadings had weakened or damaged the array, even though there was some erosion of Kapton due to atomic oxygen attack. Based on the results of this testing, it is apparent that the International Space Station#s solar arrays should survive the low Earth orbital atomic oxygen environment and docking threats which are anticipated over its expected mission life.

A model to assess the Mars Telecommunications Network relay robustness

NASA Technical Reports Server (NTRS)

Girerd, Andre R.; Meshkat, Leila; Edwards, Charles D., Jr.; Lee, Charles H.

2005-01-01

The relatively long mission durations and compatible radio protocols of current and projected Mars orbiters have enabled the gradual development of a heterogeneous constellation providing proximity communication services for surface assets. The current and forecasted capability of this evolving network has reached the point that designers of future surface missions consider complete dependence on it. Such designers, along with those architecting network requirements, have a need to understand the robustness of projected communication service. A model has been created to identify the robustness of the Mars Network as a function of surface location and time. Due to the decade-plus time horizon considered, the network will evolve, with emerging productive nodes and nodes that cease or fail to contribute. The model is a flexible framework to holistically process node information into measures of capability robustness that can be visualized for maximum understanding. Outputs from JPL's Telecom Orbit Analysis Simulation Tool (TOAST) provide global telecom performance parameters for current and projected orbiters. Probabilistic estimates of orbiter fuel life are derived from orbit keeping burn rates, forecasted maneuver tasking, and anomaly resolution budgets. Orbiter reliability is estimated probabilistically. A flexible scheduling framework accommodates the projected mission queue as well as potential alterations.

Project Physics Text 5, Models of the Atom.

ERIC Educational Resources Information Center

Harvard Univ., Cambridge, MA. Harvard Project Physics.

Basic atomic theories are presented in this fifth unit of the Project Physics text for use by senior high students. Chemical basis of atomic models in the early years of the 18th Century is discussed n connection with Dalton's theory, atomic properties, and periodic tables. The discovery of electrons is described by using cathode rays, Millikan's…

An atomic mean-field spin-orbit approach within exact two-component theory for a non-perturbative treatment of spin-orbit coupling

NASA Astrophysics Data System (ADS)

Liu, Junzi; Cheng, Lan

2018-04-01

An atomic mean-field (AMF) spin-orbit (SO) approach within exact two-component theory (X2C) is reported, thereby exploiting the exact decoupling scheme of X2C, the one-electron approximation for the scalar-relativistic contributions, the mean-field approximation for the treatment of the two-electron SO contribution, and the local nature of the SO interactions. The Hamiltonian of the proposed SOX2CAMF scheme comprises the one-electron X2C Hamiltonian, the instantaneous two-electron Coulomb interaction, and an AMF SO term derived from spherically averaged Dirac-Coulomb Hartree-Fock calculations of atoms; no molecular relativistic two-electron integrals are required. Benchmark calculations for bond lengths, harmonic frequencies, dipole moments, and electric-field gradients for a set of diatomic molecules containing elements across the periodic table show that the SOX2CAMF scheme offers a balanced treatment for SO and scalar-relativistic effects and appears to be a promising candidate for applications to heavy-element containing systems. SOX2CAMF coupled-cluster calculations of molecular properties for bismuth compounds (BiN, BiP, BiF, BiCl, and BiI) are also presented and compared with experimental results to further demonstrate the accuracy and applicability of the SOX2CAMF scheme.

Studies of the chemistry of the nightside ionosphere of Venus

NASA Technical Reports Server (NTRS)

Fox, J. L.

1991-01-01

A combination of numerical modeling and analysis of the Pioneer Venus UADS data base is studied, specifically data from the orbiter ion mass spectrometer (OIMS), orbiter neutral mass spectrometer (ONMS), and orbiter electron temperature probe (OETP). A one dimensional model of the Venus nightside ionosphere was set up in which downward fluxes of atomic ions are introduced at the upper boundary to simulate transport of ions from the dayside. The model shows that the densities of mass-28 ions, CO(+) + N(2+), resulting from an influx of atomic ions from the dayside are quite small, due to the high ionization potentials of CO and N2 that make chemical production difficult. A look at the data reveals that the actual densities of mass-28 ions are quite variable, from values near 10 to more than 10(exp 4) cm(exp -3). The excess mass-28 ions are assumed to be produced by electron precipitation and that the presence of high densities of mass-28 ions is a signature of auroral precipitation. A discussion of the atomic oxygen green line in the nightglow of Venus, which is produced mainly by dissociative recombination of O(2+), is presented. Original calculations of production rates of excited states for models based on Pioneer Venus data are also presented.

Spin-orbit coupling manipulating composite topological spin textures in atomic-molecular Bose-Einstein condensates

NASA Astrophysics Data System (ADS)

Liu, Chao-Fei; Juzeliūnas, Gediminas; Liu, W. M.

2017-02-01

Atomic-molecular Bose-Einstein condensates (BECs) offer brand new opportunities to revolutionize quantum gases and probe the variation of fundamental constants with unprecedented sensitivity. The recent realization of spin-orbit coupling (SOC) in BECs provides a new platform for exploring completely new phenomena unrealizable elsewhere. In this study, we find a way of creating a Rashba-Dresselhaus SOC in atomic-molecular BECs by combining the spin-dependent photoassociation and Raman coupling, which can control the formation and distribution of a different type of topological excitation—carbon-dioxide-like skyrmion. This skyrmion is formed by two half-skyrmions of molecular BECs coupling with one skyrmion of atomic BECs, where the two half-skyrmions locate at both sides of one skyrmion. Carbon-dioxide-like skyrmion can be detected by measuring the vortices structures using the time-of-flight absorption imaging technique in real experiments. Furthermore, we find that SOC can effectively change the occurrence of the Chern number in k space, which causes the creation of topological spin textures from some separated carbon-dioxide-like monomers each with topological charge -2 to a polymer chain of the skyrmions. This work helps in creating dual SOC atomic-molecular BECs and opens avenues to manipulate topological excitations.

A theoretical investigation on the neutral Cu(I) phosphorescent complexes with azole-based and phosphine mixed ligand

NASA Astrophysics Data System (ADS)

Ding, Xiao-Li; Shen, Lu; Zou, Lu-Yi; Ma, Ming-Shuo; Ren, Ai-Min

2018-04-01

A theoretical study on a series of neutral heteroleptic Cu(I) complexes with different azole-pyridine-based N^N ligands has been presented to get insight into the effect of various nitrogen atoms in the azole ring on photophysical properties. The results reveal that the highest occupied molecular orbital (HOMO) levels and the emission wavelengths of these complexes are mainly governed by the nitrogen atom number in azole ring. With the increasing number of nitrogen atom , the electron density distribution of HOMO gradually extend from the N^N ligand to the whole molecule, meanwhile, the improved contribution from Cu(d) orbits in HOMO results in an effective mixing of various charge transfermodes, and hence, the fast radiative decay(kr) and the slow non-radiative decay rate(knr) are achieved. The photoluminescence quantum yield (PLQY) show an apparent dependence on the nitrogen atom number in the five-membered nitrogen heterocycles. However, the increasing number of nitrogen atoms is not necessary for increasing PLQY. The complex 3 with 1,2,4-triazole-pyridine-based N^N ligands is considered to be a potential emitter with high phosphorescence efficiency. Finally, we hope that our investigations will contribute to systematical understanding and guiding for material molecular engineering.

Natural bond orbital approach to the transmission of substituent effect through the fulvene and benzene ring systems.

PubMed

Oziminski, Wojciech P; Krygowski, Tadeusz M

2011-03-01

Electronic structure of 22 monosubstituted derivatives of benzene and exocyclically substituted fulvene with substituents: B(OH)(2), BH(2), CCH, CF(3), CH(3), CHCH(2), CHO, Cl, CMe(3), CN, COCH(3), CONH(2), COOH, F, NH(2), NMe(2), NO, NO(2), OCH(3), OH, SiH(3), SiMe(3) were studied theoretically by means of Natural Bond Orbital analysis. It is shown, that sum of π-electron population of carbon atoms of the fulvene and benzene rings, pEDA(F) and pEDA(B), respectively correlate well with Hammett substituent constants [Formula in text] and aromaticity index NICS. The substituent effect acting on pi-electron occupation at carbon atoms of the fulvene ring is significantly stronger than in the case of benzene. Electron occupations of ring carbon atoms (except C1) in fulvene plotted against each other give linear regressions with high correlation coefficients. The same is true for ortho- and para-carbon atoms in benzene. Positive slopes of the regressions indicate similar for fulvene and benzene kind of substituent effect - mostly resonance in nature. Only the regressions of occupation at the carbon atom in meta- position of benzene against ortho- and para-positions gives negative slopes and low correlation coefficients.

Application of the Covalent Bond Classification Method for the Teaching of Inorganic Chemistry

ERIC Educational Resources Information Center

Green, Malcolm L. H.; Parkin, Gerard

2014-01-01

The Covalent Bond Classification (CBC) method provides a means to classify covalent molecules according to the number and types of bonds that surround an atom of interest. This approach is based on an elementary molecular orbital analysis of the bonding involving the central atom (M), with the various interactions being classified according to the…

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" -…

Analytic energy gradient of projected Hartree-Fock within projection after variation

NASA Astrophysics Data System (ADS)

Uejima, Motoyuki; Ten-no, Seiichiro

2017-03-01

We develop a geometrical optimization technique for the projection-after-variation (PAV) scheme of the recently refined projected Hartree-Fock (PHF) as a fast alternative to the variation-after-projection (VAP) approach for optimizing the structures of molecules/clusters in symmetry-adapted electronic states at the mean-field computational cost. PHF handles the nondynamic correlation effects by restoring the symmetry of a broken-symmetry single reference wavefunction and moreover enables a black-box treatment of orbital selections. Using HF orbitals instead of PHF orbitals, our approach saves the computational cost for the orbital optimization, avoiding the convergence problem that sometimes emerges in the VAP scheme. We show that PAV-PHF provides geometries comparable to those of the complete active space self-consistent field and VAP-PHF for the tested systems, namely, CH2, O3, and the [Cu2O2 ] 2 + core, where nondynamic correlation is abundant. The proposed approach is useful for large systems mainly dominated by nondynamic correlation to find stable structures in many symmetry-adapted states.

Attenuation of Scattered Thermal Energy Atomic Oxygen

NASA Technical Reports Server (NTRS)

Banks, Bruce a.; Seroka, Katelyn T.; McPhate, Jason B.; Miller, Sharon K.

2011-01-01

The attenuation of scattered thermal energy atomic oxygen is relevant to the potential damage that can occur within a spacecraft which sweeps through atomic oxygen in low Earth orbit (LEO). Although there can be significant oxidation and resulting degradation of polymers and some metals on the external surfaces of spacecraft, there are often openings on a spacecraft such as telescope apertures, vents, and microwave cavities that can allow atomic oxygen to enter and scatter internally to the spacecraft. Atomic oxygen that enters a spacecraft can thermally accommodate and scatter to ultimately react or recombine on surfaces. The atomic oxygen that does enter a spacecraft can be scavenged by use of high erosion yield polymers to reduce its reaction on critical surfaces and materials. Polyoxymethylene and polyethylene can be used as effective atomic oxygen scavenging polymers.

Experimental verification of orbital engineering at the atomic scale: Charge transfer and symmetry breaking in nickelate heterostructures

NASA Astrophysics Data System (ADS)

Phillips, Patrick J.; Rui, Xue; Georgescu, Alexandru B.; Disa, Ankit S.; Longo, Paolo; Okunishi, Eiji; Walker, Fred; Ahn, Charles H.; Ismail-Beigi, Sohrab; Klie, Robert F.

2017-05-01

Epitaxial strain, layer confinement, and inversion symmetry breaking have emerged as powerful new approaches to control the electronic and atomic-scale structural properties of complex metal oxides. Trivalent rare-earth (RE) nickelate R E NiO3 heterostructures have been shown to be exemplars since the orbital occupancy, degeneracy, and, consequently, electronic/magnetic properties can be altered as a function of epitaxial strain, layer thickness, and superlattice structure. One recent example is the tricomponent LaTiO3-LaNiO3-LaAlO3 superlattice which exhibits charge transfer and orbital polarization as the result of its interfacial dipole electric field. A crucial step towards control of these parameters for future electronic and magnetic device applications is to develop an understanding of both the magnitude and range of the octahedral network's response towards interfacial strain and electric fields. An approach that provides atomic-scale resolution and sensitivity towards the local octahedral distortions and orbital occupancy is therefore required. Here, we employ atomic-resolution imaging coupled with electron spectroscopies and first-principles theory to examine the role of interfacial charge transfer and symmetry breaking in a tricomponent nickelate superlattice system. We find that nearly complete charge transfer occurs between the LaTiO3 and LaNiO3 layers, resulting in a mixed Ni2 +/Ni3 + valence state. We further demonstrate that this charge transfer is highly localized with a range of about 1 unit cell within the LaNiO3 layers. We also show how Wannier-function-based electron counting provides a simple physical picture of the electron distribution that connects directly with formal valence charges. The results presented here provide important feedback to synthesis efforts aimed at stabilizing new electronic phases that are not accessible by conventional bulk or epitaxial film approaches.

Drag coefficient Variability and Thermospheric models

NASA Astrophysics Data System (ADS)

Moe, Kenneth

Satellite drag coefficients depend upon a variety of factors: The shape of the satellite, its altitude, the eccentricity of its orbit, the temperature and mean molecular mass of the ambient atmosphere, and the time in the sunspot cycle. At altitudes where the mean free path of the atmospheric molecules is large compared to the dimensions of the satellite, the drag coefficients can be determined from the theory of free-molecule flow. The dependence on altitude is caused by the concentration of atomic oxygen which plays an important role by its ability to adsorb on the satellite surface and thereby affect the energy loss of molecules striking the surface. The eccentricity of the orbit determines the satellite velocity at perigee, and therefore the energy of the incident molecules relative to the energy of adsorption of atomic oxygen atoms on the surface. The temperature of the ambient atmosphere determines the extent to which the random thermal motion of the molecules influences the momentum transfer to the satellite. The time in the sunspot cycle affects the ambient temperature as well as the concentration of atomic oxygen at a particular altitude. Tables and graphs will be used to illustrate the variability of drag coefficients. Before there were any measurements of gas-surface interactions in orbit, Izakov and Cook independently made an excellent estimate that the drag coefficient of satellites of compact shape would be 2.2. That numerical value, independent of altitude, was used by Jacchia to construct his model from the early measurements of satellite drag. Consequently, there is an altitude dependent bias in the model. From the sparce orbital experiments that have been done, we know that the molecules which strike satellite surfaces rebound in a diffuse angular distribution with an energy loss given by the energy accommodation coefficient. As more evidence accumulates on the energy loss, more realistic drag coefficients are being calculated. These improved drag coefficients help evaluate the biases in present models. Moreover, they make possible the derivation of accurate densities from accelerometer measurements.

Self-consistent assessment of Englert-Schwinger model on atomic properties

NASA Astrophysics Data System (ADS)

Lehtomäki, Jouko; Lopez-Acevedo, Olga

2017-12-01

Our manuscript investigates a self-consistent solution of the statistical atom model proposed by Berthold-Georg Englert and Julian Schwinger (the ES model) and benchmarks it against atomic Kohn-Sham and two orbital-free models of the Thomas-Fermi-Dirac (TFD)-λvW family. Results show that the ES model generally offers the same accuracy as the well-known TFD-1/5 vW model; however, the ES model corrects the failure in the Pauli potential near-nucleus region. We also point to the inability of describing low-Z atoms as the foremost concern in improving the present model.

Self-consistent assessment of Englert-Schwinger model on atomic properties.

PubMed

Lehtomäki, Jouko; Lopez-Acevedo, Olga

2017-12-21

Our manuscript investigates a self-consistent solution of the statistical atom model proposed by Berthold-Georg Englert and Julian Schwinger (the ES model) and benchmarks it against atomic Kohn-Sham and two orbital-free models of the Thomas-Fermi-Dirac (TFD)-λvW family. Results show that the ES model generally offers the same accuracy as the well-known TFD-15vW model; however, the ES model corrects the failure in the Pauli potential near-nucleus region. We also point to the inability of describing low-Z atoms as the foremost concern in improving the present model.

Protocol for Atomic Oxygen Testing of Materials in Ground-Based Facilities. No. 2

NASA Technical Reports Server (NTRS)

Minton, Timothy K.

1995-01-01

A second version of standard guidelines is proposed for improving materials testing in ground-based atomic oxygen environments for the purpose of predicting the durability of the tested materials in low Earth orbit (LEO). Accompanying these guidelines are background information and notes about testing. Both the guidelines and the additional information are intended to aid users who wish to evaluate the potential hazard of atomic oxygen in LEO to a candidate space component without actually flying the component in space, and to provide a framework for more consistent atomic oxygen testing in the future.

Atomic Oxygen Durability Evaluation of Protected Polymers Using Thermal Energy Plasma Systems

NASA Technical Reports Server (NTRS)

Banks, Bruce A.; Rutledge, Sharon K.; Degroh, Kim K.; Stidham, Curtis R.; Gebauer, Linda; Lamoreaux, Cynthia M.

1995-01-01

The durability evaluation of protected polymers intended for use in low Earth orbit (LEO) has necessitated the use of large-area, high-fluence, atomic oxygen exposure systems. Two thermal energy atomic oxygen exposure systems which are frequently used for such evaluations are radio frequency (RF) plasma ashers and electron cyclotron resonance plasma sources. Plasma source testing practices such as ample preparation, effective fluence prediction, atomic oxygen flux determination, erosion measurement, operational considerations, and erosion yield measurements are presented. Issues which influence the prediction of in-space durability based on ground laboratory thermal energy plasma system testing are also addressed.

Vibrational spectroscopic and DFT calculation studies of 2-amino-7-bromo-5-oxo-[1]benzopyrano [2,3-b]pyridine-3 carbonitrile.

PubMed

Premkumar, S; Jawahar, A; Mathavan, T; Kumara Dhas, M; Milton Franklin Benial, A

2015-03-05

The vibrational spectra of 2-amino-7-bromo-5-oxo-[1]benzopyrano [2,3-b]pyridine-3 carbonitrile were recorded using fourier transform-infrared and fourier transform-Raman spectrometer. The optimized structural parameters, vibrational frequencies, Mulliken atomic charge distribution, frontier molecular orbitals, thermodynamic properties, temperature dependence of thermodynamic parameters, first order hyperpolarizability and natural bond orbital calculations of the molecule were performed using the Gaussian 09 program. The vibrational frequencies were assigned on the basis of potential energy distribution calculation using the VEDA 4.0 program. The calculated first order hyperpolarizability of ABOBPC molecule was obtained as 6.908×10(-30) issue, which was 10.5 times greater than urea. The nonlinear optical activity of the molecule was also confirmed by the frontier molecular orbitals and natural bond orbital analysis. The frontier molecular orbitals analysis shows that the lower energy gap of the molecule, which leads to the higher value of first order hyperpolarizability. The natural bond orbital analysis indicates that the nonlinear optical activity of the molecule arises due to the π→π(∗) transitions. The Mulliken atomic charge distribution confirms the presence of intramolecular charge transfer within the molecule. The reactive site of the molecule was predicted from the molecular electrostatic potential contour map. The values of thermo dynamic parameters were increasing with increasing temperature. Copyright © 2014 Elsevier B.V. All rights reserved.

Molecular orbital study of some eight-coordinate sulfur chelate complexes of molybdenum

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

Perkins, P.G.; Schultz, F.A.

1983-03-30

A number of molybdenum complexes involving the formal oxidation states Mo(IV) and Mo(V) have been studied by a self-consistent-field molecular orbital technique. All the complexes were of dodecahedral geometry and had eight sulfurs chelated to the central metal atom. In all, a series of five tetrakis complexes was studied, including the ligands dithiocarbamate (dtc), thioxanthate (txn), 1,1-dicyano-2,2-ethylenedithiolate (i-mnt), 1-cyano-1-carbethoxy-2,2-ethylenedithiolate (ced), and 1,1-dicarbethoxy-2,2-ethylenedithiolate (ded). The 4d orbitals were included on molybdenum, and the empty 3d levels on all sulfur atoms. The results show that the highest occupied molecular orbital in each case has over 90% metal d/sub xy/ character. Further, themore » energy of this orbital is linearly related to the reversible half-wave potentials for Mo(IV) ..-->.. Mo(V) and Mo(V) ..-->.. Mo(VI) oxidations of the complexes. A further irreversible oxidation observed experimentally also is closely related to the calculated energy levels. Relationships between the calculated results and Mo 3d/sub 5///sub 2/ X-ray photoelectron binding energies, EPR parameters, and charge-transfer absorption energies are discussed. Electrochemical and spectroscopic properties of these MoS/sub 8/ complexes can be understood in terms of a manifold of orbital energies that retain approximately constant spacings between one another and that move up or down in absolute energy in response to the charge donated or withdrawn by the ligands.« less

Ionic Impurity in a Bose-Einstein Condensate at Submicrokelvin Temperatures

NASA Astrophysics Data System (ADS)

Kleinbach, K. S.; Engel, F.; Dieterle, T.; Löw, R.; Pfau, T.; Meinert, F.

2018-05-01

Rydberg atoms immersed in a Bose-Einstein condensate interact with the quantum gas via electron-atom and ion-atom interaction. To suppress the typically dominant electron-neutral interaction, Rydberg states with a principal quantum number up to n =190 are excited from a dense and tightly trapped micron-sized condensate. This allows us to explore a regime where the Rydberg orbit exceeds the size of the atomic sample by far. In this case, a detailed line shape analysis of the Rydberg excitation spectrum provides clear evidence for ion-atom interaction at temperatures well below a microkelvin. Our results may open up ways to enter the quantum regime of ion-atom scattering for the exploration of charged quantum impurities and associated polaron physics.

Heavy Atom Effect of Bromine Significantly Enhances Exciton Utilization of Delayed Fluorescence Luminogens.

PubMed

Gan, Shifeng; Hu, Shimin; Li, Xiang-Long; Zeng, Jiajie; Zhang, Dongdong; Huang, Tianyu; Luo, Wenwen; Zhao, Zujin; Duan, Lian; Su, Shi-Jian; Tang, Ben Zhong

2018-05-23

Raising triplet exciton utilization of pure organic luminescent materials is of significant importance for efficiency advancement of organic light-emitting diodes (OLEDs). Herein, by introducing bromine atom(s) onto a typical molecule (bis(carbazol-9-yl)-4,5-dicyanobenzene) with thermally activated delayed fluorescence, we demonstrate that the heavy atom effect of bromine can increase spin-orbit coupling and promote the reverse intersystem crossing, which endow the molecules with more distinct delayed fluorescence. In consequence, the triplet exciton utilization is improved greatly with the increase of bromine atoms, affording apparently advanced external quantum efficiencies of OLEDs. Utilizing the enhancement effect of bromine atoms on delayed fluorescence should be a simple and promising design concept for efficient organic luminogens with high exciton utilization.

Making two dysprosium atoms rotate —Einstein-de Haas effect revisited

NASA Astrophysics Data System (ADS)

Górecki, Wojciech; Rzążewski, Kazimierz

2016-10-01

We present a numerical study of the behaviour of two magnetic dipolar atoms trapped in a harmonic potential and exhibiting the standard Einstein-de Haas effect while subject to a time-dependent homogeneous magnetic field. Using a simplified description of the short-range interaction and the full expression for the dipole-dipole forces we show that under experimentally realisable conditions two dysprosium atoms may be pumped to a high (l > 20) value of the relative orbital angular momentum.

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

Kawahara, Hajime, E-mail: divrot@gmail.com

We consider the effect of planetary spin on the planetary radial velocity (PRV) in dayside spectra of exoplanets. To understand the spin effect qualitatively, we derive an analytic formula of the intensity-weighted radial velocity from the planetary surface on the following assumptions: (1) constant and solid rotation without precession, (2) stable and uniform distribution of molecules/atoms, (3) emission models from the dayside hemisphere, and (4) a circular orbit. On these assumptions, we find that the curve of the PRV is distorted by the planetary spin and this anomaly is characterized by the spin radial velocity at the equator and amore » projected angle on a celestial plane between the spin axis and the axis of orbital motion {lambda}{sub p} in a manner analogous to the Rossiter-McLaughlin effect. The latter can constrain the planetary obliquity. Creating mock PRV data with 3 km s{sup -1} accuracy, we demonstrate how {lambda}{sub p} and the spin radial velocity at the equator are estimated. We find that the stringent constraint of eccentricity is crucial to detect the spin effect. Though our formula is still qualitative, we conclude that the PRV in the dayside spectra will be a powerful means for constraining the planetary spin.« less

BepiColombo — The Next Step of Mercury Exploration with Two Orbiting Spacecraft

NASA Astrophysics Data System (ADS)

Benkhoff, J.

2018-05-01

BepiColombo is a joint project between ESA and JAXA. The mission consists of two orbiters — the Mercury Planetary Orbiter and the Mercury Magnetospheric Orbiter. From dedicated orbits, the spacecraft will be studying the planet and its environment.

Three-Dimensional Printing of a Scalable Molecular Model and Orbital Kit for Organic Chemistry Teaching and Learning

ERIC Educational Resources Information Center

Penny, Matthew R.; Cao, Zi Jing; Patel, Bhaven; dos Santos, Bruno Sil; Asquith, Christopher R. M.; Szulc, Blanka R.; Rao, Zenobia X.; Muwaffak, Zaid; Malkinson, John P.; Hilton, Stephen T.

2017-01-01

Three-dimensional (3D) chemical models are a well-established learning tool used to enhance the understanding of chemical structures by converting two-dimensional paper or screen outputs into realistic three-dimensional objects. While commercial atom model kits are readily available, there is a surprising lack of large molecular and orbital models…

Understanding the quantum nature of low-energy C(3Pj) + He inelastic collisions

NASA Astrophysics Data System (ADS)

Bergeat, Astrid; Chefdeville, Simon; Costes, Michel; Morales, Sébastien B.; Naulin, Christian; Even, Uzi; Kłos, Jacek; Lique, François

2018-05-01

Inelastic collisions that occur between open-shell atoms and other atoms or molecules, and that promote a spin-orbit transition, involve multiple interaction potentials. They are non-adiabatic by nature and cannot be described within the Born-Oppenheimer approximation; in particular, their theoretical modelling becomes very challenging when the collision energies have values comparable to the spin-orbit splitting. Here we study inelastic collisions between carbon in its ground state C(3Pj=0) and helium atoms—at collision energies in the vicinity of spin-orbit excitation thresholds ( 0.2 and 0.5 kJ mol-1)—that result in spin-orbit excitation to C(3Pj=1) and C(3Pj=2). State-to-state integral cross-sections are obtained from crossed-beam experiments with a beam source that provides an almost pure beam of C(3Pj=0) . We observe very good agreement between experimental and theoretical results (acquired using newly calculated potential energy curves), which validates our characterization of the quantum dynamical resonances that are observed. Rate coefficients at very low temperatures suitable for chemical modelling of the interstellar medium are also calculated.

Gauge-origin dependence in electronic g-tensor calculations

NASA Astrophysics Data System (ADS)

Glasbrenner, Michael; Vogler, Sigurd; Ochsenfeld, Christian

2018-06-01

We present a benchmark study on the gauge-origin dependence of the electronic g-tensor using data from unrestricted density functional theory calculations with the spin-orbit mean field ansatz. Our data suggest in accordance with previous studies that g-tensor calculations employing a common gauge-origin are sufficiently accurate for small molecules; however, for extended molecules, the introduced errors can become relevant and significantly exceed the basis set error. Using calculations with the spin-orbit mean field ansatz and gauge-including atomic orbitals as a reference, we furthermore show that the accuracy and reliability of common gauge-origin approaches in larger molecules depends strongly on the locality of the spin density distribution. We propose a new pragmatic ansatz for choosing the gauge-origin which takes the spin density distribution into account and gives reasonably accurate values for molecules with a single localized spin center. For more general cases like molecules with several spatially distant spin centers, common gauge-origin approaches are shown to be insufficient for consistently achieving high accuracy. Therefore the computation of g-tensors using distributed gauge-origin methods like gauge-including atomic orbitals is considered as the ideal approach and is recommended for larger molecular systems.

Single-atom Catalysis Using Pt/Graphene Achieved through Atomic Layer Deposition

NASA Astrophysics Data System (ADS)

Sun, Shuhui; Zhang, Gaixia; Gauquelin, Nicolas; Chen, Ning; Zhou, Jigang; Yang, Songlan; Chen, Weifeng; Meng, Xiangbo; Geng, Dongsheng; Banis, Mohammad N.; Li, Ruying; Ye, Siyu; Knights, Shanna; Botton, Gianluigi A.; Sham, Tsun-Kong; Sun, Xueliang

2013-05-01

Platinum-nanoparticle-based catalysts are widely used in many important chemical processes and automobile industries. Downsizing catalyst nanoparticles to single atoms is highly desirable to maximize their use efficiency, however, very challenging. Here we report a practical synthesis for isolated single Pt atoms anchored to graphene nanosheet using the atomic layer deposition (ALD) technique. ALD offers the capability of precise control of catalyst size span from single atom, subnanometer cluster to nanoparticle. The single-atom catalysts exhibit significantly improved catalytic activity (up to 10 times) over that of the state-of-the-art commercial Pt/C catalyst. X-ray absorption fine structure (XAFS) analyses reveal that the low-coordination and partially unoccupied densities of states of 5d orbital of Pt atoms are responsible for the excellent performance. This work is anticipated to form the basis for the exploration of a next generation of highly efficient single-atom catalysts for various applications.

Single-atom Catalysis Using Pt/Graphene Achieved through Atomic Layer Deposition

PubMed Central

Sun, Shuhui; Zhang, Gaixia; Gauquelin, Nicolas; Chen, Ning; Zhou, Jigang; Yang, Songlan; Chen, Weifeng; Meng, Xiangbo; Geng, Dongsheng; Banis, Mohammad N.; Li, Ruying; Ye, Siyu; Knights, Shanna; Botton, Gianluigi A.; Sham, Tsun-Kong; Sun, Xueliang

2013-01-01

Platinum-nanoparticle-based catalysts are widely used in many important chemical processes and automobile industries. Downsizing catalyst nanoparticles to single atoms is highly desirable to maximize their use efficiency, however, very challenging. Here we report a practical synthesis for isolated single Pt atoms anchored to graphene nanosheet using the atomic layer deposition (ALD) technique. ALD offers the capability of precise control of catalyst size span from single atom, subnanometer cluster to nanoparticle. The single-atom catalysts exhibit significantly improved catalytic activity (up to 10 times) over that of the state-of-the-art commercial Pt/C catalyst. X-ray absorption fine structure (XAFS) analyses reveal that the low-coordination and partially unoccupied densities of states of 5d orbital of Pt atoms are responsible for the excellent performance. This work is anticipated to form the basis for the exploration of a next generation of highly efficient single-atom catalysts for various applications.

Influence of orbital symmetry on diffraction imaging with rescattering electron wave packets

DOE PAGES

Pullen, M. G.; Wolter, B.; Le, A. -T.; ...

2016-06-22

The ability to directly follow and time-resolve the rearrangement of the nuclei within molecules is a frontier of science that requires atomic spatial and few-femtosecond temporal resolutions. While laser-induced electron diffraction can meet these requirements, it was recently concluded that molecules with particular orbital symmetries (such as pg) cannot be imaged using purely backscattering electron wave packets without molecular alignment. Here, we demonstrate, in direct contradiction to these findings, that the orientation and shape of molecular orbitals presents no impediment for retrieving molecular structure with adequate sampling of the momentum transfer space. We overcome previous issues by showcasing retrieval ofmore » the structure of randomly oriented O 2 and C 2H 2 molecules, with π g and π u symmetries, respectively, and where their ionization probabilities do not maximize along their molecular axes. As a result, while this removes a serious bottleneck for laser-induced diffraction imaging, we find unexpectedly strong backscattering contributions from low-Z atoms.« less

Atomic-scale control of magnetic anisotropy via novel spin–orbit coupling effect in La 2/3Sr 1/3MnO 3/SrIrO 3 superlattices

DOE PAGES

Yi, Di; Liu, Jian; Hsu, Shang-Lin; ...

2016-05-19

Magnetic anisotropy (MA) is one of the most important material properties for modern spintronic devices. Conventional manipulation of the intrinsic MA, i.e., magnetocrystalline anisotropy (MCA), typically depends upon crystal symmetry. Extrinsic control over the MA is usually achieved by introducing shape anisotropy or exchange bias from another magnetically ordered material. Here we demonstrate a pathway to manipulate MA of 3d transition-metal oxides (TMOs) by digitally inserting nonmagnetic 5d TMOs with pronounced spin-orbit coupling (SOC). High-quality superlattices comprising ferromagnetic La 2/3Sr 1/3MnO 3 (LSMO) and paramagnetic SrIrO 3 (SIO) are synthesized with the precise control of thickness at the atomic scale.more » Magnetic easy-axis reorientation is observed by controlling the dimensionality of SIO, mediated through the emergence of a novel spin-orbit state within the nominally paramagnetic SIO.« less

A novel series of thiosemicarbazone drugs: From synthesis to structure

NASA Astrophysics Data System (ADS)

Ebrahimi, Hossein Pasha; Hadi, Jabbar S.; Alsalim, Tahseen A.; Ghali, Thaer S.; Bolandnazar, Zeinab

2015-02-01

A new series of thiosemicarbazones (TSCs) and their 1,3,4-thiadiazolines (TDZs) containing acetamide group have been synthesized from thiosemicarbazide compounds by the reaction of TSCs with cyclic ketones as well as aromatic aldehydes. The structures of newly synthesized 1,3,4-thiadiazole derivatives obtained by heterocyclization of the TSCs with acetic anhydride were experimentally characterized by spectral methods using IR, 1H NMR, 13C NMR and mass spectroscopic methods. Furthermore, the structural, thermodynamic, and electronic properties of the studied compounds were also studied theoretically by performing Density Functional Theory (DFT) to access reliable results to the experimental values. The molecular geometry, the highest occupied molecular orbital (HOMO), the lowest unoccupied molecular orbital (LUMO) and Mulliken atomic charges of the studied compounds have been calculated at the B3LYP method and standard 6-31+G(d,p) basis set starting from optimized geometry. The theoretical 13C chemical shift results were also calculated using the gauge independent atomic orbital (GIAO) approach and their respective linear correlations were obtained.

Spacecraft Materials in the Space Flight Environment: International Space Station - May 2002 to May 2007

NASA Technical Reports Server (NTRS)

Golden, John; Lorenz, Mary J.; Alred, John; Koontz, Steven L.; Pedley, Michael

2008-01-01

The performance of ISS spacecraft materials and systems on prolonged exposure to the low-Earth orbit (LEO) space flight is reported in this paper. In-flight data, flight crew observations, and the results of ground-based test and analysis directly supporting programmatic and operational decision-making are presented. The space flight environments definitions (both natural and induced) used for ISS design, material selection, and verification testing are shown, in most cases, to be more severe than the actual flight environment accounting for the outstanding performance of ISS as a long mission duration spacecraft. No significant ISS material or system failures have been attributed to spacecraft-environments interactions. Nonetheless, ISS materials and systems performance data is contributing to our understanding of spacecraft material interactions in the spaceflight environment so as to reduce cost and risk for future spaceflight projects and programs. Orbital inclination (51.6o) and altitude (nominally near 360 km) determine the set of natural environment factors affecting the functional life of materials and systems on ISS. ISS operates in an electrically conducting environment (the F2 region of Earth s ionosphere) with well-defined fluxes of atomic oxygen, other charged and neutral ionospheric plasma species, solar UV, VUV, and x-ray radiation as well as galactic cosmic rays, trapped radiation, and solar cosmic rays (1-4). The LEO micrometeoroid and orbital debris environment is an especially important determinant of spacecraft design and operations (5, 6). The magnitude of several environmental factors varies dramatically with latitude and longitude as ISS orbits the Earth (1-4). The high latitude orbital environment also exposes ISS to higher fluences of trapped energetic electrons, auroral electrons, solar cosmic rays, and galactic cosmic rays (1-4) than would be the case in lower inclination orbits, largely as a result of the overall shape and magnitude of the geomagnetic field (1-4). As a result, ISS exposure to many environmental factors can vary dramatically along a particular orbital ground track, and from one ground track to the next, during any 24-hour period.

Applications of Fermi-Lowdin-Orbital Self-Interaction Correction Scheme to Organic Systems

NASA Astrophysics Data System (ADS)

Baruah, Tunna; Kao, Der-You; Yamamoto, Yoh

Recent progress in treating the self-interaction errors by means of local, Lowdin-orthogonalized Fermi Orbitals offers a promising route to study the effect of self-interaction errors in the electronic structure of molecules. The Fermi orbitals depend on the location of the electronic positions, called as Fermi orbital descriptors. One advantage of using the Fermi orbitals is that the corrected Hamiltonian is unitarily invariant. Minimization of the corrected energies leads to an optimized set of centroid positions. Here we discuss the applications of this method to various systems from constituent atoms to several medium size molecules such as Mg-porphyrin, C60, pentacene etc. The applications to the ionic systems will also be discussed. De-SC0002168, NSF-DMR 125302.

Mission Plan for the Mars Surveyor 2001 Orbiter and Lander

NASA Technical Reports Server (NTRS)

Plaut, J. J.; Spencer, D. A.

1999-01-01

The Mars Surveyor 2001 Project consists of two missions to Mars, an Orbiter and a Lander, both to be launched in the spring of 2001 for October 2001 (Orbiter) and January 2002 (Lander) arrival at Mars. The Orbiter will support the Lander mission primarily as a communications relay system; the Lander will not have direct-to-Earth communications capability. Science data collected from the Orbiter will also be used to aid in the geologic interpretation of the landing site, along with data from past missions. Combining the Orbiter and Lander missions into a single Project has enabled the streamlining of many activities and an efficient use of personnel and other resources at the Jet Propulsion Laboratory and at the spacecraft contractor, Lockheed Martin Astronautics.

LADEE UVS Observations of Atoms and Dust in the Lunar Tail

NASA Technical Reports Server (NTRS)

Wooden, Diane H.; Colaprete, Anthony; Cook, Amanda M.; Shirley, Mark H.; Vargo, Kara E.; Elphic, Richard C.; Stubbs, Timothy J.; Glenar, David A.

2014-01-01

The Lunar Atmosphere and Dust Environment Explorer (LADEE) was a lunar orbiter launched in September 2013 that investigated the composition and temporal variation of the tenuous lunar exosphere and dust environment. A major goal of the mission was to characterize the dust exosphere prior to future lunar exploration activities, which may alter the lunar environment. The Ultraviolet/Visible Spectrometer (UVS) onboard LADEE addresses this goal, utilizing two sets of optics: a limbviewing telescope, and a solar-viewing telescope. We report on spectroscopic (approximately 280 - 820 nm) observations viewing down the lunar wake or along the 'lunar tail' from lunar orbit. Prior groundbased studies have observed the emission from neutral sodium atoms extended along the lunar tail, so often this region is referred to as the lunar sodium tail. UVS measurements were made on the dark side of the moon, with the UVS limb-viewing telescope pointed outward in the direction of the Moon's wake (almost anti-sun), during different lunar phases. These UVS observation activities sample a long column and allow the characterization of scattered light from dust and emission lines from atoms in the lunar tail. Observations in this UVS configuration show the largest excess of scattered blue light in our data set, indicative of the presence of small dust grains in the tail. Once lofted, nanoparticles may become charged and picked up by the solar wind, similar to the phenomena witnessed above Enceladus's northern hemisphere or by the STEREO/WAVES instrument while close to Earth's orbit. The UVS data show that small dust grains as well as atoms become entrained in the lunar tail.

Interactions of C+(2PJ) with rare gas atoms: incipient chemical interactions, potentials and transport coefficients

NASA Astrophysics Data System (ADS)

Tuttle, William D.; Thorington, Rebecca L.; Viehland, Larry A.; Breckenridge, W. H.; Wright, Timothy G.

2018-03-01

Accurate interatomic potentials were calculated for the interaction of a singly charged carbon cation, C+, with a single rare gas atom, RG (RG = Ne-Xe). The RCCSD(T) method and basis sets of quadruple-ζ and quintuple-ζ quality were employed; each interaction energy was counterpoise corrected and extrapolated to the basis set limit. The lowest C+(2P) electronic term of the carbon cation was considered, and the interatomic potentials calculated for the diatomic terms that arise from these: 2Π and 2Σ+. Additionally, the interatomic potentials for the respective spin-orbit levels were calculated, and the effect on the spectroscopic parameters was examined. In doing this, anomalously large spin-orbit splittings for RG = Ar-Xe were found, and this was investigated using multi-reference configuration interaction calculations. The latter indicated a small amount of RG → C+ electron transfer and this was used to rationalize the observations. This is taken as evidence of an incipient chemical interaction, which was also examined via contour plots, Birge-Sponer plots and various population analyses across the C+-RG series (RG = He-Xe), with the latter showing unexpected results. Trends in several spectroscopic parameters were examined as a function of the increasing atomic number of the RG atom. Finally, each set of RCCSD(T) potentials was employed, including spin-orbit coupling to calculate the transport coefficients for C+ in RG, and the results were compared with the limited available data. This article is part of the theme issue `Modern theoretical chemistry'.

Spin texture induced by oxygen vacancies in strontium perovskite (001) surfaces: A theoretical comparison between SrTiO3 and SrHfO3

NASA Astrophysics Data System (ADS)

Garcia-Castro, A. C.; Vergniory, M. G.; Bousquet, E.; Romero, A. H.

2016-01-01

The electronic structure of SrTiO3 and SrHfO3 (001) surfaces with oxygen vacancies is studied by means of first-principles calculations. We reveal how oxygen vacancies within the first atomic layer of the SrTiO3 surface (i) induce a large antiferrodistortive motion of the oxygen octahedra at the surface, (ii) drive localized magnetic moments on the Ti 3 d orbitals close to the vacancies, and (iii) form a two-dimensional electron gas localized within the first layers. The analysis of the spin texture of this system exhibits a splitting of the energy bands according to the Zeeman interaction, lowering of the Ti 3 dx y level in comparison with dx z and dy z, and also an in-plane precession of the spins. No Rashba-like splitting for the ground state or for the ab initio molecular dynamics trajectory at 400 K is recognized as suggested recently by A. F. Santander-Syro et al. [Nat. Mater. 13, 1085 (2014), 10.1038/nmat4107]. Instead, a sizable Rashba-like splitting is observed when the Ti atom is replaced by a heavier Hf atom with a much larger spin-orbit interaction. However, we observe the disappearance of the magnetism and the surface two-dimensional electron gas when full structural optimization of the SrHfO3 surface is performed. Our results uncover the sensitive interplay of spin-orbit coupling, atomic relaxations, and magnetism when tuning these Sr-based perovskites.

A measurement of the angular distribution of 5 eV atomic oxygen scattered off a solid surface in earth orbit

NASA Technical Reports Server (NTRS)

Gregory, John C.; Peters, Palmer N.

1986-01-01

The angular distribution of 5 eV atomic oxygen scattered off a polished vitreous carbon surface was measured on a recent Space Shuttle flight. The experimental apparatus was of novel design, completely passive, and used thin silver films as the recording device for oxygen atoms. Most of the incident oxygen was contained in the reflected beam and remained in an active form and probably still atoms. Allowance was made for 12 percent loss of incident atoms which are converted to CO at the carbon surface. The scattered distribution which is wide lobular, peaking 15 deg in the forward direction, shows almost but not quite full accommodation.

Alignment relaxation of Ne*(2pi [J = 1]) atoms in He-Ne* glow discharges

NASA Astrophysics Data System (ADS)

Bahrim, Cristian; Khadilkar, Vaibhav; Matsukuma, Hiraku; Hasuo, Masahiro

2009-11-01

Alignment relaxation of the Ne*(2p5 3p; 2pi [J = 1]) atoms (where i = 2, 5, 7 or 10) induced by collisions with He atoms in glow discharges at 77 K < T < 1,000 K are reported. Close-coupling many-channel quantum calculations using a model potential for the Ne*(2p5 3p) - He system are compared with measurements of the alignment relaxation using the LIFS technique and the Hanle effect. The addition of the dipole polarization potential of the Ne*(2pi [J = 1]) atoms to the spin-orbit coupling and the electrostatic interaction between Ne* and He atoms leads to good agreement between theory and experiment.

Exact solution for the hydrogen atom confined by a dielectric continuum and the correct basis set to study many-electron atoms under similar confinements

NASA Astrophysics Data System (ADS)

Martínez-Sánchez, Michael-Adán; Aquino, Norberto; Vargas, Rubicelia; Garza, Jorge

2017-12-01

The Schrödinger equation associated to the hydrogen atom confined by a dielectric continuum is solved exactly and suggests the appropriate basis set to be used when an atom is immersed in a dielectric continuum. Exact results show that this kind of confinement spread the electron density, which is confirmed through the Shannon entropy. The basis set suggested by the exact results is similar to Slater type orbitals and it was applied on two-electron atoms, where the H- ion ejects one electron for moderate confinements for distances much larger than those commonly used to generate cavities in solvent models.

Creation of half-metallic f -orbital Dirac fermion with superlight elements in orbital-designed molecular lattice

NASA Astrophysics Data System (ADS)

Cui, Bin; Huang, Bing; Li, Chong; Zhang, Xiaoming; Jin, Kyung-Hwan; Zhang, Lizhi; Jiang, Wei; Liu, Desheng; Liu, Feng

2017-08-01

Magnetism in solids generally originates from the localized d or f orbitals that are hosted by heavy transition-metal elements. Here, we demonstrate a mechanism for designing a half-metallic f -orbital Dirac fermion from superlight s p elements. Combining first-principles and model calculations, we show that bare and flat-band-sandwiched (FBS) Dirac bands can be created when C20 molecules are deposited into a two-dimensional hexagonal lattice, which are composed of f -molecular orbitals (MOs) derived from s p -atomic orbitals (AOs). Furthermore, charge doping of the FBS Dirac bands induces spontaneous spin polarization, converting the system into a half-metallic Dirac state. Based on this discovery, a model of a spin field effect transistor is proposed to generate and transport 100% spin-polarized carriers. Our finding illustrates a concept to realize exotic quantum states by manipulating MOs, instead of AOs, in orbital-designed molecular crystal lattices.

Evaluation of thermal control coatings for use on solar dynamic radiators in low earth orbit

NASA Technical Reports Server (NTRS)

Dever, Joyce A.; Rodriguez, Elvin; Slemp, Wayne S.; Stoyack, Joseph E.

1991-01-01

Thermal control coatings with high thermal emittance and low solar absorptance are needed for Space Station Freedom (SSF) solar dynamic power module radiator (SDR) surfaces for efficient heat rejection. Additionally, these coatings must be durable to low earth orbital (LEO) environmental effects of atomic oxygen, ultraviolet radiation and deep thermal cycles which occur as a result of start-up and shut-down of the solar dynamic power system. Eleven candidate coatings were characterized for their solar absorptance and emittance before and after exposure to ultraviolet (UV) radiation (200 to 400 nm), vacuum UV (VUV) radiation (100 to 200 nm) and atomic oxygen. Results indicated that the most durable and best performing coatings were white paint thermal control coatings Z-93, zinc oxide pigment in potassium silicate binder, and YB-71, zinc orthotitanate pigment in potassium silicate binder. Optical micrographs of these materials exposed to the individual environmental effects of atomic oxygen and vacuum thermal cycling showed that no surface cracking occurred.

Undercutting of defects in thin film protective coatings on polymer surfaces exposed to atomic oxygen

NASA Technical Reports Server (NTRS)

Rutledge, Sharon K.; Mihelcic, Judith A.

1989-01-01

Protection for polymeric surfaces is needed to make them durable in the low Earth orbital environment, where oxidation by atomic oxygen is the predominant failure mechanism. Thin film coatings of oxides such as silicon dioxide are viable candidates to provide this protection, but concern has been voiced over the ability of these coatings to protect when defects are present in the coating due to surface anomalies occurring during the deposition process, handling, or micrometeoroid and debris bombardment in low Earth orbit. When a defected coating protecting a polymer substrate is exposed to atomic oxygen, the defect provides a pathway to the underlying polymer allowing oxidation and subsequent undercutting to occur. Defect undercutting was studied for sputter deposited coatings of silicon dioxide on polyimide Kapton. Preliminary results indicate that undercutting may be limited as long as the coating remains intact with the substrate. Therefore, coatings may not need to be defect free to give protection to the underlying surface.

Atomic oxygen erosion considerations for spacecraft materials selection

NASA Technical Reports Server (NTRS)

Whitaker, Ann F.; Kamenetzky, Rachel R.

1993-01-01

The Long Duration Exposure Facility (LDEF) satellite carried 57 experiments that were designed to define the low-Earth orbit (LEO) space environment and to evaluate the impact of this environment on potential engineering materials and material processes. Deployed by the Shuttle Challenger in April of 1984, LDEF made over 32,000 orbits before being retrieved nearly 6 years later by the Shuttle Columbia in January of 1990. The Solar Array Passive LDEF Experiment (SAMPLE) AO171 contained approximately 300 specimens, representing numerous material classes and material processes. AO171 was located on LDEF in position A8 at a yaw of 38.1 degrees from the ram direction and was subjected to an atomic oxygen (AO) fluence of 6.93 x 10(exp 21) atoms/sq cm. LDEF AO171 data, as well as short-term shuttle data, will be discussed in this paper as it applies to engineering design applications of composites, bulk and thin film polymers, glassy ceramics, thermal control paints, and metals subjected to AO erosion.

Structure of alkali tellurite glasses from neutron diffraction and molecular orbital calculations

NASA Astrophysics Data System (ADS)

Niida, Haruki; Uchino, Takashi; Jin, Jisun; Kim, Sae-Hoon; Fukunaga, Toshiharu; Yoko, Toshinobu

2001-01-01

The structure of pure TeO2 and alkali tellurite glasses has been examined by neutron diffraction and ab initio molecular orbital methods. The experimental radial distribution functions along with the calculated results have demonstrated that the basic structural units in tellurite glasses change from highly strained TeO4 trigonal bipyramids to more regular TeO3 trigonal pyramids with increasing alkali content. It has also been shown that the TeO3 trigonal pyramids do not exist in the form of isolated units in the glass network but interact with each other to form intertrigonal Te⋯O linkages. The present results suggest that nonbridging oxygen (NBO) atoms in tellurite glasses do not exist in their "pure" form; that is, all the NBO atoms in TeO3 trigonal bipyramids will interact with the first- and/or second-neighbor Te atoms, resulting in the three-dimensional continuous random network even in tellurite glasses with over 30 mol % of alkali oxides.

Linear combination of atomic orbitals calculation of the Auger neutralization rate of He{sup +} on Al(111) (100), and (110) surfaces

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

Valdes, Diego; Blanco, J.M.; Monreal, R.C.

2005-06-15

We develop a theory of the Auger neutralization rate of ions on solid surfaces in which the matrix elements for the transition are calculated by means of a linear combination of atomic orbitals technique. We apply the theory to the calculation of the Auger rate of He{sup +} on unreconstructed Al(111) (100), and (110) surfaces, assuming He{sup +} to approach these surfaces on high symmetry positions and compare them with the results of the jellium model. Although there are substantial differences between the Auger rates calculated with both kinds of approaches, those differences tend to compensate when evaluating the integralmore » along the ion trajectory and, consequently, are of minor influence in some physical magnitudes like the ion survival probability for perpendicular energies larger than 100 eV. We find that many atoms contribute to the Auger process and small effects of lateral corrugation are registered.« less

Density-functional expansion methods: Grand challenges.

PubMed

Giese, Timothy J; York, Darrin M

2012-03-01

We discuss the source of errors in semiempirical density functional expansion (VE) methods. In particular, we show that VE methods are capable of well-reproducing their standard Kohn-Sham density functional method counterparts, but suffer from large errors upon using one or more of these approximations: the limited size of the atomic orbital basis, the Slater monopole auxiliary basis description of the response density, and the one- and two-body treatment of the core-Hamiltonian matrix elements. In the process of discussing these approximations and highlighting their symptoms, we introduce a new model that supplements the second-order density-functional tight-binding model with a self-consistent charge-dependent chemical potential equalization correction; we review our recently reported method for generalizing the auxiliary basis description of the atomic orbital response density; and we decompose the first-order potential into a summation of additive atomic components and many-body corrections, and from this examination, we provide new insights and preliminary results that motivate and inspire new approximate treatments of the core-Hamiltonian.

Leveling coatings for reducing the atomic oxygen defect density in protected graphite fiber epoxy composites

NASA Astrophysics Data System (ADS)

Jaworske, D. A.; Degroh, Kim K.; Podojil, G.; McCollum, T.; Anzic, J.

1992-11-01

Pinholes or other defect sites in a protective oxide coating provide pathways for atomic oxygen in low Earth orbit to reach underlying material. One concept of enhancing the lifetime of materials in low Earth orbit is to apply a leveling coating to the material prior to applying any reflective and protective coatings. Using a surface tension leveling coating concept, a low viscosity epoxy was applied to the surface of several composite coupons. A protective layer of 1000 A of SiO2 was deposited on top of the leveling coating, and the coupons were exposed to an atomic oxygen environment in a plasma asher. Pinhole populations per unit area were estimated by counting the number of undercut sites observed by scanning electron microscopy. Defect density values of 180,000 defects/sq cm were reduced to about 1000 defects/sq cm as a result of the applied leveling coating. These improvements occur at a mass penalty of about 2.5 mg/sq cm.

Leveling coatings for reducing the atomic oxygen defect density in protected graphite fiber epoxy composites

NASA Technical Reports Server (NTRS)

Jaworske, D. A.; Degroh, K. K.; Podojil, G.; Mccollum, T.; Anzic, J.

1992-01-01

Pinholes or other defect sites in a protective oxide coating provide pathways for atomic oxygen in low Earth orbit to reach underlying material. One concept for enhancing the lifetime of materials in low Earth orbits is to apply a leveling coating to the material prior to applying any reflective and protective coatings. Using a surface tension leveling coating concept, a low viscosity epoxy was applied to the surface of several composite coupons. A protective layer of 1000 A of SiO2 was deposited on top of the leveling coating, and the coupons were exposed to an atomic oxygen environment in a plasma asher. Pinhole populations per unit area were estimated by counting the number of undercut sites observed by scanning electron microscopy. Defect density values of 180,000 defects/sq cm were reduced to about 1000 defects/sq cm as a result of the applied leveling coating. These improvements occur at a mass penalty of about 2.5 mg/sq cm.

Leveling coatings for reducing the atomic oxygen defect density in protected graphite fiber epoxy composites

NASA Technical Reports Server (NTRS)

Jaworske, D. A.; Degroh, Kim K.; Podojil, G.; Mccollum, T.; Anzic, J.

1992-01-01

Pinholes or other defect sites in a protective oxide coating provide pathways for atomic oxygen in low Earth orbit to reach underlying material. One concept of enhancing the lifetime of materials in low Earth orbit is to apply a leveling coating to the material prior to applying any reflective and protective coatings. Using a surface tension leveling coating concept, a low viscosity epoxy was applied to the surface of several composite coupons. A protective layer of 1000 A of SiO2 was deposited on top of the leveling coating, and the coupons were exposed to an atomic oxygen environment in a plasma asher. Pinhole populations per unit area were estimated by counting the number of undercut sites observed by scanning electron microscopy. Defect density values of 180,000 defects/sq cm were reduced to about 1000 defects/sq cm as a result of the applied leveling coating. These improvements occur at a mass penalty of about 2.5 mg/sq cm.

Emergence of Huge Negative Spin-Transfer Torque in Atomically Thin Co layers

NASA Astrophysics Data System (ADS)

Je, Soong-Geun; Yoo, Sang-Cheol; Kim, Joo-Sung; Park, Yong-Keun; Park, Min-Ho; Moon, Joon; Min, Byoung-Chul; Choe, Sug-Bong

2017-04-01

Current-induced domain wall motion has drawn great attention in recent decades as the key operational principle of emerging magnetic memory devices. As the major driving force of the motion, the spin-orbit torque on chiral domain walls has been proposed and is currently extensively studied. However, we demonstrate here that there exists another driving force, which is larger than the spin-orbit torque in atomically thin Co films. Moreover, the direction of the present force is found to be the opposite of the prediction of the standard spin-transfer torque, resulting in the domain wall motion along the current direction. The symmetry of the force and its peculiar dependence on the domain wall structure suggest that the present force is, most likely, attributed to considerable enhancement of a negative nonadiabatic spin-transfer torque in ultranarrow domain walls. Careful measurements of the giant magnetoresistance manifest a negative spin polarization in the atomically thin Co films which might be responsible for the negative spin-transfer torque.

Evaluation of thermal control coatings for use on solar dynamic radiators in low Earth orbit

NASA Technical Reports Server (NTRS)

Dever, Joyce A.; Rodriguez, Elvin; Slemp, Wayne S.; Stoyack, Joseph E.

1991-01-01

Thermal control coatings with high thermal emittance and low solar absorptance are needed for Space Station Freedom (SSF) solar dynamic power module radiator (SDR) surfaces for efficient heat rejection. Additionally, these coatings must be durable to low earth orbital (LEO) environmental effects of atomic oxygen, ultraviolet radiation and deep thermal cycles which occur as a result of start-up and shut-down of the solar dynamic power system. Eleven candidate coatings were characterized for their solar absorptance and emittance before and after exposure to ultraviolet (UV) radiation (200 to 400 nm), vacuum UV (VUV) radiation (100 to 200 nm) and atomic oxygen. Results indicated that the most durable and best performing coatings were white paint thermal control coatings Z-93, zinc oxide pigment in potassium silicate binder, and YB-71, zinc orthotitanate pigment in potassium silicate binder. Optical micrographs of these materials exposed to the individual environmental effects of atomic oxygen and vacuum thermal cycling showed that no surface cracking occurred.

Interaction of benzene thiol and thiolate with small gold clusters.

PubMed

Letardi, Sara; Cleri, Fabrizio

2004-06-01

We studied the interaction between benzene thiol and thiolate molecules, and gold clusters made of 1 to 3 atoms, by means of ab initio density functional theory in the local density approximation. We find that the thiolate is energetically more stable than the thiol, however the process of detachment of H from the thiol appears to be possibly mediated by the intermediate step of H chemisorption on Au. Cleavage of the S-H bond is accompanied by a 90 degrees rotation of the molecule around the S-Au bond, showing a strong steric specificity. Such a rotation is induced by the relative energy shift of the S atom p orbitals with respect to the benzene pi ring and the Au d orbitals. By analyzing the correlation of the bond energy, bond lengths, and HOMO-LUMO gap with the number of S-Au bonds, we find that the thiolate S atom appears to prefer a low-coordination condition on Au clusters. (c) 2004 American Institute of Physics.

MIDAS: Lessons learned from the first spaceborne atomic force microscope

NASA Astrophysics Data System (ADS)

Bentley, Mark Stephen; Arends, Herman; Butler, Bart; Gavira, Jose; Jeszenszky, Harald; Mannel, Thurid; Romstedt, Jens; Schmied, Roland; Torkar, Klaus

2016-08-01

The Micro-Imaging Dust Analysis System (MIDAS) atomic force microscope (AFM) onboard the Rosetta orbiter was the first such instrument launched into space in 2004. Designed only a few years after the technique was invented, MIDAS is currently orbiting comet 67P Churyumov-Gerasimenko and producing the highest resolution 3D images of cometary dust ever made in situ. After more than a year of continuous operation much experience has been gained with this novel instrument. Coupled with operations of the Flight Spare and advances in terrestrial AFM a set of "lessons learned" has been produced, cumulating in recommendations for future spaceborne atomic force microscopes. The majority of the design could be reused as-is, or with incremental upgrades to include more modern components (e.g. the processor). Key additional recommendations are to incorporate an optical microscope to aid the search for particles and image registration, to include a variety of cantilevers (with different spring constants) and a variety of tip geometries.

The survivability of large space-borne reflectors under atomic oxygen and micrometeoroid impact

NASA Technical Reports Server (NTRS)

Gulino, D. A.

1987-01-01

Solar dynamic power system mirrors for use on space station and other spacecraft flown in low Earth orbit (LEO) are exposed to the harshness of the LEO environment. Both atomic oxygen and micrometeoroids/space debris can degrade the performance of such mirrors. Protective coatings will be required to protect oxidizable reflecting media, such as silver and aluminum, from atomic oxygen attack. Several protective coating materials have been identified as good candidates for use in this application. The durability of these coating/mirror systems after pinhole defects have been inflicted during their fabrication and deployment or through micrometeoroid/space debris impact once on-orbit is of concern. Studies of the effect of an oxygen plasma environment on protected mirror surfaces with intentionally induced pinhole defects have been conducted at NASA Lewis and are reviewed. It has been found that oxidation of the reflective layer and/or the substrate in areas adjacent to a pinhole defect, but not directly exposed by the pinhole, can occur.

Environmental Durability Issues for Solar Power Systems in Low Earth Orbit

NASA Technical Reports Server (NTRS)

Degroh, Kim K.; Banks, Bruce A.; Smith, Daniela C.

1994-01-01

Space solar power systems for use in the low Earth orbit (LEO) environment experience a variety of harsh environmental conditions. Materials used for solar power generation in LEO need to be durable to environmental threats such as atomic oxygen, ultraviolet (UV) radiation, thermal cycling, and micrometeoroid and debris impact. Another threat to LEO solar power performance is due to contamination from other spacecraft components. This paper gives an overview of these LEO environmental issues as they relate to space solar power system materials. Issues addressed include atomic oxygen erosion of organic materials, atomic oxygen undercutting of protective coatings, UV darkening of ceramics, UV embrittlement of Teflon, effects of thermal cycling on organic composites, and contamination due to silicone and organic materials. Specific examples of samples from the Long Duration Exposure Facility (LDEF) and materials returned from the first servicing mission of the Hubble Space Telescope (HST) are presented. Issues concerning ground laboratory facilities which simulate the LEO environment are discussed along with ground-to-space correlation issues.

Quantum chemical study of relative reactivities of a series of amines and nitriles - Relevance to prebiotic chemistry

NASA Technical Reports Server (NTRS)

Loew, G. H.; Berkowitz, D.; Chang, S.

1975-01-01

Using the Iterative Extended Huckel Theory (IEHT) calculations of the electron distribution and orbital energies of a series of thirteen amines, nitriles and amino-nitriles relevant to prebiotic and cosmo-chemistry have been carried out. Ground state properties such as the energy and nature of the highest occupied (HOMO) and lowest empty (LEMO) molecular orbitals, net atomic charges and number of nonbonding electrons have been identified as criteria for correlating the relative nucleophilicity of amine and nitrile nitrogens and the electrophilicity of nitrile and other unsaturated carbon atoms. The results of such correlations can be partially verified by known chemical behavior of these compounds and are used to predict and understand their role in prebiotic organic synthesis.

Velocity-gauge real-time TDDFT within a numerical atomic orbital basis set

NASA Astrophysics Data System (ADS)

Pemmaraju, C. D.; Vila, F. D.; Kas, J. J.; Sato, S. A.; Rehr, J. J.; Yabana, K.; Prendergast, David

2018-05-01

The interaction of laser fields with solid-state systems can be modeled efficiently within the velocity-gauge formalism of real-time time dependent density functional theory (RT-TDDFT). In this article, we discuss the implementation of the velocity-gauge RT-TDDFT equations for electron dynamics within a linear combination of atomic orbitals (LCAO) basis set framework. Numerical results obtained from our LCAO implementation, for the electronic response of periodic systems to both weak and intense laser fields, are compared to those obtained from established real-space grid and Full-Potential Linearized Augmented Planewave approaches. Potential applications of the LCAO based scheme in the context of extreme ultra-violet and soft X-ray spectroscopies involving core-electronic excitations are discussed.

Bond Dissociation Energies of the Tungsten Fluorides and Their Singly-Charged Ions: A Density Functional Survey

NASA Technical Reports Server (NTRS)

Dyall, Kenneth G.; Arnold, James (Technical Monitor)

1999-01-01

The dissociation of WF6 and the related singly-charged cations and anions into the lower fluorides and fluorine atoms has been investigated theoretically using density functional theory (B3LYP) and relativistic effective core potentials, with estimates of spin-orbit effects included using a simple model. The inclusion of spin-orbit is essential for a correct description of the thermochemistry. The total atomization energy of the neutral and anionic WF6 is reproduced to within 25 kcal/mol, but comparison of individual bond dissociation energies with available experimental data shows discrepancies of up to 10 kcal/mol. The results are nevertheless useful to help resolve discrepancies in experimental data and provide estimates of missing data.

Whisker/Cone growth on the thermal control surfaces experiment no. S0069

NASA Technical Reports Server (NTRS)

Zwiener, James M.; Coston, James E., Jr.; Miller, Edgar R.; Mell, Richard J.; Wilkes, Donald R.

1995-01-01

An unusual surface 'growth' was found during scanning electron microscope (SEM) investigations of the Thermal Control Surface Experiment (TCSE) S0069 front thermal cover. This 'growth' is similar to the cone type whisker growth phenomena as studied by G. K. Wehner beginning in the 1960's. Extensive analysis has identified the most probable composition of the whiskers to be a silicate type glass. Sources of the growth material are outgassing products from the experiment and orbital atomic oxygen, which occurs naturally at the orbital altitudes of the LDEF mission in the form of neutral atomic oxygen. The highly ordered symmetry and directionality of the whiskers are attributed to the long term (5.8 year) stable flight orientation of the LDEF.

Li n @B36 ( n = 1, 2) Nanosheet with Remarkable Electro-Optical Properties: A DFT Study

NASA Astrophysics Data System (ADS)

Solimannejad, Mohammad; Kamalinahad, Saeedeh; Shakerzadeh, Ehsan

2017-07-01

In this study, an attempt has been made to investigate alteration in electro-optical properties of bowl-shape B36 nanosheet due to interaction with one and two Li atoms. Our results reveal that the highest occupied molecular orbital-lowest unoccupied molecular orbital (HOMO-LUMO) gap of B36 nanosheet is decreased because of a high energy level which is formed under influence of interactions with Li atoms. Gigantic enhancement in the first hyperpolarizability ( β 0) of the studied nanosheet up to 4920.62 au is indicated owing to the effect of Li adsorption. The result of the present study may be eventuating to design and fabrication of a nanosheet with tunable electro-optical properties.

DFT studies on H 2O adsorption and its effect on CO oxidation over spinel Co 3O 4 (110) surface

NASA Astrophysics Data System (ADS)

Xu, Xiang Lan; Li, Jun Qian

2011-12-01

Adsorption of H2O and its effect on CO oxidation over spinel Co3O4 (110) surface were studied by density functional theory calculations. H2O is adsorbed favorably at the octahedral cobalt (Cooct) site through O atom on the surface. Hydrogen bonding interaction between 1s orbitals of H atoms in H2O and the 2p orbitals of surface active oxygen sites plays a key role for H2O adsorption. The inhibition effect of H2O adsorption on the CO oxidation over the surfaces is attributed to the competition between H2O and CO molecules for the surface twofold coordinated oxygen site.

Tunable spin-orbit coupling for ultracold atoms in two-dimensional optical lattices

NASA Astrophysics Data System (ADS)

Grusdt, Fabian; Li, Tracy; Bloch, Immanuel; Demler, Eugene

2017-06-01

Spin-orbit coupling (SOC) is at the heart of many exotic band structures and can give rise to many-body states with topological order. Here we present a general scheme based on a combination of microwave driving and lattice shaking for the realization of two-dimensional SOC with ultracold atoms in systems with inversion symmetry. We show that the strengths of Rashba and Dresselhaus SOC can be independently tuned in a spin-dependent square lattice. More generally, our method can be used to open gaps between different spin states without breaking time-reversal symmetry. We demonstrate that this allows for the realization of topological insulators with nontrivial spin textures closely related to the Kane-Mele model.

New Display-type Analyzer for Three-dimensional Fermi Surface Mapping and Atomic Orbital Analysis

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

Takahashi, Nobuaki; Matsuda, Hiroyuki; Shigenai, Shin

2007-01-19

We have developed and installed a new Display-type ANAlyzer (DIANA) at Ritsumeikan SR center BL-7. We measured the angle-integrated energy distribution curve of poly-crystal gold and the photoelectron intensity angular distribution (PIAD) of HOPG to estimate the total energy resolution and to check the condition of the analyzer. The total energy resolution ({delta}E/E) is up to 0.78%, which is much higher than the old type. The PIAD of HOPG we obtained was the ring pattern as expected. Therefore, a detailed three-dimensional Fermi surface mapping and an analysis of the atomic orbitals constituting the electron energy bands are possible by combiningmore » them with a linearly polarized synchrotron radiation.« less

First-principle study of geometric stabilities, electronic and magnetic properties of low coverage vanadium adsorption on graphene

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

Abdullahi, Yusuf Zuntu; Rahman, Md. Mahmudur, E-mail: mahmudur@upm.edu.my; Zainuddin, H.

2014-03-05

Stable geometries, electronic and magnetic properties of low coverage vanadium (V) atoms adsorption on graphene sheet have been investigated by first principles calculations, using generalized gradient approximation. Calculation shows that center of the ring is energetically favorable for both V adatom and perpendicular dimer after relaxation. Moreover, the proportion of orbital contribution of C-V bonding are mainly dominated by 2p{sub z} orbital of C and partially occupied by the 3d like states of V. It is also found that the low coverage V atom adsorbed graphene system is metallic and magnetic, and has demonstrated additional hint on its usefulness inmore » magnetic devices.« less

A highly sensitive chemical gas detecting device based on N-doped ZnO as a modified nanostructure media: A DFT+NBO analysis

NASA Astrophysics Data System (ADS)

Abbasi, Amirali; Sardroodi, Jaber Jahanbin

2018-02-01

We presented a density functional theory study of the adsorption of O3 and NO2 molecules on ZnO nanoparticles. Various adsorption geometries of O3 and NO2 over the nanoparticles were considered. For both O3 and NO2 adsorption systems, it was found that the adsorption on the N-doped nanoparticle is more favorable in energy than that on the pristine one. Therefore, the N-doped ZnO has a better efficiency to be utilized as O3 and NO2 detection device. For all cases, the binding sites were located on the zinc atoms of the nanoparticle. The charge analysis based on natural bond orbital (NBO) analysis indicates that charge was transferred from the surface to the adsorbed molecule. The projected density of states of the interacting atoms represent the formation of chemical bonds at the interface region. Molecular orbitals of the adsorption systems indicate that the HOMOs were mainly localized on the adsorbed O3 and NO2 molecules, whereas the electronic densities in the LUMOs were dominant at the ZnO nanocrystal surface. By examining the distribution of spin densities, we found that the magnetization was mainly located over the adsorbed molecules. For NO2 adsorbate, we found that the symmetric and asymmetric stretches were shifted to a lower frequency. The bending stretch mode was shifted to the higher frequency. Our DFT results thus provide a theoretical basis for why the adsorption of O3 and NO2 molecules on the N-doped ZnO nanoparticles may increase, giving rise to design and development of innovative and highly efficient sensor devices for O3 and NO2 recognition.

Molecular Line Lists for Scandium and Titanium Hydride Using the DUO Program

NASA Astrophysics Data System (ADS)

Lodi, Lorenzo; Yurchenko, Sergei N.; Tennyson, Jonathan

2015-06-01

Transition-metal-containing (TMC) molecules often have very complex electronic spectra because of their large number of low-lying, interacting electronic states, of the large multi-reference character of the electronic states and of the large magnitude of spin-orbit and relativistic effects. As a result, fully ab initio calculations of line positions and intensities of TMC molecules have an accuracy which is considerably worse than the one usually achievable for molecules made up by main-group atoms only. In this presentation we report on new theoretical line lists for scandium hydride ScH and titanium hydride TiH. Scandium and titanium are the lightest transition metal atoms and by virtue of their small number of valence electrons are amenable to high-level electronic-structure treatments and serve as ideal benchmark systems. We report for both systems energy curves, dipole curves and various coupling curves (including spin-orbit) characterising their electronic spectra up to about 20 000 cm-1. Curves were obtained using Internally-Contracted Multi Reference Configuration Interaction (IC-MRCI) as implemented in the quantum chemistry package MOLPRO. The curves where used for the solution of the coupled-surface ro-vibronic problem using the in-house program DUO. DUO is a newly-developed, general program for the spectroscopy of diatomic molecules and its main functionality will be described. The resulting line lists for ScH and TiH are made available as part of the Exomol project. L. Lodi, S. N. Yurchenko and J. Tennyson, Mol. Phys. (Handy special issue) in press. S. N. Yurchenko, L. Lodi, J. Tennyson and A. V. Stolyarov, Computer Phys. Comms., to be submitted.

STABLE CONIC-HELICAL ORBITS OF PLANETS AROUND BINARY STARS: ANALYTICAL RESULTS

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

Oks, E.

2015-05-10

Studies of planets in binary star systems are especially important because it was estimated that about half of binary stars are capable of supporting habitable terrestrial planets within stable orbital ranges. One-planet binary star systems (OBSS) have a limited analogy to objects studied in atomic/molecular physics: one-electron Rydberg quasimolecules (ORQ). Specifically, ORQ, consisting of two fully stripped ions of the nuclear charges Z and Z′ plus one highly excited electron, are encountered in various plasmas containing more than one kind of ion. Classical analytical studies of ORQ resulted in the discovery of classical stable electronic orbits with the shape ofmore » a helix on the surface of a cone. In the present paper we show that despite several important distinctions between OBSS and ORQ, it is possible for OBSS to have stable planetary orbits in the shape of a helix on a conical surface, whose axis of symmetry coincides with the interstellar axis; the stability is not affected by the rotation of the stars. Further, we demonstrate that the eccentricity of the stars’ orbits does not affect the stability of the helical planetary motion if the center of symmetry of the helix is relatively close to the star of the larger mass. We also show that if the center of symmetry of the conic-helical planetary orbit is relatively close to the star of the smaller mass, a sufficiently large eccentricity of stars’ orbits can switch the planetary motion to the unstable mode and the planet would escape the system. We demonstrate that such planets are transitable for the overwhelming majority of inclinations of plane of the stars’ orbits (i.e., the projections of the planet and the adjacent start on the plane of the sky coincide once in a while). This means that conic-helical planetary orbits at binary stars can be detected photometrically. We consider, as an example, Kepler-16 binary stars to provide illustrative numerical data on the possible parameters and the stability of the conic-helical planetary orbits, as well as on the transitability. Then for the general case, we also show that the power of the gravitational radiation due to this planet can be comparable or even exceed the power of the gravitational radiation due to the stars in the binary. This means that in the future, with a progress of gravitational wave detectors, the presence of a planet in a conic-helical orbit could be revealed by the noticeably enhanced gravitational radiation from the binary star system.« less

Analytical energy gradient for the two-component normalized elimination of the small component method

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

Zou, Wenli; Filatov, Michael; Cremer, Dieter, E-mail: dcremer@smu.edu

2015-06-07

The analytical gradient for the two-component Normalized Elimination of the Small Component (2c-NESC) method is presented. The 2c-NESC is a Dirac-exact method that employs the exact two-component one-electron Hamiltonian and thus leads to exact Dirac spin-orbit (SO) splittings for one-electron atoms. For many-electron atoms and molecules, the effect of the two-electron SO interaction is modeled by a screened nucleus potential using effective nuclear charges as proposed by Boettger [Phys. Rev. B 62, 7809 (2000)]. The effect of spin-orbit coupling (SOC) on molecular geometries is analyzed utilizing the properties of the frontier orbitals and calculated SO couplings. It is shown thatmore » bond lengths can either be lengthened or shortened under the impact of SOC where in the first case the influence of low lying excited states with occupied antibonding orbitals plays a role and in the second case the jj-coupling between occupied antibonding and unoccupied bonding orbitals dominates. In general, the effect of SOC on bond lengths is relatively small (≤5% of the scalar relativistic changes in the bond length). However, large effects are found for van der Waals complexes Hg{sub 2} and Cn{sub 2}, which are due to the admixture of more bonding character to the highest occupied spinors.« less

Wannier-function-based constrained DFT with nonorthogonality-correcting Pulay forces in application to the reorganization effects in graphene-adsorbed pentacene

NASA Astrophysics Data System (ADS)

Roychoudhury, Subhayan; O'Regan, David D.; Sanvito, Stefano

2018-05-01

Pulay terms arise in the Hellmann-Feynman forces in electronic-structure calculations when one employs a basis set made of localized orbitals that move with their host atoms. If the total energy of the system depends on a subspace population defined in terms of the localized orbitals across multiple atoms, then unconventional Pulay terms will emerge due to the variation of the orbital nonorthogonality with ionic translation. Here, we derive the required exact expressions for such terms, which cannot be eliminated by orbital orthonormalization. We have implemented these corrected ionic forces within the linear-scaling density functional theory (DFT) package onetep, and we have used constrained DFT to calculate the reorganization energy of a pentacene molecule adsorbed on a graphene flake. The calculations are performed by including ensemble DFT, corrections for periodic boundary conditions, and empirical Van der Waals interactions. For this system we find that tensorially invariant population analysis yields an adsorbate subspace population that is very close to integer-valued when based upon nonorthogonal Wannier functions, and also but less precisely so when using pseudoatomic functions. Thus, orbitals can provide a very effective population analysis for constrained DFT. Our calculations show that the reorganization energy of the adsorbed pentacene is typically lower than that of pentacene in the gas phase. We attribute this effect to steric hindrance.

Localizing gravitational wave sources with single-baseline atom interferometers

DOE PAGES

Graham, Peter W.; Jung, Sunghoon

2018-01-31

Localizing sources on the sky is crucial for realizing the full potential of gravitational waves for astronomy, astrophysics, and cosmology. Here in this paper, we show that the midfrequency band, roughly 0.03 to 10 Hz, has significant potential for angular localization. The angular location is measured through the changing Doppler shift as the detector orbits the Sun. This band maximizes the effect since these are the highest frequencies in which sources live for several months. Atom interferometer detectors can observe in the midfrequency band, and even with just a single baseline they can exploit this effect for sensitive angular localization.more » The single-baseline orbits around the Earth and the Sun, causing it to reorient and change position significantly during the lifetime of the source, and making it similar to having multiple baselines/detectors. For example, atomic detectors could predict the location of upcoming black hole or neutron star merger events with sufficient accuracy to allow optical and other electromagnetic telescopes to observe these events simultaneously. Thus, midband atomic detectors are complementary to other gravitational wave detectors and will help complete the observation of a broad range of the gravitational spectrum.« less

Localizing gravitational wave sources with single-baseline atom interferometers

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

Graham, Peter W.; Jung, Sunghoon

Localizing sources on the sky is crucial for realizing the full potential of gravitational waves for astronomy, astrophysics, and cosmology. Here in this paper, we show that the midfrequency band, roughly 0.03 to 10 Hz, has significant potential for angular localization. The angular location is measured through the changing Doppler shift as the detector orbits the Sun. This band maximizes the effect since these are the highest frequencies in which sources live for several months. Atom interferometer detectors can observe in the midfrequency band, and even with just a single baseline they can exploit this effect for sensitive angular localization.more » The single-baseline orbits around the Earth and the Sun, causing it to reorient and change position significantly during the lifetime of the source, and making it similar to having multiple baselines/detectors. For example, atomic detectors could predict the location of upcoming black hole or neutron star merger events with sufficient accuracy to allow optical and other electromagnetic telescopes to observe these events simultaneously. Thus, midband atomic detectors are complementary to other gravitational wave detectors and will help complete the observation of a broad range of the gravitational spectrum.« less

Charge transfer between O6+ and atomic hydrogen

NASA Astrophysics Data System (ADS)

Wu, Y.; Stancil, P. C.; Liebermann, H. P.; Buenker, R. J.; Schultz, D. R.; Hui, Y.

2011-05-01

The charge exchange process has been found to play a dominant role in the production of X-rays and/or EUV photons observed in cometary and planetary atmospheres and from the heliosphere. Charge transfer cross sections, especially state-selective cross sections, are necessary parameters in simulations of X-ray emission. In the present work, charge transfer due to collisions of ground state O6+(1s2 1 S) with atomic hydrogen has been investigated theoretically using the quantum-mechanical molecular-orbital close-coupling method (QMOCC). The multi-reference single- and double-excitation configuration interaction approach (MRDCI) has been applied to compute the adiabatic potential and nonadiabatic couplings, and the atomic basis sets used have been optimized with the method proposed previously to obtain precise potential data. Total and state-selective cross sections are calculated for energies between 10 meV/u and 10 keV/u. The QMOCC results are compared to available experimental and theoretical data as well as to new atomic-orbital close-coupling (AOCC) and classical trajectory Monte Carlo (CTMC) calculations. A recommended set of cross sections, based on the MOCC, AOCC, and CTMC calculations, is deduced which should aid in X-ray modeling studies.

Magnitude of finite-nucleus-size effects in relativistic density functional computations of indirect NMR nuclear spin-spin coupling constants.

PubMed

Autschbach, Jochen

2009-09-14

A spherical Gaussian nuclear charge distribution model has been implemented for spin-free (scalar) and two-component (spin-orbit) relativistic density functional calculations of indirect NMR nuclear spin-spin coupling (J-coupling) constants. The finite nuclear volume effects on the hyperfine integrals are quite pronounced and as a consequence they noticeably alter coupling constants involving heavy NMR nuclei such as W, Pt, Hg, Tl, and Pb. Typically, the isotropic J-couplings are reduced in magnitude by about 10 to 15 % for couplings between one of the heaviest NMR nuclei and a light atomic ligand, and even more so for couplings between two heavy atoms. For a subset of the systems studied, viz. the Hg atom, Hg(2) (2+), and Tl--X where X=Br, I, the basis set convergence of the hyperfine integrals and the coupling constants was monitored. For the Hg atom, numerical and basis set calculations of the electron density and the 1s and 6s orbital hyperfine integrals are directly compared. The coupling anisotropies of TlBr and TlI increase by about 2 % due to finite-nucleus effects.

Evaluation of Low-Earth-Orbit Environmental Effects on International Space Station Thermal Control Materials

NASA Technical Reports Server (NTRS)

Dever, Joyce A.

1998-01-01

Many spacecraft thermal control coatings in low Earth orbit (LEO) can be affected by solar ultraviolet radiation and atomic oxygen. Ultraviolet radiation can darken some polymers and oxides commonly used in thermal control materials. Atomic oxygen can erode polymer materials, but it may reverse the ultraviolet-darkening effect on oxides. Maintaining the desired solar absorptance for thermal control coatings is important to assure the proper operating temperature of the spacecraft. Thermal control coatings to be used on the International Space Station (ISS) were evaluated for their performance after exposure in the NASA Lewis Research Center's Atomic Oxygen-Vacuum Ultraviolet Exposure (AO-VUV) facility. This facility simulated the LEO environments of solar vacuum ultraviolet (VUV) radiation (wavelength range, 115 to 200 nanometers (nm)) and VUV combined with atomic oxygen. Solar absorptance was measured in vacuo to eliminate the "bleaching" effects of ambient oxygen on VUV-induced degradation. The objective of these experiments was to determine solar absorptance increases of various thermal control materials due to exposure to simulated LEO conditions similar to those expected for ISS. Work was done in support of ISS efforts at the requests of Boeing Space and Defense Systems and Lockheed Martin Vought Systems.