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Sample records for adsorbed hydrogen atoms

  1. Revisiting the inelastic electron tunneling spectroscopy of single hydrogen atom adsorbed on the Cu(100) surface.

    PubMed

    Jiang, Zhuoling; Wang, Hao; Sanvito, Stefano; Hou, Shimin

    2015-12-21

    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 of 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 4pz 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.

  2. Revisiting the inelastic electron tunneling spectroscopy of single hydrogen atom adsorbed on the Cu(100) surface

    SciTech Connect

    Jiang, Zhuoling; Wang, Hao; Sanvito, Stefano; Hou, Shimin

    2015-12-21

    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 of 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.

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

    NASA Astrophysics Data System (ADS)

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

    2016-11-01

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

  4. Theoretical study of the dynamics of atomic hydrogen adsorbed on graphene multilayers

    NASA Astrophysics Data System (ADS)

    Moaied, Mohammed; Moreno, J. A.; Caturla, M. J.; Ynduráin, Félix; Palacios, J. J.

    2015-04-01

    We present a theoretical study of the dynamics of H atoms adsorbed on graphene bilayers with Bernal stacking. First, through extensive density functional theory calculations, including van der Waals interactions, we obtain the activation barriers involved in the desorption and migration processes of a single H atom. These barriers, along with attempt rates and the energetics of H pairs, are used as input parameters in kinetic Monte Carlo simulations to study the time evolution of an initial random distribution of adsorbed H atoms. The simulations reveal that, at room temperature, H atoms occupy only one sublattice before they completely desorb or form clusters. This sublattice selectivity in the distribution of H atoms may last for sufficiently long periods of time upon lowering the temperature down to 0 ∘C . The final fate of the H atoms, namely, desorption or cluster formation, depends on the actual relative values of the activation barriers which can be tuned by doping. In some cases, a sublattice selectivity can be obtained for periods of time experimentally relevant even at room temperature. This result shows the possibility for observation and applications of the ferromagnetic state associated with such distribution.

  5. Atomic hydrogen rocket engine

    NASA Technical Reports Server (NTRS)

    Etters, R. D.; Flurchick, K.

    1981-01-01

    A rocket using atomic hydrogen propellant is discussed. An essential feature of the proposed engine is that the atomic hydrogen fuel is used as it is produced, thus eliminating the necessity of storage. The atomic hydrogen flows into a combustion chamber and recombines, producing high velocity molecular hydrogen which flows out an exhaust port. Standard thermodynamics, kinetic theory and wall recombination cross-sections are used to predict a thrust of approximately 1.4 N for a RF hydrogen flow rate of 4 x 10 to the 22nd/sec. Specific impulses are nominally from 1000 to 2000 sec. It is predicted that thrusts on the order of one Newton and specific impulses of up to 2200 sec are attainable with nominal RF discharge fluxes on the order of 10 to the 22nd atoms/sec; further refinements will probably not alter these predictions by more than a factor of two.

  6. A theoretical study of hydrogen diffraction following photodissociation of adsorbed molecules

    NASA Astrophysics Data System (ADS)

    Kosloff, Ronnie; Zeiri, Yehuda

    1992-08-01

    A new probe of surface structure is presented which is based on the photodissociation of hydrogen from an adsorbate molecule. The event creates an atomic hydrogen fragment, positioned between the adsorbate layer and the solid surface. Due to its light mass, the hydrogen dynamics is quantum mechanical in nature. A useful image is of the hydrogenic wave function behaving like a liquid able to fill all cracks. The coherent character of the hydrogenic wave function is crucial in the ability of the photodissociation experiment to act as a probe. A series of case studies has been carried out whose aim is to reveal the relation between the structure of the surface and the asymptotic energy resolved angular distribution of the hydrogen fragment. The dynamics of the hydrogen atom motion was modeled by the time dependent Schrödinger equation. The cases studied include the dissociation of a single HBr adsorbate on flat and corrugated surfaces. A broad specular peak was observed, in addition to diffraction peaks which can be correlated with the corrugation. Moreover, selective adsorption peaks, which can be correlated with the attractive part of the surface potential, have been identified. Systems in which the hydrogenic wave function scatters from several adsorbates were also investigated. It was found that the scattering is dominated by the trapping of the wave function by unstable periodic orbits. The quantization rules of these periodic orbits have been identified, creating a link between the structure of the adsorbates and the asymptotic angular distributions.

  7. Hydrogen molecule on lithium adsorbed graphene: A DFT study

    NASA Astrophysics Data System (ADS)

    Kaur, Gagandeep; Gupta, Shuchi; Gaganpreet, Dharamvir, Keya

    2016-05-01

    Electronic structure calculations for the adsorption of molecular hydrogen on lithium (Li) decorated and pristine graphene have been studied systematically using SIESTA code [1] within the framework of the first-principle DFT under the Perdew-Burke-Ernzerhof (PBE) form of the generalized gradient approximation (GGA)[2], including spin polarization. The energy of adsorption of hydrogen molecule on graphene is always enhanced by the presence of co-adsorbed lithium. The most efficient adsorption configuration is when H2 is lying parallel to lithium adsorbed graphene which is in contrast to its adsorption on pristine graphene (PG) where it prefers perpendicular orientation.

  8. Thin film atomic hydrogen detectors

    NASA Technical Reports Server (NTRS)

    Gruber, C. L.

    1977-01-01

    Thin film and bead thermistor atomic surface recombination hydrogen detectors were investigated both experimentally and theoretically. Devices were constructed on a thin Mylar film substrate. Using suitable Wheatstone bridge techniques sensitivities of 80 microvolts/2x10 to the 13th power atoms/sec are attainable with response time constants on the order of 5 seconds.

  9. Atomic hydrogen in planetary nebulae

    NASA Technical Reports Server (NTRS)

    Schneider, Stephen E.; Silverglate, Peter R.; Altschuler, Daniel R.; Giovanardi, Carlo

    1987-01-01

    The authors searched for neutral atomic hydrogen associated with 22 planetary nebulae and three evolved stars in the 21 cm line at the Arecibo Observatory. Objects whose radial velocities permitted discrimination from Galactic H I were chosen for observation. Hydrogen was detected in absorption from IC 4997. From the measurements new low limits are derived to the mass of atomic hydrogen associated with the undetected nebulae. Radio continuum observations were also made of several of the nebulae at 12.6 cm. The authors reexamine previous measurements of H I in planetary nebulae, and present the data on a consistent footing. The question of planetary nebula distances is considered at length. Finally, implications of the H I measurements for nebular evolution are discussed and it is suggested that atomic hydrogen seen in absorption was expelled from the progenitor star during the final 1000 yr prior to the onset of ionization.

  10. Silver diffusion over silicon surfaces with adsorbed tin atoms

    SciTech Connect

    Dolbak, A. E. Olshanetskii, B. Z.

    2015-02-15

    Silver diffusion over the (111), (100), and (110) surfaces of silicon with preliminarily adsorbed tin atoms is studied by Auger electron spectroscopy and low-energy electron diffraction. Diffusion is observed only on the surface of Si(111)-2√3 × 2√3-Sn. The diffusion mechanism is established. It is found that the diffusion coefficient depends on the concentration of diffusing atoms. The diffusion coefficient decreases with increasing silver concentration, while the activation energy and the preexponential factor increase.

  11. A Comprehensive Study of Hydrogen Adsorbing to Amorphous Water ice: Defining Adsorption in Classical Molecular Dynamics

    NASA Astrophysics Data System (ADS)

    Dupuy, John L.; Lewis, Steven P.; Stancil, P. C.

    2016-11-01

    Gas–grain and gas–phase reactions dominate the formation of molecules in the interstellar medium (ISM). Gas–grain reactions require a substrate (e.g., a dust or ice grain) on which the reaction is able to occur. The formation of molecular hydrogen (H2) in the ISM is the prototypical example of a gas–grain reaction. In these reactions, an atom of hydrogen will strike a surface, stick to it, and diffuse across it. When it encounters another adsorbed hydrogen atom, the two can react to form molecular hydrogen and then be ejected from the surface by the energy released in the reaction. We perform in-depth classical molecular dynamics simulations of hydrogen atoms interacting with an amorphous water-ice surface. This study focuses on the first step in the formation process; the sticking of the hydrogen atom to the substrate. We find that careful attention must be paid in dealing with the ambiguities in defining a sticking event. The technical definition of a sticking event will affect the computed sticking probabilities and coefficients. Here, using our new definition of a sticking event, we report sticking probabilities and sticking coefficients for nine different incident kinetic energies of hydrogen atoms [5–400 K] across seven different temperatures of dust grains [10–70 K]. We find that probabilities and coefficients vary both as a function of grain temperature and incident kinetic energy over the range of 0.99–0.22.

  12. An Atomic Hydrogen Mushroom

    NASA Astrophysics Data System (ADS)

    English, J.; Taylor, A. R.; Irwin, J. A.; Canadian Galactic Plane Survey Collaboration

    1998-12-01

    Neutral hydrogen ``worms'', which stream vertically from the mid-plane to high latitudes, may be conduits through which hot gas can escape into the halo. Using the Dominion Radio Astrophysical Observatory's (DRAO) Synthesis Telescope, as part of the Canadian Galactic Plane Survey, we have resolved an HI worm candidate. Although simulations have previously made general predictions, these data will constrain, for the first time, detailed numerical models of the dynamical processes generating disk-halo features. After the incorporation of the data from the 26-m DRAO's single-dish telescope, the mosaic data cube has full information on all spatial scales down to a resolution limit of 1 arcmin and a velocity resolution of 0.82 km s(-1) . Thus we delineate Rayleigh-Taylor instability-like structures and can distinguish a 5 km s(-1) line of sight velocity difference between the base and top of the worm. In general morphology, the worm is mushroom-shaped. Although it extends only a few hundred parsecs south of the midplane, the cap appears to be fragmenting. This may allow hot material from the stem's cavity, as well as UV photons, to escape to higher galactic latitudes. The preliminary estimate of the observed minimum HI mass is 1.3 x 10(5) Msolar. Our initial thin-shell model, which assumes supernovae explosions drive this outflow, gives a minimum total energy of about 100 x 10(51) ergs s(-1) .

  13. Energy storage possibilities of atomic hydrogen

    NASA Technical Reports Server (NTRS)

    Etters, R. D.; Dugan, J. V., Jr.; Palmer, R.

    1976-01-01

    The possibility of storing large amounts of energy in a free radical system such as atomic hydrogen is analyzed. Attention is focused on theoretical calculations of the ground state properties of spin-aligned atomic triplet hydrogen, deuterium, and tritium. The solid-liquid phase transition in atomic hydrogen is also examined.

  14. A theoretical study of the interaction of hydrogen and oxygen with palladium or gold adsorbed on pyridine-like nitrogen-doped graphene.

    PubMed

    Rangel, Eduardo; Magana, Luis Fernando; Sansores, Luis Enrique

    2014-12-15

    The interaction of H2 and O2 molecules in the presence of nitrogen-doped graphene decorated with either a palladium or gold atom was investigated by using density functional theory. It was found that two hydrogen molecules were adsorbed on the palladium atom. The interaction of these adsorbed hydrogen molecules with two oxygen molecules generates two hydrogen peroxide molecules first through a Eley-Rideal mechanism and then through a Langmuir-Hinshelwood mechanism. The barrier energies for this reaction were small; therefore, we expect that this process may occur spontaneously at room temperature. In the case of gold, a single hydrogen molecule is adsorbed and dissociated on the metal atom. The interaction of the dissociated hydrogen molecule on the surface with one oxygen molecule generates a water molecule. The competitive adsorption between oxygen and hydrogen molecules slightly favors oxygen adsorption.

  15. NASA atomic hydrogen standards program: An update

    NASA Technical Reports Server (NTRS)

    Reinhardt, V. S.; Kaufmann, D. C.; Adams, W. A.; Deluca, J. J.; Soucy, J. L.

    1976-01-01

    Comparisons are made between the NP series and the NX series of hydrogen masers. A field operable hydrogen maser (NR series) is also described. Atomic hydrogen primary frequency standards are in development stages. Standards are being developed for a hydrogen beam frequency standard and for a concertina hydrogen maser.

  16. The adsorption of atomic hydrogen on tellurium and formation of H 2Te

    NASA Astrophysics Data System (ADS)

    Outka, Duane A.

    1990-09-01

    The adsorption of hydrogen on a polycrystalline tellurium surface has been studied with temperature programmed desorption. Atomic hydrogen adsorbs on a tellurium surface and reacts to form H 2Te. Molecular hydrogen, in contrast, does not adsorb or react with tellurium at temperatures down to 80 K. When a tellurium surface which has been exposed to atomic hydrogen is heated, two desorption products are observed, H 2 and H 2Te. The H 2Te desorbs in three peaks at 130, 150, and 270 K. The H 2 desorbs in two peaks at 150 and 270 K. The desorption peaks at 270 K for both H 2 and H 2Te are unusually broad with a half-width of 80 K, and standard kinetic analysis of these peaks yields unusual desorption parameters. Overall, the adsorption of hydrogen on tellurium is similar to hydrogen adsorption on other covalent solids and differs in several respects from hydrogen adsorbed on metal surfaces.

  17. Hydrogen storage on palladium adsorbed graphene: A density functional theory study

    NASA Astrophysics Data System (ADS)

    Pantha, Nurapati; Khaniya, Asim; Adhikari, Narayan Prasad

    2015-07-01

    We have performed density functional theory (DFT)-based first-principles calculations to study the stability, geometrical structures, and electronic properties of a single palladium (Pd) atom adsorbed graphene with reference to pristine graphene. The study also covers the adsorption properties of molecular hydrogen/s on the most stable Pd-graphene geometry by taking into account London dispersion forces in addition to the standard DFT calculations in the Quantum ESPRESSO package. From the analysis of estimated values of binding energy of Pd on different occupation sites (i.e., bridge, hollow, and top) of graphene supercells, the bridge site is found to be the most favorable one with the magnitudes of 1.114, 1.426, and 1.433 eV in 2×2, 3×3, and 4×4 supercells, respectively. The study of the electronic properties of Pd adsorbed graphene shows a bandgap of 45 meV, which can account for the breaking of the symmetry of the graphene structure. Regarding the gaseous (hydrogen) adsorption on Pd-adatom graphene, we checked the increasing number of molecular hydrogens (H2) from one to seven on the 3×3 supercell, and found that the adsorption energy per H2 decreases on increasing hydrogen concentration and lies within the range of 0.998-0.151 eV.

  18. Hydrogen-Atom Transfer Reactions.

    PubMed

    Wang, Liang; Xiao, Jian

    2016-04-01

    The cascade [1,n]-hydrogen transfer/cyclization, recognized as the tert-amino effect one century ago, has received considerable interest in recent decades, and great achievements have been made. With the aid of this strategy, the inert C(sp(3))-H bonds can be directly functionalized into C-C, C-N, C-O bonds under catalysis of Lewis acids, Brønsted acids, as well as organocatalysts, and even merely under thermal conditions. Hydrogen can be transferred intramolecularly from hydrogen donor to acceptor in the form of hydride, or proton, followed by cyclization to furnish the cyclic products in processes featuring high atom economy. Methylene/methine adjacent to heteroatoms, e.g., nitrogen, oxygen, sulfur, can be exploited as hydride donor as well as methylene/methine without heteroatom assistance. Miscellaneous electrophilic subunits or intermediates, e.g., alkylidene malonate, carbophilic metal activated alkyne or allene, α,β-unsaturated aldehydes/ketone, saturated aldehydes/iminium, ketenimine/carbodiimide, metal carbenoid, electron-withdrawing groups activated allene/alkyne, in situ generated carbocation, can serve as hydride acceptors. This methodology has shown preeminent power to construct 5-, 6-, or 7-membered heterocyclic as well as carbon rings. In this chapter, various hydrogen donors and acceptors are adequately discussed. PMID:27573142

  19. Chiral modification of platinum: ab initio study of the effect of hydrogen coadsorption on stability and geometry of adsorbed cinchona alkaloids.

    PubMed

    Hahn, Konstanze R; Seitsonen, Ari P; Baiker, Alfons

    2015-11-01

    The cinchona alkaloids cinchonidine and cinchonine belong to the most efficient chiral modifiers for the noble metal-catalyzed enantioselective hydrogenation of C=O and C=C bonds. Under reaction conditions these modifiers are coadsorbed on the noble metal surface with hydrogen. Using density functional theory, we studied the effect of coadsorbed hydrogen on the adsorption mode of cinchonidine and cinchonine on a Pt(111) surface at different hydrogen coverages. The theoretical study indicates that the presence of coadsorbed hydrogen affects both the adsorption geometry as well as the stability of the adsorbed cinchona alkaloids. At all hydrogen coverages the cinchona alkaloids are found to be adsorbed via anchoring of the quinoline moiety. In the absence of hydrogen as well as at low hydrogen coverage the quinoline moiety adsorbs nearly parallel to the surface, whereas at higher hydrogen coverage it becomes tilted. Higher hydrogen coverage as well as partial hydrogenation of the quinoline part of the cinchona alkaloid and hydrogen transfer to the C[double bond, length as m-dash]C double bond at 10, 11 position of the quinuclidine moiety destabilize the adsorbed cinchona alkaloid, whereas hydrogen transfer to the nitrogen atom of the quinoline and the quinuclidine moiety stabilizes the adsorbed molecule. The stability as well as the adsorption geometry of the cinchona alkaloids are affected by the coadsorbed hydrogen and are proposed to influence the efficiency of the enantiodifferentiating ability of the chirally modified platinum surface.

  20. Chiral modification of platinum: ab initio study of the effect of hydrogen coadsorption on stability and geometry of adsorbed cinchona alkaloids.

    PubMed

    Hahn, Konstanze R; Seitsonen, Ari P; Baiker, Alfons

    2015-11-01

    The cinchona alkaloids cinchonidine and cinchonine belong to the most efficient chiral modifiers for the noble metal-catalyzed enantioselective hydrogenation of C=O and C=C bonds. Under reaction conditions these modifiers are coadsorbed on the noble metal surface with hydrogen. Using density functional theory, we studied the effect of coadsorbed hydrogen on the adsorption mode of cinchonidine and cinchonine on a Pt(111) surface at different hydrogen coverages. The theoretical study indicates that the presence of coadsorbed hydrogen affects both the adsorption geometry as well as the stability of the adsorbed cinchona alkaloids. At all hydrogen coverages the cinchona alkaloids are found to be adsorbed via anchoring of the quinoline moiety. In the absence of hydrogen as well as at low hydrogen coverage the quinoline moiety adsorbs nearly parallel to the surface, whereas at higher hydrogen coverage it becomes tilted. Higher hydrogen coverage as well as partial hydrogenation of the quinoline part of the cinchona alkaloid and hydrogen transfer to the C[double bond, length as m-dash]C double bond at 10, 11 position of the quinuclidine moiety destabilize the adsorbed cinchona alkaloid, whereas hydrogen transfer to the nitrogen atom of the quinoline and the quinuclidine moiety stabilizes the adsorbed molecule. The stability as well as the adsorption geometry of the cinchona alkaloids are affected by the coadsorbed hydrogen and are proposed to influence the efficiency of the enantiodifferentiating ability of the chirally modified platinum surface. PMID:26426825

  1. Experiments with trapped hydrogen atoms and neutrons

    NASA Astrophysics Data System (ADS)

    Ramsey, Norman F.

    1995-01-01

    The earliest trapped atom coherent resonance experiments were with material traps or bottles. In the atomic hydrogen maser the atoms are trapped inside a teflon-coated quartz bulb for about a second. Neutrons have been trapped for hundreds of seconds in suitably coated bottles or in superconducting magnetic traps. Results from experiments with trapped atoms and neutrons are given.

  2. Experiments with trapped hydrogen atoms and neutrons

    NASA Astrophysics Data System (ADS)

    Ramsey, Norman F.

    1993-03-01

    The earliest trapped atom coherent resonance experiments were with material traps or bottles. In the atomic hydrogen maser, the atoms are trapped inside a teflon-coated quartz bulb for about a second. Neutrons have been trapped for hundreds of seconds in suitably coated bottles or in superconducting magnetic traps. Results from experiments with trapped atoms and neutrons are reported.

  3. Application of Henry's Law for Binding Energies of Adsorbed Hydrogen

    NASA Astrophysics Data System (ADS)

    Gillespie, Andrew; Dohnke, Elmar; Stalla, David; Sweany, Mark; Pfeifer, Peter

    2015-03-01

    The method of isosteres is the simplest method used to calculate the differential enthalpy of adsorption. However, it is incredibly sensitive to the choice of model and respective fitting parameters. For a set of isotherms measured on a specific sample, most models converge upon a similar value at high coverage, but are inconsistent in the low pressure regime. In this talk, we investigate the application of various models for localized and mobile adsorption at low pressures in order to obtain binding energy of hydrogen to the adsorbent surface. Henry's Law analysis of the Langmuir Model of adsorption yield binding energies in excellent agreement with those obtained from the Clausius Clapeyron relation. Work supported by DOE-EERE, Award No. DE-FG36-08GO18142.

  4. Effects of hydrogen atom spin exchange collisions on atomic hydrogen maser oscillation frequency

    NASA Technical Reports Server (NTRS)

    Crampton, S. B.

    1979-01-01

    Frequency shifts due to collisions between hydrogen atoms in an atomic hydrogen maser frequency standard are studied. Investigations of frequency shifts proportional to the spin exchange frequency shift cross section and those proportional to the duration of exchange collisions are discussed. The feasibility of operating a hydrogen frequency standard at liquid helium temperatures is examined.

  5. Atomic hydrogen as a launch vehicle propellant

    NASA Technical Reports Server (NTRS)

    Palaszewski, Bryan A.

    1990-01-01

    An analysis of several atomic hydrogen launch vehicles was conducted. A discussion of the facilities and the technologies that would be needed for these vehicles is also presented. The Gross Liftoff Weights (GLOW) for two systems were estimated; their specific impulses (I sub sp) were 750 and 1500 lb (sub f)/s/lb(sub m). The atomic hydrogen launch vehicles were also compared to the currently planned Advanced Launch System design concepts. Very significant GLOW reductions of 52 to 58 percent are possible over the Advanced Launch System designs. Applying atomic hydrogen propellants to upper stages was also considered. Very high I(sub sp) (greater than 750 1b(sub f)/s/lb(sub m) is needed to enable a mass savings over advanced oxygen/hydrogen propulsion. Associated with the potential benefits of high I(sub sp) atomic hydrogen are several challenging problems. Very high magnetic fields are required to maintain the atomic hydrogen in a solid kilogauss (3 Tesla). Also the storage temperature of the propellant is 4 K. This very low temperature will require a large refrigeration facility for the launch vehicle. The design considerations for a very high recombination rate for the propellant are also discussed. A recombination rate of 210 cm/s is predicted for atomic hydrogen. This high recombination rate can produce very high acceleration for the launch vehicle. Unique insulation or segmentation to inhibit the propellant may be needed to reduce its recombination rate.

  6. Properties of SBA-15 modified by iron nanoparticles as potential hydrogen adsorbents and sensors

    NASA Astrophysics Data System (ADS)

    Bouazizi, N.; Ouargli, R.; Nousir, S.; Slama, R. Ben; Azzouz, A.

    2015-02-01

    SBA-15-Fe was synthesized via the incorporation of Fe0 nanoparticles (Fe(0)-Nps) in the mesoporous channels. Electron microscopy and X-ray diffraction showed that dispersion of fine iron NPs occurs mainly inside the channels of SBA-15, producing a slight structure compaction. This was accompanied by a significant improvement of both the affinity towards hydrogen and electrical conductivity, as supported by hydrogen adsorption tests and impedance measurements. CO2 thermal programmed desorption measurements revealed an attenuation of the acid character of the solid surface. This was explained in terms of strong iron interaction with the lattice oxygen atoms that reduces the SiO-H bond polarity. The close vicinity of fine Fe(0)-Nps combined with the large pore size of SBA-15 appear to contribute to a synergistic improvement of the electrical conductivity. The results reported herein open new prospects for SBA-15 as potential adsorbents for hydrogen storage and carriers for hydrogen sensors. The use of iron in lieu of noble metals for designing such materials is a novelty, because such applications of iron-loaded silica have not been envisaged so far due to the high reactivity of iron towards air and water. The development of such technologies, if any, should address this issue.

  7. The Hydrogen Atom: The Rutherford Model

    NASA Astrophysics Data System (ADS)

    Tilton, Homer Benjamin

    1996-06-01

    Early this century Ernest Rutherford established the nuclear model of the hydrogen atom, presently taught as representing the best visual model after modification by Niels Bohr and Arnold Sommerfeld. It replaced the so-called "plum pudding" model of J. J. Thomson which held sway previously. While the Rutherford model represented a large step forward in our understanding of the hydrogen atom, questions remained, and still do.

  8. Energy storage possibilities of atomic hydrogen

    NASA Technical Reports Server (NTRS)

    Etters, R. D.; Dugan, J. V., Jr.; Palmer, R.

    1976-01-01

    Several recent experiments designed to produce and store macroscopic quantities of atomic hydrogen are discussed. The bulk, ground state properties of atomic hydrogen, deuterium, and tritium systems are calculated assuming that all pair interactions occur via the atomic triplet potential. The conditions required to obtain this system, including inhibition of recombination through the energetically favorable singlet interaction, are discussed. The internal energy, pressure, and compressibility are calculated applying the Monte Carlo technique with a quantum mechanical variational wavefunction. The system studied consisted of 32 atoms in a box with periodic boundary conditions. Results show that atomic triplet hydrogen and deuterium remain gaseous at 0 K; i.e., the internal energy is positive at all molar volumes considered.

  9. Solid Hydrogen Formed for Atomic Propellants

    NASA Technical Reports Server (NTRS)

    Palaszewski, Bryan A.

    2000-01-01

    Several experiments on the formation of solid hydrogen particles in liquid helium were recently conducted at the NASA Glenn Research Center at Lewis Field. The solid hydrogen experiments are the first step toward seeing these particles and determining their shape and size. The particles will ultimately store atoms of boron, carbon, or hydrogen, forming an atomic propellant. Atomic propellants will allow rocket vehicles to carry payloads many times heavier than possible with existing rockets or allow them to be much smaller and lighter. Solid hydrogen particles are preferred for storing atoms. Hydrogen is generally an excellent fuel with a low molecular weight. Very low temperature hydrogen particles (T < 4 K) can prevent the atoms from recombining, making it possible for their lifetime to be controlled. Also, particles that are less than 1 mm in diameter are preferred because they can flow easily into a pipe when suspended in liquid helium. The particles and atoms must remain at this low temperature until the fuel is introduced into the engine combustion (or recombination) chamber. Experiments were, therefore, planned to look at the particles and observe their formation and any changes while in liquid helium.

  10. Hydrogen as an atomic beam standard

    NASA Technical Reports Server (NTRS)

    Peters, H. E.

    1972-01-01

    After a preliminary discussion of feasibility, new experimental work with a hydrogen beam is described. A space focused magnetic resonance technique with separated oscillatory fields is used with a monochromatic beam of cold hydrogen atoms which are selected from a higher temperature source. The first resonance curves and other experimental results are presented. These results are interpreted from the point of view of accuracy potential and frequency stability, and are compared with hydrogen maser and cesium beam capabilities.

  11. Atomic hydrogen interaction with Ru(1010).

    PubMed

    Vesselli, E; Comelli, G; Rosei, R

    2004-05-01

    The interaction of atomic hydrogen with clean and deuterium precovered Ru(1010) was studied by means of temperature-programmed desorption (TPD) spectroscopy. Compared to molecular hydrogen experiments, after exposure of the clean surface to gas-phase atomic hydrogen at 90 K, two additional peaks grow in the desorption spectra at 115 and 150 K. The surface saturation coverage, determined by equilibrium between abstraction and adsorption reactions, is 2.5 monolayers. Preadsorbed deuterium abstraction experiments with gas-phase atomic hydrogen show that a pure Eley-Rideal mechanism is not involved in the process, while a hot atom (HA) kinetics describes well the reaction. By least-squares fitting of the experimental data, a simplified HA kinetic model yields an abstraction cross section value of 0.5 +/- 0.2 angstroms2. The atomic hydrogen interaction with an oxygen precovered surface was also studied by means of both TPD and x-ray photoelectron spectroscopy: oxygen hydrogenation and water production take place already at very low temperature (90 K).

  12. Electron-hole pair excitation determines the mechanism of hydrogen atom adsorption.

    PubMed

    Bünermann, Oliver; Jiang, Hongyan; Dorenkamp, Yvonne; Kandratsenka, Alexander; Janke, Svenja M; Auerbach, Daniel J; Wodtke, Alec M

    2015-12-11

    How much translational energy atoms and molecules lose in collisions at surfaces determines whether they adsorb or scatter. The fact that hydrogen (H) atoms stick to metal surfaces poses a basic question. Momentum and energy conservation demands that the light H atom cannot efficiently transfer its energy to the heavier atoms of the solid in a binary collision. How then do H atoms efficiently stick to metal surfaces? We show through experiments that H-atom collisions at an insulating surface (an adsorbed xenon layer on a gold single-crystal surface) are indeed nearly elastic, following the predictions of energy and momentum conservation. In contrast, H-atom collisions with the bare gold surface exhibit a large loss of translational energy that can be reproduced by an atomic-level simulation describing electron-hole pair excitation. PMID:26612832

  13. Reactivity and Catalytic Activity of Hydrogen Atom Chemisorbed Silver Clusters.

    PubMed

    Manzoor, Dar; Pal, Sourav

    2015-06-18

    Metal clusters of silver have attracted recent interest of researchers as a result of their potential in different catalytic applications and low cost. However, due to the completely filled d orbital and very high first ionization potential of the silver atom, the silver-based catalysts interact very weakly with the reacting molecules. In the current work, density functional theory calculations were carried out to investigate the effect of hydrogen atom chemisorption on the reactivity and catalytic properties of inert silver clusters. Our results affirm that the hydrogen atom chemisorption leads to enhancement in the binding energy of the adsorbed O2 molecule on the inert silver clusters. The increase in the binding energy is also characterized by the decrease in the Ag-O and increase in the O-O bond lengths in the case of the AgnH silver clusters. Pertinent to the increase in the O-O bond length, a significant red shift in the O-O stretching frequency is also noted in the case of the AgnH silver clusters. Moreover, the hydrogen atom chemisorbed silver clusters show low reaction barriers and high heat of formation of the final products for the environmentally important CO oxidation reaction as compared to the parent catalytically inactive clusters. The obtained results were compared with those of the corresponding gold and hydrogen atom chemisorbed gold clusters obtained at the same level of theory. It is expected the current computational study will provide key insights for future advances in the design of efficient nanosilver-based catalysts through the adsorption of a small atom or a ligand.

  14. Atomic hydrogen as a launch vehicle propellant

    NASA Technical Reports Server (NTRS)

    Palaszewski, Bryan A.

    1990-01-01

    An analysis of several atomic hydrogen launch vehicles was conducted. A discussion of the facilities and the technologies that would be needed for these vehicles is also presented. The Gross Liftoff Weights (GLOW) for two systems were estimated; their specific impulses (I sub sp) were 750 and 1500 lb(sub f)/s/lb(sub m). The atomic hydrogen launch vehicles were also compared to the currently planned Advanced Launch System design concepts. Very significant GLOW reductions of 52 to 58 percent are possible over the Advanced Launch System designs. Applying atomic hydrogen propellants to upper stages was also considered. Very high I(sub sp) (greater than 750 lb(sub f)/s/lb(sub m)) is needed to enable a mass savings over advanced oxygen/hydrogen propulsion. Associated with the potential benefits of high I(sub sp) atomic hydrogen are several challenging problems. Very high magnetic fields are required to maintain the atomic hydrogen in a solid hydrogen matrix. The magnetic field strength was estimated to be 30 kilogauss (3 Tesla). Also the storage temperature of the propellant is 4 K. This very low temperature will require a large refrigeration facility for the launch vehicle. The design considerations for a very high recombination rate for the propellant are also discussed. A recombination rate of 210 cm/s is predicted for atomic hydrogen. This high recombination rate can produce very high acceleration for the launch vehicle. Unique insulation or segmentation to inhibit the propellant may be needed to reduce its recombination rate.

  15. Atomic hydrogen as a launch vehicle propellant

    SciTech Connect

    Palaszewski, B.A.

    1990-01-01

    An analysis of several atomic hydrogen launch vehicles was conducted. A discussion of the facilities and the technologies that would be needed for these vehicles is also presented. The Gross Liftoff Weights (GLOW) for two systems were estimated; their specific impulses (I{sub sp}) were 750 and 1500 lb{sub f}/s/lb{sub m}. The atomic hydrogen launch vehicles were also compared to the currently planned Advanced Launch System design concepts. Very significant GLOW reductions of 52 to 58 percent are possible over the Advanced Launch System designs. Applying atomic hydrogen propellants to upper stages was also considered. Very high I{sub sp} (greater than 750 lb{sub f}/s/lb{sub m}) is needed to enable a mass savings over advanced oxygen/hydrogen propulsion. Associated with the potential benefits of high I(sub sp) atomic hydrogen are several challenging problems. Very high magnetic fields are required to maintain the atomic hydrogen in a solid hydrogen matrix. The magnetic field strength was estimated to be 30 kilogauss (3 Tesla). Also the storage temperature of the propellant is 4 K. This very low temperature will require a large refrigeration facility for the launch vehicle. The design considerations for a very high recombination rate for the propellant are also discussed. A recombination rate of 210 cm/s is predicted for atomic hydrogen. This high recombination rate can produce very high acceleration for the launch vehicle. Unique insulation or segmentation to inhibit the propellant may be needed to reduce its recombination rate.

  16. Electronic and magnetic properties of nonmetal atoms adsorbed ReS{sub 2} monolayers

    SciTech Connect

    Zhang, Xiaoou; Li, Qingfang

    2015-08-14

    The stable configurations and electronic and magnetic properties of nonmetal atoms (H, N, P, O, S, F, and Cl) adsorbed ReS{sub 2} monolayers have been investigated by first-principles calculations. It is found that H, O, S, F, and Cl prefer to occupy the peak sites of S atoms, while both N and P atoms favor the valley sites of S atoms. The ReS{sub 2} sheet exhibits a good adsorption capability to nonmetal atoms. The reconstruction of the surface is pronounced in N- and P-adsorbed ReS{sub 2} monolayers. In H-adsorbed case, the Fermi level is pulled into the conduction band, which results in the semiconductor-metal transition. The same magnetic moment of 1μ{sub B} is found in the N-, P-, F-, and Cl-adsorbed ReS{sub 2} monolayers, while the mechanisms of forming magnetic moment for N (P)- and F (Cl)-adsorbed cases are different. In addition, the spatial extensions of spin density in P-, F-, and Cl-adsorbed cases are larger than that in N-adsorbed case, which is more suitable to achieve long-range magnetic coupling interaction at low defect concentrations. Our results provide insight for achieving metal-free magnetism and a tunable band gap for various electronic and spintronic devices based on ReS{sub 2}.

  17. Location of hydrogen atoms in hydronium jarosite

    NASA Astrophysics Data System (ADS)

    Spratt, Henry J.; Avdeev, Maxim; Pfrunder, Michael C.; McMurtrie, John; Rintoul, Llew; Martens, Wayde N.

    2014-07-01

    Various models for the crystal structure of hydronium jarosite were determined from Rietveld refinements against neutron powder diffraction patterns collected at ambient temperature and also single-crystal X-ray diffraction data. The possibility of a lower symmetry space group for hydronium jarosite that has been suggested by the literature was investigated. It was found the space group is best described as , the same for other jarosite minerals. The hydronium oxygen atom was found to occupy the site (3a Wyckoff site). Inadequately refined hydronium bond angles and bond distances without the use of restraints are due to thermal motion and disorder of the hydronium hydrogen atoms across numerous orientations. However, the acquired data do not permit a precise determination of these orientations; the main feature up/down disorder of hydronium is clear. Thus, the highest symmetry model with the least disorder necessary to explain all data was chosen: The hydronium hydrogen atoms were modeled to occupy an m (18 h Wyckoff site) with 50 % fractional occupancy, leading to disorder across two orientations. A rigid body description of the hydronium ion rotated by 60° with H-O-H bond angles of 112° and O-H distances of 0.96 Å was optimal. This rigid body refinement suggests that hydrogen bonds between hydronium hydrogen atoms and basal sulfate oxygen atoms are not predominant. Instead, hydrogen bonds are formed between hydronium hydrogen atoms and hydroxyl oxygen atoms. The structure of hydronium alunite is expected to be similar given that alunite supergroup minerals are isostructural.

  18. The adsorption of a hydrogen atom on the two types of boron sheets surface

    NASA Astrophysics Data System (ADS)

    Boroznina, E. V.; Borkhoeva, N. N.; Boroznin, S. V.

    2015-01-01

    The possible connection between the atom of hydrogen and the surface of twodimensional boron sheets have been investigated. The calculations were carried out within the model of molecular cluster with the use of quantum chemical MNDO scheme. Two types of BS were studied: triangular BS (TBS) and α-sheet of boron atoms (αBS). The hydrogen atoms attacking BS have been simulated by a step-by-step approach for all atom locations. The surface patterns of potential energy for these processes were built. The analysis of curves showed that the active atom of hydrogen is adsorbed on the surface of BS. The adsorption distances (Rad) and the adsorption energy (Ead) were calculated. We have proved that αBS has a greater sorption capacity than hydrogen TBS.

  19. Interaction between adsorbed hydrogen and potassium on a carbon nanocone containing material as studied by photoemission

    SciTech Connect

    Yu, Xiaofeng; Raaen, Steinar

    2015-09-14

    Hydrogen adsorption on a potassium doped carbon nanocone containing material was studied by photoelectron spectroscopy and work function measurement. The valence band spectra indicate that there is charge transfer from potassium to carbon. Upon deposition on carbon potassium is in its ionic state for lower doping and shows both ionic and metallic behavior at higher doping. Adsorption of hydrogen facilitates diffusion of potassium on the carbon material as seen by changes in the K{sub 2p} core level spectrum. Variations in the measured sample work function indicate that hydrogen initially adsorb on the K dopants and subsequently adsorb on the carbon cone containing material.

  20. Ionization of polarized hydrogen atoms

    SciTech Connect

    Alessi, J.G.

    1983-01-01

    Methods are discussed for the production of polarized H/sup -/ ions from polarized atoms produced in ground state atomic beam sources. Present day sources use ionizers of two basic types - electron ionizers for H/sup +/ Vector production followed by double charge exchange in a vapor, or direct H/sup -/ Vector production by charge exchange of H/sup 0/ with Cs/sup 0/. Both methods have ionization efficiencies of less than 0.5%. Ionization efficiencies in excess of 10% may be obtained in the future by the use of a plasma ionizer plus charge exchange in Cs or Sr vapor, or ionization by resonant charge exchange with a self-extracted D/sup -/ beam from a ring magnetron or HCD source. 36 references, 4 figures.

  1. Trapping of hydrogen atoms in X-irradiated salts at room temperature and the decay kinetics

    NASA Technical Reports Server (NTRS)

    May, C. E.; Philipp, W. H.; Marsik, S. J.

    1974-01-01

    The salts (hypophosphites, formates, a phosphite, a phosphate, and an oxalate) were X-irradiated, whereby hydrogen formed chemically by a radiolytic process becomes trapped in the solid. By room temperature vacuum extraction, the kinetics for the evolution of this trapped hydrogen was studied mass spectrometrically. All salts except two exhibited second-order kinetics. The two exceptions (NaH2PO2(H2O) and K2HPO4) showed first-order kinetics. Based on experimental results, the escape of hydrogen involves three steps: the diffusion of hydrogen atoms from the bulk to the surface, association of these atoms on the surface (rate controlling step for second-order hydrogen evolution), and the desorption of molecular hydrogen from the surface. The hydrogen does not escape if the irradiated salt is stored in air, apparently because adsorbed air molecules occupy surface sites required in the escape mechanism.

  2. Uranium Recovery from Seawater: Development of Fiber Adsorbents Prepared via Atom-Transfer Radical Polymerization

    SciTech Connect

    Saito, Tomonori; Brown, Suree; Chatterjee, Sabornie; Kim, Jungseung; Tsouris, Costas; Mayes, Richard T; Kuo, Li-Jung; Gill, Gary; Oyola, Yatsandra; Janke, Christopher James; Dai, Sheng

    2014-01-01

    A novel adsorbent preparation method using atom-transfer radical polymerization (ATRP) combined with radiation-induced graft polymerization (RIGP) was developed to synthesize an adsorbent for uranium recovery from seawater. The ATRP method allowed a much higher degree of grafting on the adsorbent fibers (595 2818%) than that allowed by RIGP alone. The adsorbents were prepared with varied composition of amidoxime groups and hydrophilic acrylate groups. The successful preparation revealed that both ligand density and hydrophilicity were critical for optimal performance of the adsorbents. Adsorbents synthesized in this study showed a relatively high performance (141 179 mg/g at 49 62 % adsorption) in laboratory screening tests using a uranium concentration of ~6 ppm. This performance is much higher than that of known commercial adsorbents. However, actual seawater experiment showed impeded performance compared to the recently reported high-surface-area-fiber adsorbents, due to slow adsorption kinetics. The impeded performance motivated an investigation of the effect of hydrophilic block addition on the graft chain terminus. The addition of hydrophilic block on the graft chain terminus nearly doubled the uranium adsorption capacity in seawater, from 1.56 mg/g to 3.02 mg/g. The investigation revealed the importance of polymer chain conformation, in addition to ligand and hydrophilic group ratio, for advanced adsorbent synthesis for uranium recovery from seawater.

  3. Moller Polarimetry with Atomic Hydrogen Targets

    SciTech Connect

    Eugene Chudakov; Vladimir Luppov

    2003-10-19

    A novel proposal of using polarized atomic hydrogen gas, stored in an ultra-cold magnetic trap, as the target for electron beam polarimetry based on Moller scattering is discussed. Such a target of practically 100% polarized electrons could provide a superb systematic accuracy of about 0.5% for beam polarization measurements. The feasibility studies for the CEBAF electron beam have been performed.

  4. Compact microwave cavity for hydrogen atomic clock

    NASA Technical Reports Server (NTRS)

    Zhang, Dejun; Zhang, Yan; Fu, Yigen; Zhang, Yanjun

    1992-01-01

    A summary is presented that introduces the compact microwave cavity used in the hydrogen atomic clock. Special emphasis is placed on derivation of theoretical calculating equations of main parameters of the microwave cavity. A brief description is given of several methods for discriminating the oscillating modes. Experimental data and respective calculated values are also presented.

  5. Atomic line emission analyzer for hydrogen isotopes

    DOEpatents

    Kronberg, J.W.

    1993-03-30

    Apparatus for isotopic analysis of hydrogen comprises a low pressure chamber into which a sample of hydrogen is introduced and then exposed to an electrical discharge to excite the electrons of the hydrogen atoms to higher energy states and thereby cause the emission of light on the return to lower energy states, a Fresnel prism made at least in part of a material anomalously dispersive to the wavelengths of interest for dispersing the emitted light, and a photodiode array for receiving the dispersed light. The light emitted by the sample is filtered to pass only the desired wavelengths, such as one of the lines of the Balmer series for hydrogen, the wavelengths of which differ slightly from one isotope to another. The output of the photodiode array is processed to determine the relative amounts of each isotope present in the sample. Additionally, the sample itself may be recovered using a metal hydride.

  6. Atomic line emission analyzer for hydrogen isotopes

    DOEpatents

    Kronberg, James W.

    1993-01-01

    Apparatus for isotopic analysis of hydrogen comprises a low pressure chamber into which a sample of hydrogen is introduced and then exposed to an electrical discharge to excite the electrons of the hydrogen atoms to higher energy states and thereby cause the emission of light on the return to lower energy states, a Fresnel prism made at least in part of a material anomalously dispersive to the wavelengths of interest for dispersing the emitted light, and a photodiode array for receiving the dispersed light. The light emitted by the sample is filtered to pass only the desired wavelengths, such as one of the lines of the Balmer series for hydrogen, the wavelengths of which differ slightly from one isotope to another. The output of the photodiode array is processed to determine the relative amounts of each isotope present in the sample. Additionally, the sample itself may be recovered using a metal hydride.

  7. Atomic line emission analyzer for hydrogen isotopes

    DOEpatents

    Kronberg, J.W.

    1991-05-08

    Apparatus for isotopic analysis of hydrogen comprises a low pressure chamber into which a sample of hydrogen is introduced and then exposed to an electrical discharge to excite the electrons of the hydrogen atoms to higher energy states and thereby cause the emission of light on the return to lower energy states, a Fresnel prism made at least in part of a material anomalously dispersive to the wavelengths of interest for dispersing the emitted light, and a photodiode array for receiving the dispersed light. The light emitted by the sample is filtered to pass only the desired wavelengths, such as one of the lines of the Balmer series for hydrogen, the wavelengths of which differ slightly from one isotope to another. The output of the photodiode array is processed to determine the relative amounts of each isotope present in the sample. Additionally, the sample itself may be recovered using, a metal hydride.

  8. Loss of hydrogen atoms in H{sub 2} plasma on the surfaces of materials used in EUV lithography

    SciTech Connect

    Zyryanov, S. M.; Kovalev, A. S.; Lopaev, D. V.; Malykhin, E. M.; Rakhimov, A. T.; Rakhimova, T. V.; Koshelev, K. N.; Krivtsun, V. M.

    2011-10-15

    Low-pressure hydrogen is an important component of the working medium in extreme ultraviolet (EUV) projection lithography. Under the action of EUV photons and fast secondary electrons on the gas medium, plasma and atomic hydrogen, actively interacting with the surface, are produced. This interaction is very important, because it largely determines the lifetime of the multilayered EUV optics. In this study, the loss of atomic hydrogen under the conditions of a low pressure (<10 Torr) RF plasma discharge on the surfaces of materials used in EUV lithography is investigated. The surface loss probabilities of H atoms on these materials are measured. It is shown that surface recombination of atomic hydrogen goes according to the Eley-Rideal mechanism via direct recombination of H atoms from the gas phase with chemically and physically adsorbed atoms. In this case, the surface recombination probability is mainly determined by the density of chemical adsorption sites. The density of adsorption sites and the desorption energy of H atoms are estimated. The desorption energy of physically adsorbed H atoms on pure metal surfaces (or surfaces exposed to plasma) is about 0.5 eV, and the density of sorption sites is close to the surface density of atoms. This results in a high loss probability of H atoms on metals ({approx}0.1). Therefore, to provide efficient transportation of hydrogen atoms, it is necessary to use materials with the lowest loss probability of H atoms, i.e., dielectrics.

  9. Beam transport of low temperature atomic hydrogen

    NASA Astrophysics Data System (ADS)

    Kaufman, W. A.

    1993-12-01

    Analytic calculations and particle tracking simulations are presented for a polarized atomic hydrogen beam produced by extraction from an ultra-cold (T=300 mK) helium film coated cell in a large solenoidal magnetic field (12 T). Initial focusing of states 1 and 2 by the solenoidal field and subsequent focusing by a sextupole are examined within the constraints imposed by the requirements of the polarized jet for the experiments NEPTUN and NEPTUN-A at UNK.

  10. Solid Hydrogen Experiments for Atomic Propellants

    NASA Technical Reports Server (NTRS)

    Palaszewski, Bryan

    2001-01-01

    This paper illustrates experiments that were conducted on the formation of solid hydrogen particles in liquid helium. Solid particles of hydrogen were frozen in liquid helium, and observed with a video camera. The solid hydrogen particle sizes, their molecular structure transitions, and their agglomeration times were estimated. article sizes of 1.8 to 4.6 mm (0.07 to 0. 18 in.) were measured. The particle agglomeration times were 0.5 to 11 min, depending on the loading of particles in the dewar. These experiments are the first step toward visually characterizing these particles, and allow designers to understand what issues must be addressed in atomic propellant feed system designs for future aerospace vehicles.

  11. Reaction of atomic hydrogen with formic acid.

    PubMed

    Cao, Qian; Berski, Slawomir; Latajka, Zdzislaw; Räsänen, Markku; Khriachtchev, Leonid

    2014-04-01

    We study the reaction of atomic hydrogen with formic acid and characterize the radical products using IR spectroscopy in a Kr matrix and quantum chemical calculations. The reaction first leads to the formation of an intermediate radical trans-H2COOH, which converts to the more stable radical trans-cis-HC(OH)2via hydrogen atom tunneling on a timescale of hours at 4.3 K. These open-shell species are observed for the first time as well as a reaction between atomic hydrogen and formic acid. The structural assignment is aided by extensive deuteration experiments and ab initio calculations at the UMP2 and UCCSD(T) levels of theory. The simplest geminal diol radical trans-cis-HC(OH)2 identified in the present work as the final product of the reaction should be very reactive, and further reaction channels are of particular interest. These reactions and species may constitute new channels for the initiation and propagation of more complex organic species in the interstellar clouds.

  12. Adsorption of atomic hydrogen on ZnO(1010): STM study.

    PubMed

    Yin, Xiu-Li; Birkner, Alexander; Hänel, Kathrin; Löber, Thomas; Köhler, Ulrich; Wöll, Christof

    2006-04-01

    The adsorption of atomic hydrogen on a single crystal ZnO(1010) surface has been studied by scanning tunneling microscopy (STM) under ultrahigh vacuum conditions at room temperature and at elevated temperatures. High resolution STM images indicate that a well-ordered (1x1) H adlayer is formed on the ZnO(1010) surface. The STM data strongly indicate that the hydrogen adsorbs on top of the oxygen atoms forming hydroxyl species. Scanning tunneling spectroscopy (STS) studies reveal a H atom induced metallization at room temperature. In contrast to the clean surface for the hydrogen-covered surface distinct defects structures consisting of missing O and Zn atoms could be identified.

  13. Direct imaging of Pt single atoms adsorbed on TiO2 (110) surfaces.

    PubMed

    Chang, Teng-Yuan; Tanaka, Yusuke; Ishikawa, Ryo; Toyoura, Kazuaki; Matsunaga, Katsuyuki; Ikuhara, Yuichi; Shibata, Naoya

    2014-01-01

    Noble metal nanoparticles (e.g., gold and platinum) supported on TiO2 surfaces are utilized in many technological applications such as heterogeneous catalysts. To fully understand their enhanced catalytic activity, it is essential to unravel the interfacial interaction between the metal atoms and TiO2 surfaces at the level of atomic dimensions. However, it has been extremely difficult to directly characterize the atomic-scale structures that result when individual metal atoms are adsorbed on the TiO2 surfaces. Here, we show direct atomic-resolution images of individual Pt atoms adsorbed on TiO2 (110) surfaces using aberration-corrected scanning transmission electron microscopy. Subangstrom spatial resolution enables us to identify five different Pt atom adsorption sites on the TiO2 (110) surface. Combining this with systematic density functional theory calculations reveals that the most favorable Pt adsorption sites are on vacancy sites of basal oxygen atoms that are located in subsurface positions relative to the top surface bridging oxygen atoms.

  14. Fourteen Years of Atomic Hydrogen from SABER

    NASA Astrophysics Data System (ADS)

    Hunt, L. A.; Mlynczak, M. G.

    2015-12-01

    We present results for atomic hydrogen in the mesopause region (80-100 km) derived from measurements made by the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) instrument on the TIMED satellite. SABER has been measuring the vertical distribution of infrared radiation emitted by various atmospheric gases for nearly 14 years, providing important information about chemical species, including atomic oxygen, atomic hydrogen, ozone and hydroxyl; temperature; and the radiation budget in the upper atmosphere. The methodology for the derivation of daytime and nighttime concentrations and volume mixing ratios will be presented. Zonal mean and global average daytime and nighttime concentrations of H, which demonstrate excellent agreement between 87 and 95 km, have been calculated and the results are compared with observations from the Solar Mesosphere Explorer (SME) satellite made nearly 30 years ago. Variability over the course of the SABER mission will be shown, including the apparent inverse dependence on the solar cycle, which stems from the temperature dependence of various reaction rate coefficients for H photochemistry. Results for H near solar max will be compared for Solar Cycles 23 and 24.

  15. Transition Probabilities for Hydrogen-Like Atoms

    NASA Astrophysics Data System (ADS)

    Jitrik, Oliverio; Bunge, Carlos F.

    2004-12-01

    E1, M1, E2, M2, E3, and M3 transition probabilities for hydrogen-like atoms are calculated with point-nucleus Dirac eigenfunctions for Z=1-118 and up to large quantum numbers l=25 and n=26, increasing existing data more than a thousandfold. A critical evaluation of the accuracy shows a higher reliability with respect to previous works. Tables for hydrogen containing a subset of the results are given explicitly, listing the states involved in each transition, wavelength, term energies, statistical weights, transition probabilities, oscillator strengths, and line strengths. The complete results, including 1 863 574 distinct transition probabilities, lifetimes, and branching fractions are available at http://www.fisica.unam.mx/research/tables/spectra/1el

  16. Positron impact ionization of atomic hydrogen

    SciTech Connect

    Acacia, P.; Campeanu, R.I.; Horbatsch, M.

    1993-05-01

    We will present integrated cross sections for ionization of atomic hydrogen by positrons. These have been calculated in a distorted-wave approximation using energy-dependent effective charges in the final channel as well as static and polarization potentials in the initial channel. We present two models for calculating the energy-dependent effective charges both of which produce results in good agreement with the recent experimental measurements of Spicher et al. This is in contrast to previous distorted-wave calculations which used fixed effective charges as well as classical trajectory calculations. Both of these latter methods produced results which were substantially below ours and the experimental data.

  17. ATOMIC HYDROGEN IN A GALACTIC CENTER OUTFLOW

    SciTech Connect

    McClure-Griffiths, N. M.; Green, J. A.; Hill, A. S.; Lockman, F. J.; Dickey, J. M.; Gaensler, B. M.; Green, A. J.

    2013-06-10

    We describe a population of small, high-velocity, atomic hydrogen clouds, loops, and filaments found above and below the disk near the Galactic center. The objects have a mean radius of 15 pc, velocity widths of {approx}14 km s{sup -1}, and are observed at |z| heights up to 700 pc. The velocity distribution of the clouds shows no signature of Galactic rotation. We propose a scenario where the clouds are associated with an outflow from a central star-forming region at the Galactic center. We discuss the clouds as entrained material traveling at {approx}200 km s{sup -1} in a Galactic wind.

  18. Functionalization of Carbon Nanotubes using Atomic Hydrogen

    NASA Technical Reports Server (NTRS)

    Khare, Bishun N.; Cassell, Alan M.; Nguyen, Cattien V.; Meyyappan, M.; Han, Jie; Arnold, Jim (Technical Monitor)

    2001-01-01

    We have investigated the irradiation of multi walled and single walled carbon nanotubes (SWNTs) with atomic hydrogen. After irradiating the SWNT sample, a band at 2940/cm (3.4 microns) that is characteristic of the C-H stretching mode is observed using Fourier transform infrared (FTIR) spectroscopy. Additional confirmation of SWNT functionalization is tested by irradiating with atomic deuterium. A weak band in the region 1940/cm (5.2 micron) to 2450/cm (4.1 micron) corresponding to C-D stretching mode is also observed in the FTIR spectrum. This technique provides a clean gas phase process for the functionalization of SWNTs, which could lead to further chemical manipulation and/or the tuning of the electronic properties of SWNTs for nanodevice applications.

  19. Isotope effects of hydrogen and atom tunnelling

    NASA Astrophysics Data System (ADS)

    Buchachenko, A. L.; Pliss, E. M.

    2016-06-01

    The abnormally high mass-dependent isotope effects in liquid-phase hydrogen (deuterium) atom transfer reactions, which are customarily regarded as quantum effects, are actually the products of two classical effects, namely, kinetic and thermodynamic ones. The former is determined by the rate constants for atom transfer and the latter is caused by nonbonded (or noncovalent) isotope effects in the solvation of protiated and deuterated reacting molecules. This product can mimic the large isotope effects that are usually attributed to tunnelling. In enzymatic reactions, tunnelling is of particular interest; its existence characterizes an enzyme as a rigid molecular machine in which the residence time of reactants on the reaction coordinate exceeds the waiting time for the tunnelling event. The magnitude of isotope effect becomes a characteristic parameter of the internal dynamics of the enzyme catalytic site. The bibliography includes 61 references.

  20. Orientational and Translational Properties of Hydrogen Films Adsorbed onto Boron Nitride

    NASA Astrophysics Data System (ADS)

    Evans, Morgan David

    As physics continues to expand its knowledge base, physicists seek new frontiers to investigate. Quantum -mechanical, two-dimensional systems have proven to be a subject that is not only rich in new discoveries (e.g., Kousterlitz-Thoules transitions and new phases of matter), but also filled with exciting predictions (e.g., new superfluids). The physisorption of a gas onto the surface of a homogenous, spacious (on a molecular scale) substrate with a low adsorption potential is one physical analogue to the much-analyzed theoretical two-dimensional system. Hydrogen in reduced dimensions has been found to have suppressed melting and freezing points, thus possibly permitting the onset of Bose condensation and a new superfluid phase. The use of boron nitride as an adsorption substrate allows for the study of physisorbed systems with a lower adsorption potential than previous studies using similar substrates (i.e., graphite and magnesium oxide). This dissertation has two parts. The first concerns the translational properties and adsorption energies of hydrogen adsorbed onto boron nitride. These properties are investigated through the use of volumetric adsorption isotherm techniques. The data suggest that the adsorption of hydrogen occurs in a step-wise manner at temperatures below 20 Kelvin. Changes in the translational phases (vapor -liquid-solid) occur between 10 to 20 Kelvin for the first four adsorbed monolayers. Isotopic effects are investigated through the use of the three common forms of hydrogen: molecular hydrogen (H_2), deuterium hydride (HD), and deuterium (D_2). The critical temperatures of the second, third, and fourth layers are determined, presented, and compared with the known phase diagrams of hydrogen isotopes adsorbed onto graphite and MgO. While the adsorption potential of the hydrogen-boron nitride system is found to be less than that of previously studied substrates, it does not translate into lower critical temperatures. The second part of this

  1. Decontamination of adsorbed chemical warfare agents on activated carbon using hydrogen peroxide solutions.

    PubMed

    Osovsky, Ruth; Kaplan, Doron; Nir, Ido; Rotter, Hadar; Elisha, Shmuel; Columbus, Ishay

    2014-09-16

    Mild treatment with hydrogen peroxide solutions (3-30%) efficiently decomposes adsorbed chemical warfare agents (CWAs) on microporous activated carbons used in protective garments and air filters. Better than 95% decomposition of adsorbed sulfur mustard (HD), sarin, and VX was achieved at ambient temperatures within 1-24 h, depending on the H2O2 concentration. HD was oxidized to the nontoxic HD-sulfoxide. The nerve agents were perhydrolyzed to the respective nontoxic methylphosphonic acids. The relative rapidity of the oxidation and perhydrolysis under these conditions is attributed to the microenvironment of the micropores. Apparently, the reactions are favored due to basic sites on the carbon surface. Our findings suggest a potential environmentally friendly route for decontamination of adsorbed CWAs, using H2O2 without the need of cosolvents or activators.

  2. Decontamination of adsorbed chemical warfare agents on activated carbon using hydrogen peroxide solutions.

    PubMed

    Osovsky, Ruth; Kaplan, Doron; Nir, Ido; Rotter, Hadar; Elisha, Shmuel; Columbus, Ishay

    2014-09-16

    Mild treatment with hydrogen peroxide solutions (3-30%) efficiently decomposes adsorbed chemical warfare agents (CWAs) on microporous activated carbons used in protective garments and air filters. Better than 95% decomposition of adsorbed sulfur mustard (HD), sarin, and VX was achieved at ambient temperatures within 1-24 h, depending on the H2O2 concentration. HD was oxidized to the nontoxic HD-sulfoxide. The nerve agents were perhydrolyzed to the respective nontoxic methylphosphonic acids. The relative rapidity of the oxidation and perhydrolysis under these conditions is attributed to the microenvironment of the micropores. Apparently, the reactions are favored due to basic sites on the carbon surface. Our findings suggest a potential environmentally friendly route for decontamination of adsorbed CWAs, using H2O2 without the need of cosolvents or activators. PMID:25133545

  3. Hydrogen atom in a laser-plasma

    NASA Astrophysics Data System (ADS)

    Falaye, Babatunde J.; Sun, Guo-Hua; Liman, Muhammed S.; Oyewumi, K. J.; Dong, Shi-Hai

    2016-11-01

    We scrutinize the behaviour of the eigenvalues of a hydrogen atom in a quantum plasma as it interacts with an electric field directed along θ  =  π and is exposed to linearly polarized intense laser field radiation. We refer to the interaction of the plasma with the laser light as laser-plasma. Using the Kramers–Henneberger (KH) unitary transformation, which is the semiclassical counterpart of the Block–Nordsieck transformation in the quantized field formalism, the squared vector potential that appears in the equation of motion is eliminated and the resultant equation is expressed in the KH frame. Within this frame, the resulting potential and the corresponding wavefunction have been expanded in Fourier series, and using Ehlotzky’s approximation we obtain a laser-dressed potential to simulate an intense laser field. By fitting the exponential-cosine-screened Coulomb potential into the laser-dressed potential, and then expanding it in Taylor series up to O≤ft({{r}4},α 09\\right) , we obtain the eigensolution (eigenvalues and wavefunction) of the hydrogen atom in laser-plasma encircled by an electric field, within the framework of perturbation theory formalism. Our numerical results show that for a weak external electric field and a very large Debye screening parameter length, the system is strongly repulsive, in contrast with the case for a strong external electric field and a small Debye screening parameter length, when the system is very attractive. This work has potential applications in the areas of atomic and molecular processes in external fields, including interactions with strong fields and short pulses.

  4. Atomic hydrogen propellants: Historical perspectives and future possibilities

    NASA Astrophysics Data System (ADS)

    Palaszewski, Bryan

    1993-02-01

    Atomic hydrogen, a very high density free-radical propellant, is anticipated to generate a specific impulse of 600-1500 lb-f sec/lb-mass performance; this may facilitate the development of unique launch vehicles. A development status evaluation is presently given for atomic hydrogen investigations. It is noted that breakthroughs are required in the production, storage, and transfer of atomic hydrogen, before this fuel can become a viable rocket propellant.

  5. Atomic hydrogen propellants: Historical perspectives and future possibilities

    NASA Technical Reports Server (NTRS)

    Palaszewski, Bryan

    1993-01-01

    Atomic hydrogen, a very high density free-radical propellant, is anticipated to generate a specific impulse of 600-1500 lb-f sec/lb-mass performance; this may facilitate the development of unique launch vehicles. A development status evaluation is presently given for atomic hydrogen investigations. It is noted that breakthroughs are required in the production, storage, and transfer of atomic hydrogen, before this fuel can become a viable rocket propellant.

  6. In-Vacuum Dissociator for Atomic-Hydrogen Masers

    NASA Technical Reports Server (NTRS)

    Vessot, R. F.

    1987-01-01

    Thermal control and vacuum sealing achieved while contamination avoided. Simple, relatively inexpensive molecular-hydrogen dissociator for atomic-hydrogen masers used on Earth or in vacuum of space. No air cooling required, and absence of elastomeric O-ring seals prevents contamination. In-vacuum dissociator for atomic hydrogen masers, hydrogen gas in glass dissociator dissociated by radio-frequency signal transmitted from surrounding 3-turn coil. Heat in glass conducted away by contacting metal surfaces.

  7. Electronic Friction-Based Vibrational Lifetimes of Molecular Adsorbates: Beyond the Independent-Atom Approximation.

    PubMed

    Rittmeyer, Simon P; Meyer, Jörg; Juaristi, J Iñaki; Reuter, Karsten

    2015-07-24

    We assess the accuracy of vibrational damping rates of diatomic adsorbates on metal surfaces as calculated within the local-density friction approximation (LDFA). An atoms-in-molecules (AIM) type charge partitioning scheme accounts for intramolecular contributions and overcomes the systematic underestimation of the nonadiabatic losses obtained within the prevalent independent-atom approximation. The quantitative agreement obtained with theoretical and experimental benchmark data suggests the LDFA-AIM scheme as an efficient and reliable approach to account for electronic dissipation in ab initio molecular dynamics simulations of surface chemical reactions. PMID:26252696

  8. The gravitational analogue to the hydrogen atom

    NASA Astrophysics Data System (ADS)

    Kober, Martin; Koch, Ben; Bleicher, Marcus

    2007-05-01

    This paper reports on a student summer project performed in 2006 at the University of Frankfurt. It is addressed to undergraduate students familiar with the basic principles of relativistic quantum mechanics and general relativity. The aim of the project was to study the Dirac equation in curved spacetime. To obtain the general relativistic Dirac equation we use the formulation of gravity as a gauge theory in the first part. After these general considerations we restrict the further discussion to the special case of the Schwarzschild metric. This setting corresponds to the hydrogen atom, with the electromagnetic field replaced by gravity. Although there is a singularity at the event horizon it turns out that a regular solution of the time-independent Dirac equation exists. Finally the Dirac equation is solved numerically using suitable boundary conditions. A summer study at the borders of quantum mechanics and general relativity.

  9. Sequential desorption energy of hydrogen from nickel clusters

    SciTech Connect

    Deepika,; Kumar, Rakesh; R, Kamal Raj.; Kumar, T. J. Dhilip

    2015-06-24

    We report reversible Hydrogen adsorption on Nickel clusters, which act as a catalyst for solid state storage of Hydrogen on a substrate. First-principles technique is employed to investigate the maximum number of chemically adsorbed Hydrogen molecules on Nickel cluster. We observe a maximum of four Hydrogen molecules adsorbed per Nickel atom, but the average Hydrogen molecules adsorbed per Nickel atom decrease with cluster size. The dissociative chemisorption energy per Hydrogen molecule and sequential desorption energy per Hydrogen atom on Nickel cluster is found to decrease with number of adsorbed Hydrogen molecules, which on optimization may help in economical storage and regeneration of Hydrogen as a clean energy carrier.

  10. Atomic-scale control of graphene magnetism by using hydrogen atoms.

    PubMed

    González-Herrero, Héctor; Gómez-Rodríguez, José M; Mallet, Pierre; Moaied, Mohamed; Palacios, Juan José; Salgado, Carlos; Ugeda, Miguel M; Veuillen, Jean-Yves; Yndurain, Félix; Brihuega, Iván

    2016-04-22

    Isolated hydrogen atoms absorbed on graphene are predicted to induce magnetic moments. Here we demonstrate that the adsorption of a single hydrogen atom on graphene induces a magnetic moment characterized by a ~20-millielectron volt spin-split state at the Fermi energy. Our scanning tunneling microscopy (STM) experiments, complemented by first-principles calculations, show that such a spin-polarized state is essentially localized on the carbon sublattice opposite to the one where the hydrogen atom is chemisorbed. This atomically modulated spin texture, which extends several nanometers away from the hydrogen atom, drives the direct coupling between the magnetic moments at unusually long distances. By using the STM tip to manipulate hydrogen atoms with atomic precision, it is possible to tailor the magnetism of selected graphene regions.

  11. Quantitative analysis of hydrogen in SiO2/SiN/SiO2 stacks using atom probe tomography

    NASA Astrophysics Data System (ADS)

    Kunimune, Yorinobu; Shimada, Yasuhiro; Sakurai, Yusuke; Inoue, Masao; Nishida, Akio; Han, Bin; Tu, Yuan; Takamizawa, Hisashi; Shimizu, Yasuo; Inoue, Koji; Yano, Fumiko; Nagai, Yasuyoshi; Katayama, Toshiharu; Ide, Takashi

    2016-04-01

    We have demonstrated that it is possible to reproducibly quantify hydrogen concentration in the SiN layer of a SiO2/SiN/SiO2 (ONO) stack structure using ultraviolet laser-assisted atom probe tomography (APT). The concentration of hydrogen atoms detected using APT increased gradually during the analysis, which could be explained by the effect of hydrogen adsorption from residual gas in the vacuum chamber onto the specimen surface. The amount of adsorbed hydrogen in the SiN layer was estimated by analyzing another SiN layer with an extremely low hydrogen concentration (<0.2 at. %). Thus, by subtracting the concentration of adsorbed hydrogen, the actual hydrogen concentration in the SiN layer was quantified as approximately 1.0 at. %. This result was consistent with that obtained by elastic recoil detection analysis (ERDA), which confirmed the accuracy of the APT quantification. The present results indicate that APT enables the imaging of the three-dimensional distribution of hydrogen atoms in actual devices at a sub-nanometer scale.

  12. Chiral modification of platinum by co-adsorbed cinchonidine and trifluoroacetic acid: origin of enhanced stereocontrol in the hydrogenation of trifluoroacetophenone.

    PubMed

    Meemken, Fabian; Baiker, Alfons; Schenker, Sebastian; Hungerbühler, Konrad

    2014-01-27

    Cinchonidine (CD) adsorbed onto a platinum metal catalyst leads to rate acceleration and induces strong stereocontrol in the asymmetric hydrogenation of trifluoroacetophenone. Addition of catalytic amounts of trifluoroacetic acid (TFA) significantly enhances the enantiomeric excess from 50 to 92%. The origin of the enantioselectivity bestowed by co-adsorbed CD and TFA is investigated by using in situ attenuated total reflection infrared spectroscopy and modulation excitation spectroscopy. Molecular interactions between the chiral modifier (CD), acid additive (TFA) and the trifluoro-activated substrate at the solid-liquid interface are elucidated under conditions relevant to catalytic hydrogenations, that is, on a technical Pt/Al2O3 catalyst in the presence of H2 and solvent. Monitoring of the unmodified and modified surface during the hydrogenation provides an insight into the phenomenon of rate enhancement and the crucial interactions of CD with the ketone, corresponding product alcohol, and TFA. Comparison of the diastereomeric interactions occurring on the modified surface and in the liquid solution shows a striking difference for the chiral preferences of CD. The spectroscopic data, in combination with calculations of molecular structures and energies, sheds light on the reaction mechanism of the heterogeneous asymmetric hydrogenation of trifluoromethyl ketones and the involvement of TFA in the diastereomeric intermediate surface complex: the quinuclidine N atom of the adsorbed CD forms an N-H-O-type hydrogen-bonding interaction not only with the trifluoro-activated ketone but also with the corresponding alcohol and the acid additive. Strong evidence is provided that it is a monodentate acid/base adduct in which the carboxylate of TFA resides at the quinuclidine N-atom of CD, which imparts a better stereochemical control.

  13. Organic silicon compounds anf hydrogen sulfide removal from biogas by mineral and adsorbent

    NASA Astrophysics Data System (ADS)

    Choi, J.

    2015-12-01

    Biogas utilized for energy production needs to be free from organic silicon compounds and hydrogen sulfide , as their burning has damaging effects on utilities and humans; organic silicon compounds and hydrogen sulfide can be found in biogas produced from biomass wastes, due to their massive industrial use in synthetic product,such as cosmetics, detergents and paints.Siloxanes and hydrogen sulfide removal from biogas can be carried out by various methods (Ajhar et al., 2010); aim of the present work is to find a single practical andeconomic way to drastically and simultaneously reduce both hydrogen sulfide and the siloxanes concentration to less than 1 ppm. Some commercial activated carbons previously selected (Monteleoneet al., 2011) as being effective in hydrogen sulfide up taking have been tested in an adsorption measurement apparatus, by flowing both hydrogen sulphide and volatile siloxane (Decamethycyclopentasiloxane or D5) in a nitrogen stream,typically 25-300 ppm D5 over N2, through an clay minerals, Fe oxides and Silica; the adsorption process was analyzed by varying some experimental parameters (concentration, grain size, bed height). The best silica shows an adsorption capacity of 0.2 g D5 per gram of silica. The next thermo gravimetric analysis (TGA) confirms the capacity data obtained experimentally by the breakthrough curve tests.The capacity results depend on D5 and hydrogen sulphide concentrations. A regenerative silica process is then carried out byheating the silica bed up to 200 ° C and flushing out the adsorbed D5 and hydrogen sulphide samples in a nitrogen stream in athree step heating procedure up to 200 ° C. The adsorption capacity is observed to degrade after cyclingthe samples through several adsorption-desorption cycles.

  14. Hirshfeld atom refinement for modelling strong hydrogen bonds.

    PubMed

    Woińska, Magdalena; Jayatilaka, Dylan; Spackman, Mark A; Edwards, Alison J; Dominiak, Paulina M; Woźniak, Krzysztof; Nishibori, Eiji; Sugimoto, Kunihisa; Grabowsky, Simon

    2014-09-01

    High-resolution low-temperature synchrotron X-ray diffraction data of the salt L-phenylalaninium hydrogen maleate are used to test the new automated iterative Hirshfeld atom refinement (HAR) procedure for the modelling of strong hydrogen bonds. The HAR models used present the first examples of Z' > 1 treatments in the framework of wavefunction-based refinement methods. L-Phenylalaninium hydrogen maleate exhibits several hydrogen bonds in its crystal structure, of which the shortest and the most challenging to model is the O-H...O intramolecular hydrogen bond present in the hydrogen maleate anion (O...O distance is about 2.41 Å). In particular, the reconstruction of the electron density in the hydrogen maleate moiety and the determination of hydrogen-atom properties [positions, bond distances and anisotropic displacement parameters (ADPs)] are the focus of the study. For comparison to the HAR results, different spherical (independent atom model, IAM) and aspherical (free multipole model, MM; transferable aspherical atom model, TAAM) X-ray refinement techniques as well as results from a low-temperature neutron-diffraction experiment are employed. Hydrogen-atom ADPs are furthermore compared to those derived from a TLS/rigid-body (SHADE) treatment of the X-ray structures. The reference neutron-diffraction experiment reveals a truly symmetric hydrogen bond in the hydrogen maleate anion. Only with HAR is it possible to freely refine hydrogen-atom positions and ADPs from the X-ray data, which leads to the best electron-density model and the closest agreement with the structural parameters derived from the neutron-diffraction experiment, e.g. the symmetric hydrogen position can be reproduced. The multipole-based refinement techniques (MM and TAAM) yield slightly asymmetric positions, whereas the IAM yields a significantly asymmetric position.

  15. Quantum Sticking of Atomic Hydrogen to Graphene

    NASA Astrophysics Data System (ADS)

    Zhang, Yanting; Doherty, Adam; Geragotelis, Andrew; Clougherty, Dennis

    2013-03-01

    We consider the low-energy behavior of the sticking probability of atomic hydrogen to suspended graphene. For energy transfer through the flexural modes of graphene, we find that the inelastic coupling falls in the subOhmic regime. Thus the effects of low-frequency fluctuations of the graphene sheet are crucially important for quantum sticking. We analytically solve for the low-energy asymptotic behavior of the sticking coefficient using a variational mean-field method [D.P. Clougherty and Y. Zhang, Phys. Rev. Lett. 109, 120401 (2012)]. We find that as a result of strong coupling to the low-frequency flexural modes of graphene, a new scaling law results. For suspended graphene at finite temperature, we find that at a critical incident energy, the sticking probability drops discontinuously; below this critical energy, the sticking probability is suppressed by the orthogonality catastrophe. We compare our nonperturbative variational results to those obtained by using Fermi's golden rule. We gratefully acknowledge support by the National Science Foundation under DMR-1062966.

  16. The one-dimensional hydrogen atom revisited

    NASA Astrophysics Data System (ADS)

    Palma, G.; Raff, U.

    2006-09-01

    The one-dimensional Schrodinger hydrogen atom is an interesting mathematical and physical problem for the study of bound states, eigenfunctions, and quantum-degeneracy issues. This one-dimensional physical system has given rise to some intriguing controversy for more than four decades. Presently, still no definite consensus seems to have been reached. We reanalyzed this apparently controversial problem, approaching it from a Fourier-transform representation method combined with some fundamental (basic) ideas found in self-adjoint extensions of symmetric operators. In disagreement with some previous claims, we found that the complete Balmer energy spectrum is obtained together with an odd-parity set of eigenfunctions. Closed-form solutions in both coordinate and momentum spaces were obtained. No twofold degeneracy was observed as predicted by the degeneracy theorem in one dimension, though it does not necessarily have to hold for potentials with singularities. No ground state with infinite energy exists since the corresponding eigenfunction does not satisfy the Schrodinger equation at the origin.

  17. Hydrogenation of olefin adsorbed on Pt/SiO/sub 2/

    SciTech Connect

    Kawai, T.; Burwell, R.L. Jr.

    1986-11-01

    Cyclopentene and cyclooctene have been hydrogenated in a batch reactor on supported platinum catalysts at temperatures such that over 99.99% of the olefin was in the adsorbed state and primarily on the support. Reaction temperatures were -75/sup 0/C for cyclopentene and -22/sup 0/C for cyclooctene and P(H/sub 2/) was usually 100 Torr. At coverages of one molecule of cyclopentene per nm/sub 2/ on Pt/(wide pore silica gel), the rate was zero order in olefin up to a conversion of about 70% following which the rate declined. The rate was about one-half order in hydrogen. Pt/alumina and Pt/silica gel gave similar results. Transport of olefin from the surface of the support to crystallites of platinum occurred primarily by surface migration rather than through the vapor phase. Significant contribution to hydrogenation by hydrogen spillover from platinum to silica can be excluded. Small particles of platinum on silica gel gave somewhat larger values of turnover frequency, N/sub t/, than did larger particles, at least after the pretreatment O/sub 2/, 300/sup 0/C; He, 450/sup 0/C; cool in He. N/sub t/ for cyclopentene was roughly equal to that for propylene in conventional vapor phase hydrogenation extrapolated to -75/sup 0/C.

  18. Effects of hydrogen atoms on surface conductivity of diamond film

    SciTech Connect

    Liu, Fengbin Cui, Yan; Qu, Min; Di, Jiejian

    2015-04-15

    To investigate the effects of surface chemisorbed hydrogen atoms and hydrogen atoms in the subsurface region of diamond on surface conductivity, models of hydrogen atoms chemisorbed on diamond with (100) orientation and various concentrations of hydrogen atoms in the subsurface layer of the diamond were built. By using the first-principles method based on density functional theory, the equilibrium geometries and densities of states of the models were studied. The results showed that the surface chemisorbed hydrogen alone could not induce high surface conductivity. In addition, isolated hydrogen atoms in the subsurface layer of the diamond prefer to exist at the bond centre site of the C-C bond. However, such a structure would induce deep localized states, which could not improve the surface conductivity. When the hydrogen concentration increases, the C-H-C-H structure and C-3H{sub bc}-C structure in the subsurface region are more stable than other configurations. The former is not beneficial to the increase of the surface conductivity. However, the latter would induce strong surface states near the Fermi level, which would give rise to high surface conductivity. Thus, a high concentration of subsurface hydrogen atoms in diamond would make significant contributions to surface conductivity.

  19. Surface characterization of silica glass substrates treated by atomic hydrogen

    SciTech Connect

    Inoue, Hiroyuki; Masuno, Atsunobu; Ishibashi, Keiji; Tawarayama, Hiromasa; Zhang, Yingjiu; Utsuno, Futoshi; Koya, Kazuo; Fujinoki, Akira; Kawazoe, Hiroshi

    2013-12-15

    Silica glass substrates with very flat surfaces were exposed to atomic hydrogen at different temperatures and durations. An atomic force microscope was used to measure root-mean-square (RMS) roughness and two-dimensional power spectral density (PSD). In the treatment with atomic hydrogen up to 900 °C, there was no significant change in the surface. By the treatment at 1000 °C, the changes in the RMS roughness and the PSD curves were observed. It was suggested that these changes were caused by etching due to reactions of atomic hydrogen with surface silica. By analysis based on the k-correlation model, it was found that the spatial frequency of the asperities became higher with an increase of the treatment time. Furthermore, the data showed that atomic hydrogen can flatten silica glass surfaces by controlling heat-treatment conditions. - Highlights: • Silica glass surface was treated by atomic hydrogen at various temperatures. • Surface roughness was measured by an atomic force microscope. • Roughness data were analyzed by two-dimensional power spectral density. • Atomic hydrogen can flatten silica glass surfaces.

  20. Measurement of Fatigue Crack Growth Relationships in Hydrogen Gas for Pressure Swing Adsorber Vessel Steels

    SciTech Connect

    Somerday, Brian P.; Barney, Monica

    2014-12-04

    We measured the hydrogen-assisted fatigue crack growth rates (da/dN) for SA516 Grade 70 steel as a function of stress-intensity factor range (ΔK) and load-cycle frequency to provide life-prediction data relevant to pressure swing adsorber (PSA) vessels. For ΔK values up to 18.5 MPa m1/2, the baseline da/dN versus ΔK relationship measured at 1Hz in 2.8 MPa hydrogen gas represents an upper bound with respect to crack growth rates measured at lower frequency. However, at higher ΔK values, we found that the baseline da/dN data had to be corrected to account for modestly higher crack growth rates at the lower frequencies relevant to PSA vessel operation.

  1. Measurement of Fatigue Crack Growth Relationships in Hydrogen Gas for Pressure Swing Adsorber Vessel Steels

    DOE PAGES

    Somerday, Brian P.; Barney, Monica

    2014-12-04

    We measured the hydrogen-assisted fatigue crack growth rates (da/dN) for SA516 Grade 70 steel as a function of stress-intensity factor range (ΔK) and load-cycle frequency to provide life-prediction data relevant to pressure swing adsorber (PSA) vessels. For ΔK values up to 18.5 MPa m1/2, the baseline da/dN versus ΔK relationship measured at 1Hz in 2.8 MPa hydrogen gas represents an upper bound with respect to crack growth rates measured at lower frequency. However, at higher ΔK values, we found that the baseline da/dN data had to be corrected to account for modestly higher crack growth rates at the lower frequenciesmore » relevant to PSA vessel operation.« less

  2. Atomic force microscopy of AgBr crystals and adsorbed gelatin films

    SciTech Connect

    Haugstad, G.; Gladfelter, W.L.; Keyes, M.P.; Weberg, E.B.

    1993-06-01

    Atomic force microscopy of the (111) surface of macroscopic AgBr crystals revealed steps ranging in height from two atomic layers up to 10 nm, lying predominantly along the (110) and (112) families of crystal directions. Rods of elemental Ag, formed via photoreduction, were observed along the (110) family of directions. Images of adsorbed gelatin films revealed circular pores with diameters of order 10-100 nm, extending to the AgBr surface. The length of deposition time, the pH and concentration of the gelatin solution, and the presence of steps on the AgBr surface were observed to affect the size, number, and location of pores in the gelatin films. 12 refs., 7 figs.

  3. Atomic hydrogen adsorption on lithium-doped graphite surfaces

    SciTech Connect

    Allouche, Alain

    2012-01-01

    The effects of lithium doping of pristine and defective graphite surfaces on hydrogen adsorption are studied by the first-principles Plane-Wave Density Functional Theory. The surface defects are simulated by a single atomic vacancy. The DFT calculation is corrected for long-range effects through semi-empirical London terms for each constituent of the system. The lithium doping of the graphite surfaces notably reinforces hydrogen atom binding. Qualitative comparison with experimental results is given using the lithium 1s energy level shifts induced by the atomic vacancy and/or hydrogen trapping.

  4. Quantum states of hydrogen atom on Pd(1 1 0) surface

    NASA Astrophysics Data System (ADS)

    Padama, Allan Abraham B.; Nakanishi, Hiroshi; Kasai, Hideaki

    2015-12-01

    The quantum states of adsorbed hydrogen atom on Pd(1 1 0) surface are investigated in this work. From the calculated potential energy surface (PES) of hydrogen atom on Pd(1 1 0), the wave functions and eigenenergies in the ground and few excited states of protium (H) and deuterium (D) are calculated. Localized wave functions of hydrogen atom exist on pseudo-threefold and long bridge sites of Pd(1 1 0). The short bridge site is a local minimum from the result of PES, however, quantum behavior of hydrogen revealed that its vibration would allow it to hop to other pseudo-threefold site (that crosses the short bridge site) than to stay on the short bridge site. Exchange of ordering of the wave functions between H and D is attributed to the difference in their masses. The calculated eigenenergies are found to be in fair agreement with experimental data based from the identified vibrations of hydrogen with component perpendicular to the surface. The activation barriers measured from the eigenenergies are in better agreement with experimental findings in comparison to the data gathered from PES.

  5. Kinetics, mechanism, and dynamics of the gas-phase H(D) atom reaction with adsorbed D(H) atom on Pt(111)

    NASA Astrophysics Data System (ADS)

    Kim, Jae-Young; Lee, Jihwa

    2000-08-01

    We have investigated the kinetics of the abstraction reaction H(D)+Dad(Had)/Pt(111) at 100 K and saturation coverage (θsat=0.95±0.06 ML) using an H(D) atom beam, in which the angle-integrated and angle-resolved product desorption rates were simultaneously monitored with two mass spectrometers. HD molecules are formed by the abstraction reaction as well as by the secondary hot atom (s-HA) reactions, Ds*(Hs*)+Had(Dad)→HD, where Ds*(Hs*) is a collisionally excited surface D(H) atom. The two reaction components of HD show quite distinct angular distributions; while the former component is sharply forward-peaked to be represented by cos12(θf-3°), the latter component preferentially desorbs at large desorption angles centered at θf˜45°. The two HD formation reactions also exhibit distinct kinetics, which could be separately identified by properly selecting the desorption angle. Concurrent desorption of D2(H2) formed by a homonuclear s-HA reaction was also observed with a relatively large yield amounting to 37%(31%) of the initially adsorbed D(H) atoms. The angular distribution of D2 is very similar to that of HD formed by the s-HA reactions. Varying the beam incidence angle has no effect on the reaction rate constants and the product branching ratio. From a kinetic analysis, we estimate a cross section σabst=1.30±0.07(1.49±0.11) Å2 for HD formation by abstraction in H(D)-on-Dad(Had) reaction. For D2(H2) formation, an effective cross section for generating reactive Ds*(Hs*) atom is estimated as σ*=1.87±0.08(1.61±0.24) Å2. These values can be translated into the probabilities Pabst=0.19(0.21), Pex=0.27(0.23), Pads=0.73(0.67), and Pscatt=0.08(0.12) for abstraction reaction, s-HA generation, adsorption, and scattering of an incident H(D) atom, respectively. The isotope effects are small and the corresponding cross sections differ at most by 15%. The mechanism-dependent product angular distributions are discussed in terms of the different reaction dynamics

  6. Atomic hydrogen and nitrogen distributions from atmosphere explorer measurements

    NASA Technical Reports Server (NTRS)

    Breig, Edward L.

    1992-01-01

    We were selective as to our approach to research activities, and devoted primary attention to two investigations concerning the global behavior of atomic hydrogen in the Earth's upper atmosphere. We derive the thermospheric concentration of H by applying the condition of charge-exchange equilibrium between hydrogen and oxygen atoms and ions to in-situ measurements of F-region composition and temperature from the series of Atmosphere Explorer (AE) aeronomy satellites. Progress and accomplishments on these chosen research projects are summarized.

  7. Muon transfer from hot muonic hydrogen atoms to neon

    SciTech Connect

    Jacot-Guillarmod, R. . Inst. de Physique); Bailey, J.M. ); Beer, G.A.; Knowles, P.E.; Mason, G.R.; Olin, A. ); Beveridge, J.L.; Marshall, G.M.; Brewer, J.H.; Forster, B.M. ); Huber, T.M. ); Kammel, P.; Zmeskal, J.

    1992-01-01

    A negative muon beam has been directed on adjacent solid layers of hydrogen and neon. Three targets differing by their deuterium concentration were investigated. Muonic hydrogen atoms can drift to the neon layer where the muon is immediately transferred. The time structure of the muonic neon X-rays follows the exponential law with a disappearance rate corresponding to the one of [mu][sup [minus]p] atoms in each target. The rates [lambda][sub pp[mu

  8. Efficient epoxidation of a terminal alkene containing allylic hydrogen atoms: trans-methylstyrene on Cu{111}.

    PubMed

    Cropley, Rachael L; Williams, Federico J; Urquhart, Andrew J; Vaughan, Owain P H; Tikhov, Mintcho S; Lambert, Richard M

    2005-04-27

    The selective oxidation of trans-methylstyrene, a phenyl-substituted propene that contains labile allylic hydrogen atoms, has been studied on Cu{111}. Mass spectrometry and synchrotron fast XPS were used to detect, respectively, desorbing gaseous products and the evolution of surface species as a function of temperature and time. Efficient partial oxidation occurs yielding principally the epoxide, and the behavior of the system is sensitive to the order in which reactants are adsorbed. The latter is understandable in terms of differences in the spatial distribution of oxygen adatoms; isolated adatoms lead to epoxidation, while islands of "oxidic" oxygen do not. NEXAFS data taken over a range of coverages and in the presence and absence of coadsorbed oxygen indicate that the adsorbed alkene lies essentially flat with the allylic hydrogen atoms close to the surface. The photoemission results and comparison with the corresponding behavior of styrene on Cu{111} strongly suggest that allylic hydrogen abstraction is indeed a critical factor that limits epoxidation selectivity. An overall mechanism consistent with the structural and reactive properties is proposed.

  9. Ultra-cold methods for polarized atomic hydrogen

    SciTech Connect

    Luppov, V. G.; Arnold, J. D.; Blinov, B. B.; Gladycheva, S. E.; Krisch, A. D.; Lin, A. M. T.; Raymond, R. S.; Bychkov, M. A.; Fimushkin, V. V.; Mochalov, V. V.; Semenov, P. A.

    1998-01-20

    Using the ultra-cold electron-spin-polarized atomic hydrogen technique, one can produce a slow monochromatic beam for use as a polarized jet target. We will first review the development of the ultra-cold technique and then discuss the recent progress on Michigan's Mark-II ultra-cold proton-spin-polarized hydrogen jet target.

  10. Topics in atomic hydrogen standard research and applications

    NASA Technical Reports Server (NTRS)

    Peters, H. E.

    1971-01-01

    Hydrogen maser based frequency and time standards have been in continuous use at NASA tracking stations since February 1970, while laboratory work at Goddard has continued in the further development and improvement of hydrogen masers. Concurrently, experimental work has been in progress with a new frequency standard based upon the hydrogen atom using the molecular beam magnetic resonance method. Much of the hydrogen maser technology is directly applicable to the new hydrogen beam standard, and calculations based upon realistic data indicate that the accuracy potential of the hydrogen atomic beam exceeds that of either the cesium beam tube or the hydrogen maser, possibly by several orders of magnitude. In addition, with successful development, the hydrogen beam standard will have several other performance advantages over other devices, particularly exceptional stability and long continuous operating life. Experimental work with a new laboratory hydrogen beam device has recently resulted in the first resonance transition curves, measurements of relative state populations, beam intensities, etc. The most important aspects of both the hydrogen maser and the hydrogen beam work are covered.

  11. Absolute frequency of an atomic hydrogen maser clock

    NASA Technical Reports Server (NTRS)

    Peters, H. E.; Hall, R. G.; Percival, D. B.

    1972-01-01

    An accurate determination was made of the unperturbed atomic hydrogen ground state hyperfine transition frequency (F=1,m=0 - F=0,m=0) in reference to present world wide realizations of internationally defined time interval. In relation to the international atomic time system, the composite value is 1,420,405,751.7755 plus or minus 0.0031 HZ.

  12. Cooperation between adsorbates accounts for the activation of atomic layer deposition reactions.

    PubMed

    Shirazi, Mahdi; Elliott, Simon D

    2015-04-14

    Atomic layer deposition (ALD) is a technique for producing conformal layers of nanometre-scale thickness, used commercially in non-planar electronics and increasingly in other high-tech industries. ALD depends on self-limiting surface chemistry but the mechanistic reasons for this are not understood in detail. Here we demonstrate, by first-principle calculations of growth of HfO2 from Hf(N(CH3)2)4-H2O and HfCl4-H2O and growth of Al2O3 from Al(CH3)3-H2O, that, for all these precursors, co-adsorption plays an important role in ALD. By this we mean that previously-inert adsorbed fragments can become reactive once sufficient numbers of molecules adsorb in their neighbourhood during either precursor pulse. Through the calculated activation energies, this 'cooperative' mechanism is shown to have a profound influence on proton transfer and ligand desorption, which are crucial steps in the ALD cycle. Depletion of reactive species and increasing coordination cause these reactions to self-limit during one precursor pulse, but to be re-activated via the cooperative effect in the next pulse. This explains the self-limiting nature of ALD.

  13. Energetics of a Li Atom adsorbed on B/N doped graphene with monovacancy

    NASA Astrophysics Data System (ADS)

    Rani, Babita; Jindal, V. K.; Dharamvir, Keya

    2016-08-01

    We use density functional theory (DFT) to study the adsorption properties and diffusion of Li atom across B/N-pyridinic graphene. Regardless of the dopant type, B atoms of B-pyridinic graphene lose electron density. On the other hand, N atoms (p-type dopants) have tendency to gain electron density in N-pyridinic graphene. Higher chemical reactivity and electronic conductivity of B/N-pyridinic graphene are responsible for stronger binding of Li with the substrates as compared to pristine graphene. The binding energy of Li with B/N-pyridinic graphene exceeds the cohesive energy of bulk Li, making it energetically unfavourable for Li to form clusters on these substrates. Li atom gets better adsorbed on N-pyridinic graphene due to an additional p-p hybridization of the orbitals while Li on B-pyridinic prefers the ionic bonding. Also, significant distortion of N-pyridinic graphene upon Li adsorption is a consequence of the change in bonding mechanism between Li atom and the substrate. Our results show that bonding character and hence binding energies between Li and graphene can be tuned with the help of B/N doping of monovacancy defects. Further, the sites for most stable adsorption are different for the two types of doped and defective graphene, leading to greater Li uptake capacity of B-pyridinic graphene near the defect. In addition, B-pyridinic graphene offering lower diffusion barrier, ensures better Li kinetics. Thus, B-pyridinic graphene presents itself as a better anode material for LIBs as compared to N-pyridinic graphene.

  14. Quantitative analysis of desorption and decomposition kinetics of formic acid on Cu(111): The importance of hydrogen bonding between adsorbed species

    SciTech Connect

    Shiozawa, Yuichiro; Koitaya, Takanori; Mukai, Kozo; Yoshimoto, Shinya; Yoshinobu, Jun

    2015-12-21

    Quantitative analysis of desorption and decomposition kinetics of formic acid (HCOOH) on Cu(111) was performed by temperature programmed desorption (TPD), X-ray photoelectron spectroscopy, and time-resolved infrared reflection absorption spectroscopy. The activation energy for desorption is estimated to be 53–75 kJ/mol by the threshold TPD method as a function of coverage. Vibrational spectra of the first layer HCOOH at 155.3 K show that adsorbed molecules form a polymeric structure via the hydrogen bonding network. Adsorbed HCOOH molecules are dissociated gradually into monodentate formate species. The activation energy for the dissociation into monodentate formate species is estimated to be 65.0 kJ/mol at a submonolayer coverage (0.26 molecules/surface Cu atom). The hydrogen bonding between adsorbed HCOOH species plays an important role in the stabilization of HCOOH on Cu(111). The monodentate formate species are stabilized at higher coverages, because of the lack of vacant sites for the bidentate formation.

  15. Quantitative analysis of desorption and decomposition kinetics of formic acid on Cu(111): The importance of hydrogen bonding between adsorbed species

    NASA Astrophysics Data System (ADS)

    Shiozawa, Yuichiro; Koitaya, Takanori; Mukai, Kozo; Yoshimoto, Shinya; Yoshinobu, Jun

    2015-12-01

    Quantitative analysis of desorption and decomposition kinetics of formic acid (HCOOH) on Cu(111) was performed by temperature programmed desorption (TPD), X-ray photoelectron spectroscopy, and time-resolved infrared reflection absorption spectroscopy. The activation energy for desorption is estimated to be 53-75 kJ/mol by the threshold TPD method as a function of coverage. Vibrational spectra of the first layer HCOOH at 155.3 K show that adsorbed molecules form a polymeric structure via the hydrogen bonding network. Adsorbed HCOOH molecules are dissociated gradually into monodentate formate species. The activation energy for the dissociation into monodentate formate species is estimated to be 65.0 kJ/mol at a submonolayer coverage (0.26 molecules/surface Cu atom). The hydrogen bonding between adsorbed HCOOH species plays an important role in the stabilization of HCOOH on Cu(111). The monodentate formate species are stabilized at higher coverages, because of the lack of vacant sites for the bidentate formation.

  16. Quantum chemical investigation on the role of Li adsorbed on anatase (101) surface nano-materials on the storage of molecular hydrogen.

    PubMed

    Srinivasadesikan, V; Raghunath, P; Lin, M C

    2015-06-01

    Lithiation of TiO2 has been shown to enhance the storage of hydrogen up to 5.6 wt% (Hu et al. J Am Chem Soc 128:11740-11741, 2006). The mechanism for the process is still unknown. In this work we have carried out a study on the adsorption and diffusion of Li atoms on the surface and migration into subsurface layers of anatase (101) by periodic density functional theory calculations implementing on-site Coulomb interactions (DFT+U). The model consists of 24 [TiO2] units with 11.097 × 7.655 Å(2) surface area. Adsorption energies have been calculated for different Li atoms (1-14) on the surface. A maximum of 13 Li atoms can be accommodated on the surface at two bridged O, Ti-O, and Ti atom adsorption sites, with 83 kcal mol(-1) adsorption energy for a single Li atom adsorbed between two bridged O atoms from where it can migrate into the subsurface layer with 27 kcal mol(-1) energy barrier. The predicted adsorption energies for H2 on the lithiated TiO2 (101) surface with 1-10 Li atoms revealed that the highest adsorption energies occurred on 1-Li, 5-Li, and 9-Li surfaces with 3.5, 4.4, and 7.6 kcal mol(-1), respectively. The values decrease rapidly with additional H2 co-adsorbed on the lithiated surfaces; the maximum H2 adsorption on the 9Li-TiO2(a) surface was estimated to be only 0.32 wt% under 100 atm H2 pressure at 77 K. The result of Bader charge analysis indicated that the reduction of Ti occurred depending on the Li atoms covered on the TiO2 surface.

  17. Concerted hydrogen atom exchange between three HF molecules

    NASA Technical Reports Server (NTRS)

    Komornicki, Andrew; Dixon, David A.; Taylor, Peter R.

    1992-01-01

    The termolecular reaction involving concerted hydrogen-atom exchange between three HF molecules was investigated with particular attention given to the effects of correlation at the various stationary points along the reaction. Using large segmented Gaussian basis sets to locate the (HF)3 stationary points at the SCF level, the geometries of the stable hydrogen-bonded trimer, which is of C(3h) symmetry, were located, together with the transition state for hydrogen exchange, which is of D(3h) symmetry. Then, using a large atomic natural orbital basis and correlating all valence electrons, the energetics of the exchange reaction were evaluated at the correlated level.

  18. Self-assembly of acetate adsorbates drives atomic rearrangement on the Au(110) surface

    PubMed Central

    Hiebel, Fanny; Shong, Bonggeun; Chen, Wei; Madix, Robert J.; Kaxiras, Efthimios; Friend, Cynthia M.

    2016-01-01

    Weak inter-adsorbate interactions are shown to play a crucial role in determining surface structure, with major implications for its catalytic reactivity. This is exemplified here in the case of acetate bound to Au(110), where the small extra energy of the van der Waals interactions among the surface-bound groups drives massive restructuring of the underlying Au. Acetate is a key intermediate in electro-oxidation of CO2 and a poison in partial oxidation reactions. Metal atom migration originates at surface defects and is likely facilitated by weakened Au–Au interactions due to bonding with the acetate. Even though the acetate is a relatively small molecule, weak intermolecular interaction provides the energy required for molecular self-assembly and reorganization of the metal surface. PMID:27731407

  19. Self-assembly of acetate adsorbates drives atomic rearrangement on the Au(110) surface

    NASA Astrophysics Data System (ADS)

    Hiebel, Fanny; Shong, Bonggeun; Chen, Wei; Madix, Robert J.; Kaxiras, Efthimios; Friend, Cynthia M.

    2016-10-01

    Weak inter-adsorbate interactions are shown to play a crucial role in determining surface structure, with major implications for its catalytic reactivity. This is exemplified here in the case of acetate bound to Au(110), where the small extra energy of the van der Waals interactions among the surface-bound groups drives massive restructuring of the underlying Au. Acetate is a key intermediate in electro-oxidation of CO2 and a poison in partial oxidation reactions. Metal atom migration originates at surface defects and is likely facilitated by weakened Au-Au interactions due to bonding with the acetate. Even though the acetate is a relatively small molecule, weak intermolecular interaction provides the energy required for molecular self-assembly and reorganization of the metal surface.

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

    SciTech Connect

    López-Moreno, S.; Romero, A. H.

    2015-04-21

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

  1. Selective adsorption of atomic hydrogen on a h-BN thin film

    SciTech Connect

    Koswattage, Kaveenga Rasika; Shimoyama, Iwao; Baba, Yuji; Sekiguchi, Tetsuhiro; Nakagawa, Kazumichi

    2011-07-07

    The adsorption of atomic hydrogen on hexagonal boron nitride (h-BN) is studied using two element-specific spectroscopies, i.e., near-edge x-ray absorption fine structure (NEXAFS) spectroscopy and x-ray photoelectron spectroscopy (XPS). B K-edge NEXAFS spectra show a clear change in the energy region of the {pi}{sup *} band before and after reaction with atomic deuterium. On the other hand, N K-edge NEXAFS spectra show only a little change. B 1s XPS spectra show a distinct component at the low binding energy side of a main component, while N 1s XPS spectra show peak broadening at the high binding energy side. These experimental results are analyzed by the discrete variational X{alpha} method with a core-hole effect and are explained by a model in which hydrogen atoms are preferentially adsorbed on the B sites of h-BN. Based on the experimental and theoretical results, we propose a site-selective property of BN material on adsorption of atomic hydrogen.

  2. Selective adsorption of atomic hydrogen on a h-BN thin film.

    PubMed

    Koswattage, Kaveenga Rasika; Shimoyama, Iwao; Baba, Yuji; Sekiguchi, Tetsuhiro; Nakagawa, Kazumichi

    2011-07-01

    The adsorption of atomic hydrogen on hexagonal boron nitride (h-BN) is studied using two element-specific spectroscopies, i.e., near-edge x-ray absorption fine structure (NEXAFS) spectroscopy and x-ray photoelectron spectroscopy (XPS). B K-edge NEXAFS spectra show a clear change in the energy region of the π* band before and after reaction with atomic deuterium. On the other hand, N K-edge NEXAFS spectra show only a little change. B 1s XPS spectra show a distinct component at the low binding energy side of a main component, while N 1s XPS spectra show peak broadening at the high binding energy side. These experimental results are analyzed by the discrete variational Xα method with a core-hole effect and are explained by a model in which hydrogen atoms are preferentially adsorbed on the B sites of h-BN. Based on the experimental and theoretical results, we propose a site-selective property of BN material on adsorption of atomic hydrogen. PMID:21744913

  3. Spin-polarized hydrogen adsorbed on the surface of superfluid {sup 4}He

    SciTech Connect

    Marín, J. M.; Boronat, J.; Markić, L. Vranješ

    2013-12-14

    The experimental realization of a thin layer of spin-polarized hydrogen H↓ adsorbed on top of the surface of superfluid {sup 4}He provides one of the best examples of a stable, nearly two-dimensional (2D) quantum Bose gas. We report a theoretical study of this system using quantum Monte Carlo methods in the limit of zero temperature. Using the full Hamiltonian of the system, composed of a superfluid {sup 4}He slab and the adsorbed H↓ layer, we calculate the main properties of its ground state using accurate models for the pair interatomic potentials. Comparing the results for the layer with the ones obtained for a strictly 2D setup, we analyze the departure from the 2D character when the density increases. Only when the coverage is rather small the use of a purely 2D model is justified. The condensate fraction of the layer is significantly larger than in 2D at the same surface density, being as large as 60% at the largest coverage studied.

  4. Characterization of an atomic hydrogen source for charge exchange experiments

    NASA Astrophysics Data System (ADS)

    Leutenegger, M. A.; Beiersdorfer, P.; Betancourt-Martinez, G. L.; Brown, G. V.; Hell, N.; Kelley, R. L.; Kilbourne, C. A.; Magee, E. W.; Porter, F. S.

    2016-11-01

    We characterized the dissociation fraction of a thermal dissociation atomic hydrogen source by injecting the mixed atomic and molecular output of the source into an electron beam ion trap containing highly charged ions and recording the x-ray spectrum generated by charge exchange using a high-resolution x-ray calorimeter spectrometer. We exploit the fact that the charge exchange state-selective capture cross sections are very different for atomic and molecular hydrogen incident on the same ions, enabling a clear spectroscopic diagnostic of the neutral species.

  5. Correlation of adsorption isotherms of hydrogen isotopes on mordenite adsorbents using reactive vacancy solution theory

    SciTech Connect

    Munakata, K.; Nakamura, A.; Kawamura, Y.

    2015-03-15

    The authors have applied the isotherm equations derived from the reactive vacancy solution theory (RVST) to correlation of experimental and highly non-ideal adsorption isotherms of hydrogen and deuterium on a mordenite adsorbent, and have examined the ability of the isotherm equations to match this correlation. Several isotherm equations such as Langmuir, Freundlich, Toth, Vacancy Solution Theory and so forth were also tested, but they did not work. For the Langmuir-Freundlich equation tests have indicated that its 'ability to correlate' of the adsorption isotherms is not satisfactory. For the multi-site Langmuir-Freundlich (MSLF) equation the correlation of the isotherms appears to be somewhat improved but remains unsatisfactory. The results show that the isotherm equations derived from RVST can better correlate the experimental isotherms.

  6. Precision Spectroscopy of Atomic Hydrogen and the Proton Size Puzzle

    NASA Astrophysics Data System (ADS)

    Udem, Thomas

    2016-05-01

    Precise determination of transition frequencies of simple atomic systems are required for a number of fundamental applications such as tests of quantum electrodynamics (QED), the determination of fundamental constants and nuclear charge radii. The sharpest transition in atomic hydrogen occurs between the metastable 2S state and the 1S ground state. Its transition frequency has now been measured with almost 15 digits accuracy using an optical frequency comb and a cesium atomic clock as a reference. A recent measurement of the Lamb shift in muonic hydrogen is in significant contradiction to the hydrogen data if QED calculations are assumed to be correct. We hope to contribute to the resolution of this so called `proton size puzzle' by providing additional experimental input from the hydrogen side.

  7. The sticking of atomic hydrogen on amorphous water ice

    SciTech Connect

    Veeraghattam, Vijay K.; Manrodt, Katie; Lewis, Steven P.; Stancil, P. C. E-mail: lewis@physast.uga.edu

    2014-07-20

    Using classical molecular dynamics, we have simulated the sticking and scattering process of a hydrogen atom on an amorphous ice film to predict the sticking probability of hydrogen on ice surfaces. A wide range of initial kinetic energies of the incident hydrogen atom (10 K-600 K) and two different ice temperatures (10 K and 70 K) were used to investigate this fundamental process in interstellar chemistry. We report here the sticking probability of atomic hydrogen as a function of incident kinetic energy, gas temperature, and substrate temperature, which can be used in astrophysical models. The current results are compared to previous theoretical and experimental studies that have reported a wide range in the sticking coefficient.

  8. Heat capacity of quantum adsorbates: Hydrogen and helium on evaporated gold films

    SciTech Connect

    Birmingham, J.T. |

    1996-06-01

    The author has constructed an apparatus to make specific heat measurements of quantum gases adsorbed on metallic films at temperatures between 0.3 and 4 K. He has used this apparatus to study quench-condensed hydrogen films between 4 and 923 layers thick with J = 1 concentrations between 0.28 and 0.75 deposited on an evaporated gold surface. He has observed that the orientational ordering of the J = 1 molecules depends on the substrate temperature during deposition of the hydrogen film. He has inferred that the density of the films condensed at the lowest temperatures is 25% higher than in bulk H{sub 2} crystals and have observed that the structure of those films is affected by annealing at 3.4 K. The author has measured the J = 1 to J = 0 conversion rate to be comparable to that of the bulk for thick films; however, he found evidence that the gold surface catalyzes conversion in the first two to four layers. He has also used this apparatus to study films of {sup 4}He less than one layer thick adsorbed on an evaporated gold surface. He shows that the phase diagram of the system is similar to that for {sup 4}He/graphite although not as rich in structure, and the phase boundaries occur at different coverages and temperatures. At coverages below about half a layer and at sufficiently high temperatures, the {sup 4}He behaves like a two-dimensional noninteracting Bose gas. At lower temperatures and higher coverages, liquidlike and solidlike behavior is observed. The Appendix shows measurements of the far-infrared absorptivity of the high-{Tc} superconductor La{sub 1.87}Sr{sub 0.13}CuO{sub 4}.

  9. Electronic Structures of Hydrogen and Oxygen Adsorbed Tungsten (3, 2, 0) and Tungsten (8, 7, 0) Surfaces

    NASA Astrophysics Data System (ADS)

    Bao, Zhuo; Bostwick, Aaron; Rotenberg, Eli; Kevan, Stephen

    2011-03-01

    The Valence band electronic structues of Hydrogen adsorbed and Oxygen adsorbed Tungsten stepped surfaces, Tungsten (3, 2, 0) and (8, 7, 0) surface are investigated using angular-resolved photoemission techniques and ab-initio electronic structure calculation methods. The band features of surface states at different Hydrogen and Oxygen coverages are experimentally distinguished by using photon-energy scanning method. Quasi-one- dimensional band features are found in the surface states with saturated Oxygen coverages of both stepped surfaces. The effects of adsorbate coverages on dimensionalities of surface electronic states are studied using high-resolution band mapping methods and ab-initio calculation methods. Thanks to Department of Energy for the financial supporting of this project.

  10. Manipulation of adsorbed atoms and creation of new structures on room-temperature surfaces with a scanning tunneling microscope.

    PubMed

    Whitman, L J; Stroscio, J A; Dragoset, R A; Celotta, R J

    1991-03-01

    A general method of manipulating adsorbed atoms and molecules on room-temperature surfaces with the use of a scanning tunneling microscope is described. By applying an appropriate voltage pulse between the sample and probe tip, adsorbed atoms can be induced to diffuse into the region beneath the tip. The field-induced diffusion occurs preferentially toward the tip during the voltage pulse because of the local potential energy gradient arising from the interaction of the adsorbate dipole moment with the electric field gradient at the surface. Depending upon the surface and pulse parameters, cesium (Cs) structures from one nanometer to a few tens of nanometers across have been created in this way on the (110) surfaces of gallium arsenide (GaAs) and indium antimonide (InSb), including structures that do not naturally occur.

  11. Theoretical realization of cluster-assembled hydrogen storage materials based on terminated carbon atomic chains.

    PubMed

    Liu, Chun-Sheng; An, Hui; Guo, Ling-Ju; Zeng, Zhi; Ju, Xin

    2011-01-14

    The capacity of carbon atomic chains with different terminations for hydrogen storage is studied using first-principles density functional theory calculations. Unlike the physisorption of H(2) on the H-terminated chain, we show that two Li (Na) atoms each capping one end of the odd- or even-numbered carbon chain can hold ten H(2) molecules with optimal binding energies for room temperature storage. The hybridization of the Li 2p states with the H(2)σ orbitals contributes to the H(2) adsorption. However, the binding mechanism of the H(2) molecules on Na arises only from the polarization interaction between the charged Na atom and the H(2). Interestingly, additional H(2) molecules can be bound to the carbon atoms at the chain ends due to the charge transfer between Li 2s2p (Na 3s) and C 2p states. More importantly, dimerization of these isolated metal-capped chains does not affect the hydrogen binding energy significantly. In addition, a single chain can be stabilized effectively by the C(60) fullerenes termination. With a hydrogen uptake of ∼10 wt.% on Li-coated C(60)-C(n)-C(60) (n = 5, 8), the Li(12)C(60)-C(n)-Li(12)C(60) complex, keeping the number of adsorbed H(2) molecules per Li and stabilizing the dispersion of individual Li atoms, can serve as better building blocks of polymers than the (Li(12)C(60))(2) dimer. These findings suggest a new route to design cluster-assembled hydrogen storage materials based on terminated sp carbon chains.

  12. Cold atomic hydrogen in the inner galaxy

    NASA Technical Reports Server (NTRS)

    Dickey, J. M.; Garwood, R. W.

    1986-01-01

    The VLA is used to measure 21 cm absorption in directions with the absolute value of b less than 1 deg., the absolute value of 1 less than 25 deg. to probe the cool atomic gas in the inner galaxy. Abundant H I absorption is detected; typical lines are deep and narrow, sometimes blending in velocity with adjacent features. Unlike 21 cm emission not all allowed velocities are covered: large portions of the l-v diagram are optically thin. Although not similar to H I emission, the absorption shows a striking correspondence with CO emission in the inner galaxy: essentially every strong feature detected in one survey is seen in the other. The provisional conclusion is that in the inner galaxy most cool atomic gas is associated with molecular cloud complexes. There are few or no cold atomic clouds devoid of molecules in the inner galaxy, although these are common in the outer galaxy.

  13. Calculation of vibrational frequencies of atoms adsorbed on metal surfaces: H, O, and S on Ni(100) and Ni(111) as examples

    SciTech Connect

    Black, J.E.; Bopp, P.; Luetzenkirchen, K.; Wolfsberg, M.

    1982-06-15

    We present vibrational frequencies calculated for H, O, and S atoms adsorbed on Ni(111) and Ni(100) surfaces. The calculations are done for a single atom adsorbed on nickel clusters, and also for a single atom and periodic arrangements of atoms on an infinite nickel substrate. We are able to indicate under what conditions a simple cluster calculation will yield vibrational frequencies suitable for comparison with experiment.

  14. Thermochemical nonequilibrium in atomic hydrogen at elevated temperatures

    NASA Technical Reports Server (NTRS)

    Scott, R. K.

    1972-01-01

    A numerical study of the nonequilibrium flow of atomic hydrogen in a cascade arc was performed to obtain insight into the physics of the hydrogen cascade arc. A rigorous mathematical model of the flow problem was formulated, incorporating the important nonequilibrium transport phenomena and atomic processes which occur in atomic hydrogen. Realistic boundary conditions, including consideration of the wall electrostatic sheath phenomenon, were included in the model. The governing equations of the asymptotic region of the cascade arc were obtained by writing conservation of mass and energy equations for the electron subgas, an energy conservation equation for heavy particles and an equation of state. Finite-difference operators for variable grid spacing were applied to the governing equations and the resulting system of strongly coupled, stiff equations were solved numerically by the Newton-Raphson method.

  15. Atomic hydrogen on Mars - Measurements at solar minimum

    NASA Technical Reports Server (NTRS)

    Levine, J. S.; Mcdougal, D. S.; Anderson, D. E., Jr.; Barker, E. S.

    1978-01-01

    The Copernicus Orbiting Astronomical Observatory was used to obtain measurements of Mars Lyman-alpha (1215.671-angstrom) emission at the solar minimum, which has resulted in the first information on atomic hydrogen concentrations in the upper atmosphere of Mars at the solar minimum. The Copernicus measurements, coupled with the Viking in situ measurements of the temperature (170 plus or minus 30 K) of the upper atmosphere of Mars, indicate that the atomic hydrogen number density at the exobase of Mars (250 kilometers) is about 60 times greater than that deduced from Mariner 6 and 7 Lyman-alpha measurements obtained during a period of high solar activity. The Copernicus results are consistent with Hunten's hypothesis of the diffusion-limited escape of atomic hydrogen from Mars.

  16. Sensor for measuring the atomic fraction in highly dissociated hydrogen

    SciTech Connect

    Gardner, W.L.

    1994-12-31

    Atomic hydrogen is a very important constituent for processes ranging from cleaning oxide from GaAs and annealing amorphous silicon to the deposition of diamond. Because the usual techniques for measuring atomic fraction are either expensive and cumbersome to use, or unsuitable for application to highly dissociated hydrogen, a specially designed sensor was developed. Sensor design is based on a diffusion tube with noncatalytic walls, having one end open to the atom source and a catalytic closure at the other end. The sensor is simple and inexpensive to fabricate, and determining atom density is straightforward. Sensor design also inhibits thermal runaway, which occurs when atom density is high enough to impart enough recombination energy to the non-catalytic surface to substantially raise its temperature. While recombination coefficients for such surfaces are very low near room temperature, they increase nearly exponentially with temperature unless actively cooled. With the use of a straightforward calibration scheme to determine the variation in species fraction along the diffusion tube, the atomic fraction at the tube opening is determined. Design strategy, implementation considerations, and calibration method are presented. In addition, data obtained from an atomic hydrogen source are compared to relevant published data.

  17. Proton form factor effects in hydrogenic atoms

    SciTech Connect

    Daza, F. Garcia; Kelkar, N. G.; Nowakowski, M.

    2011-10-21

    The proton structure corrections to the hyperfine splittings in electronic and muonic hydrogen are evaluated using the Breit potential with electromagnetic form factors. In contrast to other methods, the Breit equation with q{sup 2} dependent form factors is just an extension of the standard Breit equation which gives the hyperfine splitting Hamiltonian. Precise QED corrections are comparable to the structure corrections which therefore need to be evaluated ab initio.

  18. Atomic hydrogen distribution. [in Titan atmospheric model

    NASA Technical Reports Server (NTRS)

    Tabarie, N.

    1974-01-01

    Several possible H2 vertical distributions in Titan's atmosphere are considered with the constraint of 5 km-A a total quantity. Approximative calculations show that hydrogen distribution is quite sensitive to two other parameters of Titan's atmosphere: the temperature and the presence of other constituents. The escape fluxes of H and H2 are also estimated as well as the consequent distributions trapped in the Saturnian system.

  19. Ultra-cold methods for polarized atomic hydrogen

    SciTech Connect

    Luppov, V.G.; Arnold, J.D.; Blinov, B.B.; Bychkov, M.A.; Gladycheva, S.E.; Krisch, A.D.; Lin, A.M.; Raymond, R.S.; Fimushkin, V.V.; Bychkov, M.A.; Mochalov, V.V.; Semenov, P.A.

    1998-01-01

    Using the ultra-cold electron-spin-polarized atomic hydrogen technique, one can produce a slow monochromatic beam for use as a polarized jet target. We will first review the development of the ultra-cold technique and then discuss the recent progress on Michigan{close_quote}s Mark-II ultra-cold proton-spin-polarized hydrogen jet target. {copyright} {ital 1998 American Institute of Physics.}

  20. Controlling the spin of co atoms on pt(111) by hydrogen adsorption.

    PubMed

    Dubout, Q; Donati, F; Wäckerlin, C; Calleja, F; Etzkorn, M; Lehnert, A; Claude, L; Gambardella, P; Brune, H

    2015-03-13

    We investigate the effect of H adsorption on the magnetic properties of individual Co atoms on Pt(111) with scanning tunneling microscopy. For pristine Co atoms, we detect no inelastic features in the tunnel spectra. Conversely, CoH and CoH2 show a number of low-energy vibrational features in their differential conductance identified by isotope substitution. Only the fcc-adsorbed species present conductance steps of magnetic origin, with a field splitting identifying their effective spin as Seff=2 for CoH and 3/2 for CoH2. The exposure to H2 and desorption through tunnel electrons allow the reversible control of the spin in half-integer steps. Because of the presence of the surface, the hydrogen-induced spin increase is opposite to the spin sequence of CoHn molecules in the gas phase.

  1. Muon transfer from hot muonic hydrogen atoms to neon

    SciTech Connect

    Jacot-Guillarmod, R.; Bailey, J.M.; Beer, G.A.; Knowles, P.E.; Mason, G.R.; Olin, A.; Beveridge, J.L.; Marshall, G.M.; Brewer, J.H.; Forster, B.M.; Huber, T.M.; Kammel, P.; Zmeskal, J.; Kunselman, A.R.; Petitjean, C.

    1992-12-31

    A negative muon beam has been directed on adjacent solid layers of hydrogen and neon. Three targets differing by their deuterium concentration were investigated. Muonic hydrogen atoms can drift to the neon layer where the muon is immediately transferred. The time structure of the muonic neon X-rays follows the exponential law with a disappearance rate corresponding to the one of {mu}{sup {minus}p} atoms in each target. The rates {lambda}{sub pp{mu}} and {lambda}{sub pd} can be extracted.

  2. Michigan ultra-cold polarized atomic hydrogen jet target

    NASA Astrophysics Data System (ADS)

    Blinov, B. B.; Gladycheva, S. E.; Kageya, T.; Kantsyrev, D. Yu.; Krisch, A. D.; Luppov, V. G.; Morozov, V. S.; Murray, J. R.; Raymond, R. S.; Borisov, N. S.; Fimushkin, V. V.; Grishin, V. N.; Mysnik, A. I.; Kleppner, D.

    2001-06-01

    To study spin effects in high energy collisions, we are developing an ultra-cold high-density jet target of proton-spin-polarized hydrogen atoms. The target uses a 12 Tesla magnetic field and a 0.3 K separation cell coated with superfluid helium-4 to produce a slow monochromatic electron-spin-polarized atomic hydrogen beam, which is then focused by a superconducting sextupole into the interaction region. In recent tests, we studied a polarized beam of hydrogen atoms focused by the superconducting sextupole into a compression tube detector, which measured the polarized atoms' intensity. The Jet produced, at the detector, a spin-polarized atomic hydrogen beam with a measured intensity of about 2.8.1015 H s-1 and a FWHM area of less than 0.13 cm2. This intensity corresponds to a free jet density of about 1.1012 H cm-3 with a proton polarization of about 50%. When the transition RF unit is installed, we expect a proton polarization higher than 90%. .

  3. Slow metastable atomic hydrogen beam by optical pumping

    NASA Astrophysics Data System (ADS)

    Harvey, K. C.

    1982-05-01

    A beam source of atomic hydrogen is described which produces metastable atoms in the 2S1/2 state by optical pumping. A beam flux of 1016 atoms/s is generated in the ground state. The atoms in the beam pass in front of a lamp producing Lyman-β (1026 Å) radiation, where some of them are excited to the 3P level and cascade with a branching ratio of 12% to the 2S1/2 state. The number of metastable atoms produced is measured by quenching them with an electric field and detecting the emitted Lyman-α (1216 Å) radiation. Beams of 106 metastable atoms/s were obtained. Using the Bethe-Lamb theory for the quenching process, a metastable beam effective temperature of 100 K was measured.

  4. Probing the heliosphere with energetic hydrogen atoms

    NASA Technical Reports Server (NTRS)

    Hsieh, K. C.; Shih, K. L.; Jokipii, J. R.; Grzedzielski, S.

    1992-01-01

    The idea of using energetic neutral atoms (ENAs), produced by charge exchange between energetic ions and ambient neutral atoms, as a diagnostic tool to investigate planetary magnetospheres from a distance has been extended to the investigation of the heliosphere. The paper explores what one can reasonably expect of the heliospheric ENA (HSENA) and what criteria would be imposed on HSENA instruments by concentrating on 10-10 exp 3 keV protons in quiet-time interplanetary space, solar-flare events, corotating interaction regions, and populations have distinctive signatures and that the detection of these particles can reveal energy spatial and propagation of ions in 3D interplanetary space, including the solar-wind termination shock. Such breadth of information could not be gained by in situ means.

  5. Hydrogen atom temperature measured with wavelength-modulated laser absorption spectroscopy in large scale filament arc negative hydrogen ion source

    SciTech Connect

    Nakano, H. Goto, M.; Tsumori, K.; Kisaki, M.; Ikeda, K.; Nagaoka, K.; Osakabe, M.; Takeiri, Y.; Kaneko, O.; Nishiyama, S.; Sasaki, K.

    2015-04-08

    The velocity distribution function of hydrogen atoms is one of the useful parameters to understand particle dynamics from negative hydrogen production to extraction in a negative hydrogen ion source. Hydrogen atom temperature is one of the indicators of the velocity distribution function. To find a feasibility of hydrogen atom temperature measurement in large scale filament arc negative hydrogen ion source for fusion, a model calculation of wavelength-modulated laser absorption spectroscopy of the hydrogen Balmer alpha line was performed. By utilizing a wide range tunable diode laser, we successfully obtained the hydrogen atom temperature of ∼3000 K in the vicinity of the plasma grid electrode. The hydrogen atom temperature increases as well as the arc power, and becomes constant after decreasing with the filling of hydrogen gas pressure.

  6. Low resistance Cu3Ge compounds formation by the low temperature treatment of Cu/Ge system in atomic hydrogen

    NASA Astrophysics Data System (ADS)

    Kazimirov, A. I.; Erofeev, E. V.; Fedin, I. V.; Kagadei, V. A.; Yurjev, Y. N.

    2016-06-01

    The research deals with the regularities for Cu3Ge compound formation under the low temperature treatment of a double-layer Cu/Ge system deposited on i-GaAs substrate in atomic hydrogen flow. The treatment of a Cu/Ge/i-GaAs system with layer thicknesses, respectively, of 122 and 78 nm, in atomic hydrogen with a flow rate of 1015 at.cm-2s-1 for a duration of 2.5-10 min at room temperature, leads to an interdiffusion of Cu and Ge and formation of a polycrystalline film containing stoichiometric phase Cu3Ge. The film consists of vertically oriented grains of dimensions 100-150 nm and has a minimum specific resistance of 4.5 μΩ cm. Variation in the treatment duration of Cu/Ge/i-GaAs samples in atomic hydrogen affects Cu and Ge distribution profiles, the phase composition of films formed, and the specific resistance of the latter. As observed, Cu3Ge compound synthesis at room temperature demonstrates the stimulative effects characteristic of atomic hydrogen treatment for both Cu and Ge diffusion and for the chemical reaction of Cu3Ge compound generation. Activation of these processes can be conditioned by the energy released during recombination of hydrogen atoms adsorbed on the surface of a Cu/Ge/i-GaAs sample.

  7. Photoionization of atoms and molecules. [of hydrogen, helium, and xenon

    NASA Technical Reports Server (NTRS)

    Samson, J. A. R.

    1976-01-01

    A literature review on the present state of knowledge in photoionization is presented. Various experimental techniques that have been developed to study photoionization, such as fluorescence and photoelectron spectroscopy, mass spectroscopy, are examined. Various atoms and molecules were chosen to illustrate these techniques, specifically helium and xenon atoms and hydrogen molecules. Specialized photoionization such as in positive and negative ions, excited states, and free radicals is also treated. Absorption cross sections and ionization potentials are also discussed.

  8. Hydrogen spillover on Rh/TiO2: the FTIR study of donated electrons, co-adsorbed CO and H/D exchange.

    PubMed

    Panayotov, D; Ivanova, E; Mihaylov, M; Chakarova, K; Spassov, T; Hadjiivanov, K

    2015-08-28

    Hydrogen dissociation and spillover on supported metal nanoparticles have received renewed interest because these chemical processes are closely related to applications in heterogeneous catalysis and hydrogen storage. In heterogeneous catalysis, spillover can control the reaction rate and selectivity of a wide range of reactions, e.g. hydrogenation, synthesis of methanol and hydroisomerization. In this work, we combine three spectroscopic approaches, i.e. the FT-IR spectroscopy of donated electrons, co-adsorbed CO and H/D exchange, to obtain detailed information on the dynamics of hydrogen interaction with a model 1.3% Rh/TiO2 catalyst. Our spectroscopic results helped us to build a physical picture of the processes occurring during the H-spillover on Rh/TiO2. It was found that molecular H2 dissociates on nanocrystalline Rh; H atoms spillover onto the titania thus protonating the semiconductor, while donating electrons to shallow trap (ST) states and the conduction band (CB) of TiO2. These donated electrons are observed by their specific IR features. By simultaneously monitoring the changes in the vibrational modes of CO, and, the infrared absorbance due to transitions involving CB and ST electrons, we found that both CO-reduced and partially re-oxidized Rh nanocrystallites promote the H-spillover and thus the n-doping of TiO2 materials. Upon evacuation, the process reverses: hydrogen atoms spillover back to Rh nanoparticles where they recombine to form H2 molecules that desorb from the surface. These new mechanistic insights into the process of H2 dissociation and spillover on the powder Rh/TiO2 catalyst call for further model surface science studies with model metal nanoparticle-single crystal substrate systems, in which a detailed picture of energetics and spatial distribution of hydrogen and injected electrons could be obtained.

  9. Variational Perturbation Treatment of the Confined Hydrogen Atom

    ERIC Educational Resources Information Center

    Montgomery, H. E., Jr.

    2011-01-01

    The Schrodinger equation for the ground state of a hydrogen atom confined at the centre of an impenetrable cavity is treated using variational perturbation theory. Energies calculated from variational perturbation theory are comparable in accuracy to the results from a direct numerical solution. The goal of this exercise is to introduce the…

  10. The Confined Hydrogen Atom with a Moving Nucleus

    ERIC Educational Resources Information Center

    Fernandez, Francisco M.

    2010-01-01

    We study the hydrogen atom confined to a spherical box with impenetrable walls but, unlike earlier pedagogical articles on the subject, we assume that the nucleus also moves. We obtain the ground-state energy approximately by means of first-order perturbation theory and show that it is greater than that for the case in which the nucleus is clamped…

  11. Probability of Locating the Electron in a Hydrogen Atom

    NASA Astrophysics Data System (ADS)

    Mak, Thomas C. W.; Li, Wai-Kee

    2000-04-01

    A variety of numerical problems, along with their solutions, regarding the probability of locating the electron in a hydrogen atom are given. These problems range from simple substitution exercises to graduate-level take-home questions. Comments on the physical meaning of some of the results are also provided. These problems may be easily modified by teachers to suit their purposes.

  12. Quantitative calculation of the absorption spectrum of the hydrogen atom

    NASA Astrophysics Data System (ADS)

    Ogilvie, J. F.; Fee, G. J.

    2014-03-01

    With mathematical software (Maple), we have calculated quantitatively the entire absorption spectrum of the hydrogen atom in its electronic ground state for transitions to both discrete and continuum states, within the purview of non-relativistic wave mechanics. We present plots of wave functions in both coordinate and momentum representations and the calculated spectra.

  13. 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…

  14. Role of adsorbed hydrogen species on ruthenium and molybdenum sulfides. Characterization by inelastic neutron scattering, thermoanalysis methods and model reactions

    SciTech Connect

    Lacroix, M.; Jobic, H.; Dumonteil, C.; Afanasiev, P.

    1996-12-31

    The interaction of hydrogen over unsupported MoS{sub 2} and RuS{sub 2} has been investigated as a function of the sulfur to metal ratio. On these solids the presence of sulfur deficient sites is required to generate an activity and to allow hydrogen chemisorption. The nature of the adsorbed species differs depending on the catalyst under investigation. On RuS{sub 2}, two types of hydrogen were evidenced by thermoflash desorption and inelastic neutron scattering: one was assigned to hydrogen adsorbed on surface sulfur anions while the other one is retained on coordinatively unsaturated ruthenium cations. By contrast, only SH groups were detected on MoS{sub 2}. ESR measurements have shown that a fraction of chemisorbed hydrogen induces a modification of the concentration of paramagnetic Mo(V) and Mo(III) species. Thus both solids behave differently towards an hydrogen atmosphere. RuS{sub 2} has a pseudometallic comportment whereas for MoS{sub 2} redox or acid base properties are involved.

  15. Microwave plasma generation of hydrogen atoms for rocket propulsion

    NASA Technical Reports Server (NTRS)

    Chapman, R.; Filpus, J.; Morin, T.; Snellenberger, R.; Asmussen, J.; Hawley, M.; Kerber, R.

    1981-01-01

    A flow microwave plasma reaction system is used to study the conversion of hydrogen to hydrogen atoms as a function of pressure, power density, cavity tuning, cavity mode, and time in the plasma zone. Hydrogen atom concentration is measured down-stream from the plasma by NOCl titration. Extensive modeling of the plasma and recombination zones is performed with the plasma zone treated as a backmix reaction system and the recombination zone treated as a plug flow. The thermodynamics and kinetics of the recombination process are examined in detail to provide an understanding of the conversion of recombination energy to gas kinetic energy. It is found that cavity tuning, discharge stability, and optimum power coupling are critically dependent on the system pressure, but nearly independent of the flow rate.

  16. Atomic hydrogen doping in single-crystal vanadium dioxide

    NASA Astrophysics Data System (ADS)

    Ji, Heng; Hardy, Will; Wei, Jiang; Lin, Jian; Paik, Hanjong; Schlom, Darrell; Natelson, Douglas

    2014-03-01

    Vanadium dioxide is a strongly correlated material with a bulk metal-to-insulator transition (MIT) near 340 K. Previous experiments in single-crystal nanowires (J. Wei et al., Nature Nano. 7, 357-362 (2012)) have shown that catalytic doping with atomic hydrogen can stabilize the high temperature metallic state. In this experiment, we used a hot filament source to split hydrogen molecules and directly dope atomic hydrogen into VO2 material, including epitaxial films and nanowires, without any catalyst. From observations of the wire samples, we infer the relative diffusion rates of H in the monoclinic and rutile crystal structures. Transport measurements of the doped film samples show no temperature-driven transition, but rather a conducting state down to 2K. We present Hall and magnetoresistance measurements on macroscale and mesoscale devices fabricated from the doped films.

  17. Transition state geometry in radical hydrogen atom abstraction

    NASA Astrophysics Data System (ADS)

    Denisov, Evgenii T.; Shestakov, Alexander F.; Denisova, Taisa G.

    2012-12-01

    The interatomic distances in the transition states of radical hydrogen atom abstraction reactions X•+HY → XH+Y• determined by quantum chemical calculations are systematized and generalized. It is shown that depending on the reaction centre structure, these reactions can be subdivided into classes with the same X...Y interatomic distance in each class. The transition state geometries found by the methods of intersecting parabolas and intersecting Morse curves are also presented. The X...H...Y fragments are almost linear, the hydrogen atom position being determined by the reaction enthalpy. The effects of triplet repulsion, electronegativities and radii of X and Y atoms, the presence of adjoining π-bonds, and steric effects on the X...Y interatomic distances are analyzed and characterized. The bibliography includes 62 references.

  18. Atomic cobalt on nitrogen-doped graphene for hydrogen generation

    NASA Astrophysics Data System (ADS)

    Fei, Huilong; Dong, Juncai; Arellano-Jiménez, M. Josefina; Ye, Gonglan; Dong Kim, Nam; Samuel, Errol L. G.; Peng, Zhiwei; Zhu, Zhuan; Qin, Fan; Bao, Jiming; Yacaman, Miguel Jose; Ajayan, Pulickel M.; Chen, Dongliang; Tour, James M.

    2015-10-01

    Reduction of water to hydrogen through electrocatalysis holds great promise for clean energy, but its large-scale application relies on the development of inexpensive and efficient catalysts to replace precious platinum catalysts. Here we report an electrocatalyst for hydrogen generation based on very small amounts of cobalt dispersed as individual atoms on nitrogen-doped graphene. This catalyst is robust and highly active in aqueous media with very low overpotentials (30 mV). A variety of analytical techniques and electrochemical measurements suggest that the catalytically active sites are associated with the metal centres coordinated to nitrogen. This unusual atomic constitution of supported metals is suggestive of a new approach to preparing extremely efficient single-atom catalysts.

  19. Atomic hydrogen maser active oscillator cavity and bulb design optimization

    NASA Technical Reports Server (NTRS)

    Peters, H. E.; Washburn, P. J.

    1984-01-01

    The performance characteristics and reliability of the active oscillator atomic hydrogen maser depend upon oscillation parameters which characterize the interaction region of the maser, the resonant cavity and atom storage bulb assembly. With particular attention to use of the cavity frequency switching servo (1) to reduce cavity pulling, it is important to maintain high oscillation level, high atomic beam flux utilization efficiency, small spin exchange parameter and high cavity quality factor. It is also desirable to have a small and rigid cavity and bulb structure and to minimize the cavity temperature sensitivity. Curves for a novel hydrogen maser cavity configuration which is partially loaded with a quartz dielectric cylinder and show the relationships between cavity length, cavity diameter, bulb size, dielectric thickness, cavity quality factor, filling factor and cavity frequency temperature coefficient are presented. The results are discussed in terms of improvement in maser performance resulting from particular design choices.

  20. Atomic cobalt on nitrogen-doped graphene for hydrogen generation

    PubMed Central

    Fei, Huilong; Dong, Juncai; Arellano-Jiménez, M. Josefina; Ye, Gonglan; Dong Kim, Nam; Samuel, Errol L.G.; Peng, Zhiwei; Zhu, Zhuan; Qin, Fan; Bao, Jiming; Yacaman, Miguel Jose; Ajayan, Pulickel M.; Chen, Dongliang; Tour, James M.

    2015-01-01

    Reduction of water to hydrogen through electrocatalysis holds great promise for clean energy, but its large-scale application relies on the development of inexpensive and efficient catalysts to replace precious platinum catalysts. Here we report an electrocatalyst for hydrogen generation based on very small amounts of cobalt dispersed as individual atoms on nitrogen-doped graphene. This catalyst is robust and highly active in aqueous media with very low overpotentials (30 mV). A variety of analytical techniques and electrochemical measurements suggest that the catalytically active sites are associated with the metal centres coordinated to nitrogen. This unusual atomic constitution of supported metals is suggestive of a new approach to preparing extremely efficient single-atom catalysts. PMID:26487368

  1. Atomic cobalt on nitrogen-doped graphene for hydrogen generation.

    PubMed

    Fei, Huilong; Dong, Juncai; Arellano-Jiménez, M Josefina; Ye, Gonglan; Dong Kim, Nam; Samuel, Errol L G; Peng, Zhiwei; Zhu, Zhuan; Qin, Fan; Bao, Jiming; Yacaman, Miguel Jose; Ajayan, Pulickel M; Chen, Dongliang; Tour, James M

    2015-01-01

    Reduction of water to hydrogen through electrocatalysis holds great promise for clean energy, but its large-scale application relies on the development of inexpensive and efficient catalysts to replace precious platinum catalysts. Here we report an electrocatalyst for hydrogen generation based on very small amounts of cobalt dispersed as individual atoms on nitrogen-doped graphene. This catalyst is robust and highly active in aqueous media with very low overpotentials (30 mV). A variety of analytical techniques and electrochemical measurements suggest that the catalytically active sites are associated with the metal centres coordinated to nitrogen. This unusual atomic constitution of supported metals is suggestive of a new approach to preparing extremely efficient single-atom catalysts. PMID:26487368

  2. FTIR study of ammonia formation via the successive hydrogenation of N atoms trapped in a solid N2 matrix at low temperatures.

    PubMed

    Hidaka, Hiroshi; Watanabe, Motohiro; Kouchi, Akira; Watanabe, Naoki

    2011-09-21

    A Fourier transform infrared absorption spectroscopy (FTIR) study showed that NH(3) was formed by the successive reaction of hydrogen atoms with nitrogen atoms in an N(2) matrix at 10 K. Reactions appeared to proceed via the Langmuir-Hinshelwood mechanism because NH(3) formation was not observed at 20 K. At this temperature, H atoms did not adsorb significantly onto the N(2) matrix; i.e., the surface residence times were short. Furthermore, NH(3) yields via the successive hydrogenation of N atoms were significant, even after H atom deposition onto the N(2) matrix containing trapped N atoms onto which had been deposited a superficial pure solid N(2) adlayer. This result clearly indicates that H atoms diffuse in pure solid N(2) matrices at 10 K.

  3. Electron-impact ionization of atomic hydrogen

    SciTech Connect

    Baertschy, Mark D.

    2000-02-14

    Since the invention of quantum mechanics, even the simplest example of collisional breakup in a system of charged particles, e{sup {minus}} + H {r_arrow} H{sup +} + e{sup {minus}} + e{sup {minus}}, has stood as one of the last unsolved fundamental problems in atomic physics. A complete solution requires calculating the energies and directions for a final state in which three charged particles are moving apart. Advances in the formal description of three-body breakup have yet to lead to a viable computational method. Traditional approaches, based on two-body formalisms, have been unable to produce differential cross sections for the three-body final state. Now, by using a mathematical transformation of the Schrodinger equation that makes the final state tractable, a complete solution has finally been achieved, Under this transformation, the scattering wave function can be calculated without imposing explicit scattering boundary conditions. This approach has produced the first triple differential cross sections that agree on an absolute scale with experiment as well as the first ab initio calculations of the single differential cross section.

  4. Sudden perturbation of hydrogen atoms by intense ultrashort laser pulses

    SciTech Connect

    Lugovskoy, A. V.; Bray, I.

    2005-12-15

    We study theoretically how hydrogen atoms respond to intense ultrashort laser pulses of duration {tau} shorter than the inverse of the initial-state energy {epsilon}{sub i}{sup -1}. An analytical expression for the evolution operator S is derived up to the first order of the sudden perturbation approximation. This approximation treats the laser-atom interaction beyond the dipole approximation and yields S as a series in the small parameter {epsilon}{sub i}{tau}. It is shown that the effect of realistic laser pulses on atoms begins at the first order of {epsilon}{sub i}{tau}. Transitions between atomic (nlm) states of different m become possible due to the action of the pulse's magnetic field. Transitions between states of same m and arbitrary l become possible if the static Coulomb potential is taken into account during the pulse.

  5. Distinct metallization and atomization transitions in dense liquid hydrogen.

    PubMed

    Mazzola, Guglielmo; Sorella, Sandro

    2015-03-13

    We perform molecular dynamics simulations driven by accurate quantum Monte Carlo forces on dense liquid hydrogen. There is a recent report of a complete atomization transition between a mixed molecular-atomic liquid and a completely dissociated fluid in an almost unaccessible pressure range [Nat. Commun. 5, 3487 (2014)]. Here, instead, we identify a different transition between the fully molecular liquid and the mixed-atomic fluid at ∼400  GPa, i.e., in a much more interesting pressure range. We provide numerical evidence supporting the metallic behavior of this intermediate phase. Therefore, we predict that the metallization at finite temperature occurs in this partially dissociated molecular fluid, well before the complete atomization of the liquid. At high temperature this first-order transition becomes a crossover, in very good agreement with the experimental observation. Several systematic tests supporting the quality of our large scale calculations are also reported.

  6. Unparticle contribution to the hydrogen atom ground state energy

    NASA Astrophysics Data System (ADS)

    Wondrak, Michael F.; Nicolini, Piero; Bleicher, Marcus

    2016-08-01

    In the present work we study the effect of unparticle modified static potentials on the energy levels of the hydrogen atom. By using Rayleigh-Schrödinger perturbation theory, we obtain the energy shift of the ground state and compare it with experimental data. Bounds on the unparticle energy scale ΛU as a function of the scaling dimension dU and the coupling constant λ are derived. We show that there exists a parameter region where bounds on ΛU are stringent, signaling that unparticles could be tested in atomic physics experiments.

  7. Laser stripping of hydrogen atoms by direct ionization

    DOE PAGES

    Brunetti, E.; Becker, W.; Bryant, H. C.; Jaroszynski, D. A.; Chou, W.

    2015-05-08

    Direct ionization of hydrogen atoms by laser irradiation is investigated as a potential new scheme to generate proton beams without stripping foils. The time-dependent Schrödinger equation describing the atom-radiation interaction is numerically solved obtaining accurate ionization cross-sections for a broad range of laser wavelengths, durations and energies. Parameters are identified where the Doppler frequency up-shift of radiation colliding with relativistic particles can lead to efficient ionization over large volumes and broad bandwidths using currently available lasers.

  8. Semirelativistic model for ionization of atomic hydrogen by electron impact

    SciTech Connect

    Attaourti, Y.; Taj, S.; Manaut, B.

    2005-06-15

    We present a semirelativistic model for the description of the ionization process of atomic hydrogen by electron impact in the first Born approximation by using the Darwin wave function to describe the bound state of atomic hydrogen and the Sommerfeld-Maue wave function to describe the ejected electron. This model, accurate to first order in Z/c in the relativistic correction, shows that, even at low kinetic energies of the incident electron, spin effects are small but not negligible. These effects become noticeable with increasing incident electron energies. All analytical calculations are exact and our semirelativistic results are compared with the results obtained in the nonrelativistic Coulomb Born approximation both for the coplanar asymmetric and the binary coplanar geometries.

  9. Fluorescence Quenching of Benzaldehyde in Water by Hydrogen Atom Abstraction.

    PubMed

    Fletcher, Katharyn; Bunz, Uwe H F; Dreuw, Andreas

    2016-09-01

    We computed the mechanism of fluorescence quenching of benzaldehyde in water through relaxed potential energy surface scans. Time-dependent density functional theory calculations along the protonation coordinate from water to benzaldehyde reveal that photoexcitation to the bright ππ* (S3 ) state is immediately followed by ultrafast decay to the nπ* (S1 ) state. Evolving along this state, benzaldehyde (BA) abstracts a hydrogen atom, resulting in a BAH(.) and OH(.) radical pair. Benzaldehyde does not act as photobase in water, but abstracts a hydrogen atom from a nearby solvent molecule. The system finally decays back to the ground state by non-radiative decay and an electron transfers back to the OH(.) radical. Proton transfer from BAH(+) to OH(-) restores the initial situation, BA in water. PMID:27305520

  10. Quadrupole photoionization of hydrogen atoms in Debye plasmas

    SciTech Connect

    Lin, C. Y.; Ho, Y. K.

    2010-09-15

    Although a great deal of effort has been devoted to investigating dipole photoionization of plasma-embedded atoms, far less is known about the corresponding quadrupole transitions. In the present work, quadrupole photoionization processes for the ground and excited states of hydrogen atoms in Debye plasma are explored using the method of complex coordinate rotation. The plasma shielding effects on the quadrupole photoionization cross sections are reported for a variety of Debye screening lengths and compared to the dipole results accordingly. Under the perturbation of plasma screening, shape resonances and Cooper-type minima occurring in both dipole and quadrupole photoionization cross sections are presented and discussed. Comparisons are made to other theoretical calculations for the dipole photoionization with good agreement. The present quadrupole results are the first predictions for hydrogen photoionization in Debye plasmas.

  11. Analytic Solution of a Two-Dimensional Hydrogen Atom

    NASA Astrophysics Data System (ADS)

    Yang, Xiao-Li.

    1990-03-01

    The two dimensional hydrogen atom problem is solved analytically in both the relativistic and non-relativistic cases. In the nonrelativistic case, exact formulae for energy eigenvalues and eigenfunctions for both the discrete and continuous parts of the spectrum, dipole matrix elements, DC Stark effect, single- and two-photon transition rate, fine and hyperfine structures are obtained. The binding energy of the ground state is found to be reduced by a factor of four from that of a three dimensional hydrogen atom. In the relativistic case, exact analytic expressions for discrete eigen energy and normalized eigen wave function are derived. It is shown that the solution to the Dirac equation is disjoint in the spin-coordinate space (four -component spinor) in contrast to the three dimensional counterpart. This surprising result is a consequence of the planar motion of the electron.

  12. Fluorescence Quenching of Benzaldehyde in Water by Hydrogen Atom Abstraction.

    PubMed

    Fletcher, Katharyn; Bunz, Uwe H F; Dreuw, Andreas

    2016-09-01

    We computed the mechanism of fluorescence quenching of benzaldehyde in water through relaxed potential energy surface scans. Time-dependent density functional theory calculations along the protonation coordinate from water to benzaldehyde reveal that photoexcitation to the bright ππ* (S3 ) state is immediately followed by ultrafast decay to the nπ* (S1 ) state. Evolving along this state, benzaldehyde (BA) abstracts a hydrogen atom, resulting in a BAH(.) and OH(.) radical pair. Benzaldehyde does not act as photobase in water, but abstracts a hydrogen atom from a nearby solvent molecule. The system finally decays back to the ground state by non-radiative decay and an electron transfers back to the OH(.) radical. Proton transfer from BAH(+) to OH(-) restores the initial situation, BA in water.

  13. Solid Hydrogen Experiments for Atomic Propellants: Image Analyses

    NASA Technical Reports Server (NTRS)

    Palaszewski, Bryan

    2002-01-01

    This paper presents the results of detailed analyses of the images from experiments that were conducted on the formation of solid hydrogen particles in liquid helium. Solid particles of hydrogen were frozen in liquid helium, and observed with a video camera. The solid hydrogen particle sizes, their agglomerates, and the total mass of hydrogen particles were estimated. Particle sizes of 1.9 to 8 mm (0.075 to 0.315 in.) were measured. The particle agglomerate sizes and areas were measured, and the total mass of solid hydrogen was computed. A total mass of from 0.22 to 7.9 grams of hydrogen was frozen. Compaction and expansion of the agglomerate implied that the particles remain independent particles, and can be separated and controlled. These experiment image analyses are one of the first steps toward visually characterizing these particles, and allow designers to understand what issues must be addressed in atomic propellant feed system designs for future aerospace vehicles.

  14. Hydrogenated fullerenes dimer, peanut and capsule: An atomic comparison

    NASA Astrophysics Data System (ADS)

    EL-Barbary, A. A.

    2016-04-01

    Hydrogenated fullerenes are detected in the Universe in space but their identification is still unsolved task. Therefore, this paper provides useful information about hydrogenated fullerenes (dimer, peanut and capsule) using DFT method at the B3LYP/6-31G(d) level of theory. The stability, geometric structures, hydrogen adsorption energies and NMR chemical shifts are calculated. The results show that the energy of most stable isomer of C118 dimer is lower than the energies sum of C60 and C58 cages by 1.77 eV and the energy per carbon atom of C144 capsule is more stable than C60 cage by 126.98 meV. Also, endohedral Ti-doped C118 dimer and C128 peanut are found to be most stable structures than exohedral Ti-doped C118 dimer and C128 peanut by 2.19 eV/Ti and 3.52 eV/Ti, respectively. The hydrogenation process is found to be enhanced (especially at the caps) for endohedral Ti-doped C118 dimer and C128 peanut through electronic surface modifications. The most active hydrogenation sites are selected and it is found that the most stable hydrogenation sites are Houts1 and Houts3 for fullerenes and endohedral Ti-doped fullerenes, respectively.

  15. Mesoporous Silica Nanoparticles as an Adsorbent for Preconcentration and Determination of Trace Amount of Nickel in Environmental Samples by Atom Trap Flame Atomic Absorption Spectrometry

    NASA Astrophysics Data System (ADS)

    Shirkhanloo, H.; Falahnejad, M.; Zavvar Mousavi, H.

    2016-01-01

    A rapid enrichment method based on solid-phase extraction (SPE) has been established for preconcentration and separation of trace Ni(II) ions in water samples prior to their determination by atom trap flame atomic absorption spectrometry. A column filled with bulky NH2-UVM7 was used as the novel adsorbent. Under optimal conditions, the linear range, limit of detection (LOD), and preconcentration factor (PF) were 3-92 μg/L, 0.8 μg/L, and 100, respectively. The validity of the method was checked by the standard reference material.

  16. Effects of wall coatings and temperature on hydrogen atom surface recombination

    NASA Technical Reports Server (NTRS)

    Wong, E. L.; Baker, C. E.

    1973-01-01

    The efficiency of various surface coatings and materials toward inhibiting hydrogen atom surface recombination was investigated over a temperature range of 77 to 298 K. A flow discharge, mass spectrometer technique was used to make the experimental measurements. Hydrogen atoms were monitored directly, and these measurements were expressed as ratios of mass spectrometer peak heights for atomic and molecular hydrogen. Several of the surface coatings studied were efficient at reducing hydrogen atom surface recombination at room temperature. However, as the temperature was lowered, this efficiency was drastically reduced. Calibration of the mass spectrometer for atomic and molecular hydrogen indicated that mass spectrometer discrimination against hydrogen atoms was severe. Mass spectrometer sensitivity for hydrogen atoms was only about one-sixth of that for molecular hydrogen.

  17. Probing the effects of 2D confinement on hydrogen dynamics in water and ice adsorbed in graphene oxide sponges.

    PubMed

    Romanelli, Giovanni; Senesi, Roberto; Zhang, Xuan; Loh, Kian Ping; Andreani, Carla

    2015-12-21

    We studied the single particle dynamics of water and ice adsorbed in graphene oxide (GO) sponges at T = 293 K and T = 20 K. We used Deep Inelastic Neutron Scattering (DINS) at the ISIS neutron and muon spallation source to derive the hydrogen mean kinetic energy, 〈EK〉, and momentum distribution, n(p). The goal of this work was to study the hydrogen dynamics under 2D confinement and the potential energy surface, fingerprinting the hydrogen interaction with the layered structure of the GO sponge. The observed scattering is interpreted within the framework of the impulse approximation. Samples of both water and ice adsorbed in GO show n(p) functions with almost harmonic and anisotropic line shapes and 〈EK〉 values in excess of the values found at the corresponding temperatures in the bulk. The hydrogen dynamics are discussed in the context of the interaction between the interfacial water and ice and the confining hydrophilic surface of the GO sponge. PMID:26556604

  18. Infrared atomic hydrogen line formation in luminous stars

    NASA Technical Reports Server (NTRS)

    Krolik, J. H.; Smith, H. A.

    1981-01-01

    Infrared atomic hydrogen lines observed in luminous stars, generally attributed to compact circumstellar H II regions, can also be formed in the winds likely to emanate from these stars. Implications are discussed for the class of obscured infrared point sources showing these lines, and an illustrative model is derived for the BN object in Orion. Such stellar winds should also produce weak, but detectable, radio emission.

  19. Lamb shift in the hydrogen atom: Leading logarithmic corrections

    SciTech Connect

    Karshenboim, S.G.

    1995-04-01

    The leading logarithmic correction to the difference of the Lamb shifts of the 1s{sub 1/2} and 2s{sub 1/2} levels is found. The difference {Delta}E{sub L}(1s{sub 1/2}) {minus} 8{Delta}E{sub L}(2s{sub 1/2}) for the hydrogen atom is found to be {minus}187.236(11) MHz. 13 refs., 2 figs.

  20. Continuous coherent Lyman- alpha excitation of atomic hydrogen.

    PubMed

    Eikema, K S; Walz, J; Hänsch, T W

    2001-06-18

    The 1S-2P transition in atomic hydrogen has been observed for the first time with almost natural linewidth. We employ a unique source of continuous coherent Lyman- alpha radiation based on four-wave mixing in mercury. The output of the source has been improved 40-fold to yield 20 nW. This demonstration shows that laser cooling and detection with continuous Lyman- alpha radiation has excellent prospects for future experiments with antihydrogen.

  1. Continuous Coherent Lyman-{alpha} Excitation of Atomic Hydrogen

    SciTech Connect

    Eikema, K. S. E.; Walz, J.; Hansch, T. W.

    2001-06-18

    The 1S{minus}2P transition in atomic hydrogen has been observed for the first time with almost natural linewidth. We employ a unique source of continuous coherent Lyman-{alpha} radiation based on four-wave mixing in mercury. The output of the source has been improved 40-fold to yield 20nW. This demonstration shows that laser cooling and detection with continuous Lyman-{alpha} radiation has excellent prospects for future experiments with antihydrogen.

  2. Amide-Substituted Titanocenes in Hydrogen-Atom Transfer Catalysis.

    PubMed

    Zhang, Yong-Qiang; Jakoby, Verena; Stainer, Katharina; Schmer, Alexander; Klare, Sven; Bauer, Mirko; Grimme, Stefan; Cuerva, Juan Manuel; Gansäuer, Andreas

    2016-01-22

    Two new catalytic systems for hydrogen-atom transfer (HAT) catalysis involving the N-H bonds of titanocene(III) complexes with pendant amide ligands are reported. In a monometallic system, a bifunctional catalyst for radical generation and reduction through HAT catalysis depending on the coordination of the amide ligand is employed. The pendant amide ligand is used to activate Crabtree's catalyst to yield an efficient bimetallic system for radical generation and HAT catalysis. PMID:26636435

  3. Uranium Adsorbent Fibers Prepared by Atom-Transfer Radical Polymerization from Chlorinated Polypropylene and Polyethylene Trunk Fibers

    SciTech Connect

    Brown, Suree; Chatterjee, Sabornie; Li, Meijun; Yue, Yanfeng; Tsouris, Costas; Janke, Christopher J.; Saito, Tomonori; Dai, Sheng

    2015-12-10

    Seawater contains a large amount of uranium (~4.5 billion tons) which can serve as a limitless supply of an energy source. However, in order to make the recovery of uranium from seawater economically feasible, lower manufacturing and deployment costs are required, and thus, solid adsorbents must have high uranium uptake, reusability, and high selectivity toward uranium. In this study, atom-transfer radical polymerization (ATRP), without the radiation-induced graft polymerization (RIGP), was used for grafting acrylonitrile (AN) and tert-butyl acrylate (tBA) from a new class of trunk fibers, forming adsorbents in a readily deployable form. The new class of trunk fibers was prepared by the chlorination of PP round fiber, hollow-gear-shaped PP fiber, and hollow-gear-shaped PE fiber. During ATRP, degrees of grafting (d.g.) varied according to the structure of active chlorine sites on trunk fibers and ATRP conditions, and the d.g. as high as 2570% was obtained. Resulting adsorbent fibers were evaluated in U-spiked simulated seawater and the maximum adsorption capacity of 146.6 g U/kg, much higher than that of a standard adsorbent JAEA fiber (75.1 g/kg), was obtained. This new type of trunk fibers can be used for grafting a variety of uranium-interacting ligands, including designed ligands that are highly selective toward uranium.

  4. Uranium Adsorbent Fibers Prepared by Atom-Transfer Radical Polymerization from Chlorinated Polypropylene and Polyethylene Trunk Fibers

    DOE PAGES

    Brown, Suree; Chatterjee, Sabornie; Li, Meijun; Yue, Yanfeng; Tsouris, Costas; Janke, Christopher J.; Saito, Tomonori; Dai, Sheng

    2015-12-10

    Seawater contains a large amount of uranium (~4.5 billion tons) which can serve as a limitless supply of an energy source. However, in order to make the recovery of uranium from seawater economically feasible, lower manufacturing and deployment costs are required, and thus, solid adsorbents must have high uranium uptake, reusability, and high selectivity toward uranium. In this study, atom-transfer radical polymerization (ATRP), without the radiation-induced graft polymerization (RIGP), was used for grafting acrylonitrile (AN) and tert-butyl acrylate (tBA) from a new class of trunk fibers, forming adsorbents in a readily deployable form. The new class of trunk fibers wasmore » prepared by the chlorination of PP round fiber, hollow-gear-shaped PP fiber, and hollow-gear-shaped PE fiber. During ATRP, degrees of grafting (d.g.) varied according to the structure of active chlorine sites on trunk fibers and ATRP conditions, and the d.g. as high as 2570% was obtained. Resulting adsorbent fibers were evaluated in U-spiked simulated seawater and the maximum adsorption capacity of 146.6 g U/kg, much higher than that of a standard adsorbent JAEA fiber (75.1 g/kg), was obtained. This new type of trunk fibers can be used for grafting a variety of uranium-interacting ligands, including designed ligands that are highly selective toward uranium.« less

  5. Alkane desaturation by concerted double hydrogen atom transfer to benzyne.

    PubMed

    Niu, Dawen; Willoughby, Patrick H; Woods, Brian P; Baire, Beeraiah; Hoye, Thomas R

    2013-09-26

    The removal of two vicinal hydrogen atoms from an alkane to produce an alkene is a challenge for synthetic chemists. In nature, desaturases and acetylenases are adept at achieving this essential oxidative functionalization reaction, for example during the biosynthesis of unsaturated fatty acids, eicosanoids, gibberellins and carotenoids. Alkane-to-alkene conversion almost always involves one or more chemical intermediates in a multistep reaction pathway; these may be either isolable species (such as alcohols or alkyl halides) or reactive intermediates (such as carbocations, alkyl radicals, or σ-alkyl-metal species). Here we report a desaturation reaction of simple, unactivated alkanes that is mechanistically unique. We show that benzynes are capable of the concerted removal of two vicinal hydrogen atoms from a hydrocarbon. The discovery of this exothermic, net redox process was enabled by the simple thermal generation of reactive benzyne intermediates through the hexadehydro-Diels-Alder cycloisomerization reaction of triyne substrates. We are not aware of any single-step, bimolecular reaction in which two hydrogen atoms are simultaneously transferred from a saturated alkane. Computational studies indicate a preferred geometry with eclipsed vicinal C-H bonds in the alkane donor.

  6. Manufacture and deflagration of an atomic hydrogen propellant

    NASA Technical Reports Server (NTRS)

    Rosen, G.

    1974-01-01

    It is observed that the use of very low temperatures (in the range from 0.1 to 1.5 K) produced by advanced cryogenic apparatus and the use of very strong magnetic fields (in the range from 50 to 100 kG) produced by superconducting magnets can yield a significant improvement in the atomic hydrogen trapping effectiveness of an H2 matrix. The use of a radioactive beta-ray emiter isotope may yield H-H2 propellants (with a specific impulse of about 740 sec) by secondary electron impact dissociations of H2 in an impregnated matrix maintained below 1 K in a strong magnetic field. Another method for manufacturing an H-H2 propellant involves bombardment of supercooled solid H2 with a cyclotron-produced beam of 10-MeV hydrogen atoms. The matrix-isolated atomic hydrogen must be used directly without prior melting as a solid propellant, and an analysis of the steady deflagration is presented.

  7. An experimental limit on parity mixing in atomic hydrogen

    SciTech Connect

    Fehrenbach, C.C.W.

    1993-12-31

    An experiment was performed to detect the forbidden E1 transition between two hyperfine levels of the 2S state of atomic hydrogen. Such a transition, with {Delta}l = 0, violates parity symmetry. The technique used was to induce an interference between the forbidden transition and a parity-allowed E1 transition polarized by a DC electric field. The two induced transitions were driven coherently in a single microwave cavity. A magnetic field was used to shift the atoms into resonance with the RF radiation and to make the 2S and 2P states degenerate in energy, which would maximize any parity-violating mixing between these states. The measurements were made by passing a beam of hydrogen through the microwave cavity, and monitoring the state of the emerging atoms. To separate the parity-violating component of the transition rate from the parity-conserving part, the change in the transition rate was monitored when the handedness of the interaction region was reversed. From the transition asymmetry it was possible to extract the size of the proton-spin dependent part of a general parity-violating interaction between an electron and a proton. This can be stated in terms of a dimensionless constant C{sub 2}. The result of this experiment is C{sub 2p} = 1.5 {plus_minus} 22. The error bound represents a 95% confidence level and is an improvement of an order of magnitude over previous limits set by similar experiments in hydrogen.

  8. The hydrogen atom in plasmas with an external electric field

    SciTech Connect

    Bahar, M. K.; Soylu, A.

    2014-09-15

    We numerically solve the Schrödinger equation, using a more general exponential cosine screened Coulomb (MGECSC) potential with an electric field, in order to investigate the screening and weak external electric field effects on the hydrogen atom in plasmas. The MGECSC potential is examined for four different cases, corresponding to different screening parameters of the potential and the external electric field. The influences of the different screening parameters and the weak external electric field on the energy eigenvalues are determined by solving the corresponding equations using the asymptotic iteration method (AIM). It is found that the corresponding energy values shift when a weak external electric field is applied to the hydrogen atom in a plasma. This study shows that a more general exponential cosine screened Coulomb potential allows the influence of an applied, weak, external electric field on the hydrogen atom to be investigated in detail, for both Debye and quantum plasmas simultaneously. This suggests that such a potential would be useful in modeling similar effects in other applications of plasma physics, and that AIM is an appropriate method for solving the Schrödinger equation, the solution of which becomes more complex due to the use of the MGECSC potential with an applied external electric field.

  9. A First Principles study on Boron-doped Graphene decorated by Ni-Ti-Mg atoms for Enhanced Hydrogen Storage Performance

    NASA Astrophysics Data System (ADS)

    Nachimuthu, Santhanamoorthi; Lai, Po-Jung; Leggesse, Ermias Girma; Jiang, Jyh-Chiang

    2015-11-01

    We proposed a new solid state material for hydrogen storage, which consists of a combination of both transition and alkaline earth metal atoms decorating a boron-doped graphene surface. Hydrogen adsorption and desorption on this material was investigated using density functional theory calculations. We find that the diffusion barriers for H atom migration and desorption energies are lower than for the previously designed mediums and the proposed medium can reach the gravimetric capacity of ~6.5 wt % hydrogen, which is much higher than the DOE target for the year 2015. Molecular Dynamics simulations show that metal atoms are stably adsorbed on the B doped graphene surface without clustering, which will enhance the hydrogen storage capacity.

  10. A First Principles study on Boron-doped Graphene decorated by Ni-Ti-Mg atoms for Enhanced Hydrogen Storage Performance

    PubMed Central

    Nachimuthu, Santhanamoorthi; Lai, Po-Jung; Leggesse, Ermias Girma; Jiang, Jyh-Chiang

    2015-01-01

    We proposed a new solid state material for hydrogen storage, which consists of a combination of both transition and alkaline earth metal atoms decorating a boron-doped graphene surface. Hydrogen adsorption and desorption on this material was investigated using density functional theory calculations. We find that the diffusion barriers for H atom migration and desorption energies are lower than for the previously designed mediums and the proposed medium can reach the gravimetric capacity of ~6.5 wt % hydrogen, which is much higher than the DOE target for the year 2015. Molecular Dynamics simulations show that metal atoms are stably adsorbed on the B doped graphene surface without clustering, which will enhance the hydrogen storage capacity. PMID:26577659

  11. Zero-Temperature Structures of Atomic Metallic Hydrogen

    NASA Astrophysics Data System (ADS)

    McMahon, Jeffrey; Ceperley, David

    2011-03-01

    Since the first prediction of an atomic metallic phase of hydrogen by Wigner and Huntington over 75 years ago, there have been many theoretical efforts aimed at determining the crystal structures of the zero-temperature phases. We present results from ab initio random structure searching with density functional theory performed to determine the ground state structures from 500 GPa to 5 TPa. We estimate that molecular hydrogen dissociates into a monatomic body-centered tetragonal structure near 500 GPa (rs = 1.225), which then remains stable to 2.5 TPa (rs = 0.969). At higher pressures, hydrogen stabilizes in an . . . ABCABC . . . planar structure that is remarkably similar to the ground state of lithium, which compresses to the face-centered cubic lattice beyond 5 TPa (rs < 0.86). Our results provide a complete ab initio description of the atomic metallic crystal structures of hydrogen, resolving one of the most fundamental and long outstanding issues concerning the structures of the elements.

  12. The atomic hydrogen cloud in the saturnian system

    NASA Astrophysics Data System (ADS)

    Tseng, W.-L.; Johnson, R. E.; Ip, W.-H.

    2013-09-01

    The importance of Titan's H torus shaped by solar radiation pressure and of hydrogen atoms flowing out of Saturn's atmosphere in forming the broad hydrogen cloud in Saturn's magnetosphere is still debated. Since the Saturnian system also contains a water product torus which originates from the Enceladus plumes, the icy ring particles, and the inner icy satellites, as well as Titan's H2 torus, we have carried out a global investigation of the atomic hydrogen cloud taking into account all sources. We show that the velocity and angle distributions of the hot H ejected from Saturn's atmosphere following electron-impact dissociation of H2 are modified by collisions with the ambient atmospheric H2 and H. This in turn affects the morphology of the escaping hydrogen from Saturn, as does the morphology of the ionospheric electron distribution. Although an exact agreement with the Cassini observations is not obtained, our simulations show that H directly escaping from Titan is the dominant contributor in the outer magnetosphere. Of the total number of H observed by Cassini from 1 to 5RS, ∼5.7×1034, our simulations suggest ∼20% is from dissociation in the Enceladus torus, ∼5-10% is from dissociation of H2 in the atmosphere of the main rings, and ∼50% is from Titan's H torus, implying that ∼20% comes from Saturn atmosphere.

  13. Reactions of atomic hydrogen in water : solvent and isotope effects.

    SciTech Connect

    Bartels, D. M.

    1999-06-10

    It has been known for many years that hydrogen atoms can be easily created and studied in water using radiolytic techniques [1]. The use of CW EPR detection coupled with electron radiolysis proved extremely useful in estimating many reaction rates, and revealed the interesting phenomenon of chemically induced dynamic electron polarization (CIDEP) [2]. In recent years, we have made use of pulsed EPR detection to make precision reaction rate measurements which avoid the complications of CIDEP [3]. Activation energies and H/D isotope effects measured in these studies [4-14] will be described below. An interesting aspect of the hydrogen atom reactions is the effect of hydrophobic solvation. EPR evidence--an almost gas-phase hyperfine coupling and extremely narrow linewidth--is quite convincing to show that the H atom is just a minimally perturbed gas phase atom inside a small ''bubble''. In several systems we have found that the hydrophobic free energy of solvation dominates the solvent effect on reaction rates.

  14. Reactions of butadiyne. 1: The reaction with hydrogen atoms

    NASA Technical Reports Server (NTRS)

    Schwanebeck, W.; Warnatz, J.

    1984-01-01

    The reaction of hydrogen (H) atoms with butadiene (C4H2) was studied at room temperature in a pressure range between w mbar and 10 mbar. The primary step was an addition of H to C4H2 which is in its high pressure range at p 1 mbar. Under these conditions the following addition of a second H atom lies in the transition region between low and high pressure range. Vibrationally excited C4H4 can be deactivated to form buten-(1)-yne-(3)(C4H4) or decomposes into two C2H2 molecules. The rate constant at room temperature for primary step is given. The second order rate constant for the consumption of buten-(1)-yne-(3) is an H atom excess at room temperature is given.

  15. Ultrafast effective multilevel atom method for primordial hydrogen recombination

    SciTech Connect

    Ali-Haiemoud, Yacine; Hirata, Christopher M.

    2010-09-15

    Cosmological hydrogen recombination has recently been the subject of renewed attention because of its importance for predicting the power spectrum of cosmic microwave background anisotropies. It has become clear that it is necessary to account for a large number n > or approx. 100 of energy shells of the hydrogen atom, separately following the angular momentum substates in order to obtain sufficiently accurate recombination histories. However, the multilevel atom codes that follow the populations of all these levels are computationally expensive, limiting recent analyses to only a few points in parameter space. In this paper, we present a new method for solving the multilevel atom recombination problem, which splits the problem into a computationally expensive atomic physics component that is independent of the cosmology and an ultrafast cosmological evolution component. The atomic physics component follows the network of bound-bound and bound-free transitions among excited states and computes the resulting effective transition rates for the small set of 'interface' states radiatively connected to the ground state. The cosmological evolution component only follows the populations of the interface states. By pretabulating the effective rates, we can reduce the recurring cost of multilevel atom calculations by more than 5 orders of magnitude. The resulting code is fast enough for inclusion in Markov chain Monte Carlo parameter estimation algorithms. It does not yet include the radiative transfer or high-n two-photon processes considered in some recent papers. Further work on analytic treatments for these effects will be required in order to produce a recombination code usable for Planck data analysis.

  16. Hydrogen atom density in narrow-gap microwave hydrogen plasma determined by calorimetry

    NASA Astrophysics Data System (ADS)

    Yamada, Takahiro; Ohmi, Hiromasa; Kakiuchi, Hiroaki; Yasutake, Kiyoshi

    2016-02-01

    The density of hydrogen (H) atoms in the narrow-gap microwave hydrogen plasma generated under high-pressure conditions is expected to be very high because of the high input power density of the order of 104 W/cm3. For measuring the H atom density in such a high-pressure and high-density plasma, power-balance calorimetry is suited since a sufficient signal to noise ratio is expected. In this study, H atom density in the narrow-gap microwave hydrogen plasma has been determined by the power-balance calorimetry. The effective input power to the plasma is balanced with the sum of the powers related to the out-going energy per unit time from the plasma region via heat conduction, outflow of high-energy particles, and radiation. These powers can be estimated by simple temperature measurements using thermocouples and optical emission spectroscopy. From the power-balance data, the dissociation fraction of H2 molecules is determined, and the obtained maximum H atom density is (1.3 ± 0.2) × 1018 cm-3. It is found that the H atom density increases monotonically with increasing the energy invested per one H2 molecule within a constant plasma volume.

  17. Concerted hydrogen atom exchange between three HF molecules

    NASA Technical Reports Server (NTRS)

    Komornicki, Andrew; Dixon, David A.; Taylor, Peter R.

    1992-01-01

    We have investigated the termolecular reaction involving concerted hydrogen exchange between three HF molecules, with particular emphasis on the effects of correlation at the various stationary points along the reaction. Using an extended basis, we have located the geometries of the stable hydrogen-bonded trimer, which is of C(sub 3h) symmetry, and the transition state for hydrogen exchange, which is of D(sub 3h) symmetry. The energies of the exchange reation were then evaluated at the correlated level, using a large atomic natural orbital basis and correlating all valence electrons. Several correlation treatments were used, namely, configration interaction with single and double excitations, coupled-pair functional, and coupled-cluster methods. We are thus able to measure the effect of accounting for size-extensivity. Zero-point corrections to the correlated level energetics were determined using analytic second derivative techniques at the SCF level. Our best calculations, which include the effects of connected triple excitations in the coupled-cluster procedure, indicate that the trimer is bound by 9 +/- 1 kcal/mol relative to three separate monomers, in excellent agreement with previous estimates. The barrier to concerted hydrogen exchange is 15 kcal/mol above the trimer, or only 4.7 kcal/mol above three separated monomers. Thus the barrier to hydrogen exchange between HF molecules via this termolecular process is very low.

  18. Hydrogen-hydrogen interaction in planar biphenyl: a theoretical study based on the interacting quantum atoms and Hirshfeld atomic energy partitioning methods.

    PubMed

    Eskandari, Kiamars; Van Alsenoy, Christian

    2014-10-01

    The nature of H-H interaction between ortho-hydrogen atoms in planar biphenyl is investigated by two different atomic energy partitioning methods, namely fractional occupation iterative Hirshfeld (FOHI) and interacting quantum atoms (IQA), and compared with the traditional virial-based approach of quantum theory of atoms in molecules (QTAIM). In agreement with Bader's hypothesis of H-H bonding, partitioning the atomic energy into intra-atomic and interatomic terms reveals that there is a net attractive interaction between the ortho-hydrogens in the planar biphenyl. This falsifies the classical view of steric repulsion between the hydrogens. In addition, in contrast to the traditional QTAIM energy analysis, both FOHI and IQA show that the total atomic energy of the ortho-hydrogens remains almost constant when they participate in the H-H interaction. Although, the interatomic part of atomic energy of the hydrogens plays a stabilizing role during the formation of the H-H bond, it is almost compensated by the destabilizing effects of the intra-atomic parts and consequently, the total energy of the hydrogens remains constant. The trends in the changes of intra-atomic and interatomic energy terms of ortho-hydrogens during H-H bond formation are very similar to those observed for the H2 molecule.

  19. Role of Double Hydrogen Atom Transfer Reactions in Atmospheric Chemistry.

    PubMed

    Kumar, Manoj; Sinha, Amitabha; Francisco, Joseph S

    2016-05-17

    Hydrogen atom transfer (HAT) reactions are ubiquitous and play a crucial role in chemistries occurring in the atmosphere, biology, and industry. In the atmosphere, the most common and traditional HAT reaction is that associated with the OH radical abstracting a hydrogen atom from the plethora of organic molecules in the troposphere via R-H + OH → R + H2O. This reaction motif involves a single hydrogen transfer. More recently, in the literature, there is an emerging framework for a new class of HAT reactions that involves double hydrogen transfers. These reactions are broadly classified into four categories: (i) addition, (ii) elimination, (iii) substitution, and (iv) rearrangement. Hydration and dehydration are classic examples of addition and elimination reactions, respectively whereas tautomerization or isomerization belongs to a class of rearrangement reactions. Atmospheric acids and water typically mediate these reactions. Organic and inorganic acids are present in appreciable levels in the atmosphere and are capable of facilitating two-point hydrogen bonding interactions with oxygenates possessing an hydroxyl and/or carbonyl-type functionality. As a result, acids influence the reactivity of oxygenates and, thus, the energetics and kinetics of their HAT-based chemistries. The steric and electronic effects of acids play an important role in determining the efficacy of acid catalysis. Acids that reduce the steric strain of 1:1 substrate···acid complex are generally better catalysts. Among a family of monocarboxylic acids, the electronic effects become important; barrier to the catalyzed reaction correlates strongly with the pKa of the acid. Under acid catalysis, the hydration of carbonyl compounds leads to the barrierless formation of diols, which can serve as seed particles for atmospheric aerosol growth. The hydration of sulfur trioxide, which is the principle mechanism for atmospheric sulfuric acid formation, also becomes barrierless under acid catalysis

  20. Role of Double Hydrogen Atom Transfer Reactions in Atmospheric Chemistry.

    PubMed

    Kumar, Manoj; Sinha, Amitabha; Francisco, Joseph S

    2016-05-17

    Hydrogen atom transfer (HAT) reactions are ubiquitous and play a crucial role in chemistries occurring in the atmosphere, biology, and industry. In the atmosphere, the most common and traditional HAT reaction is that associated with the OH radical abstracting a hydrogen atom from the plethora of organic molecules in the troposphere via R-H + OH → R + H2O. This reaction motif involves a single hydrogen transfer. More recently, in the literature, there is an emerging framework for a new class of HAT reactions that involves double hydrogen transfers. These reactions are broadly classified into four categories: (i) addition, (ii) elimination, (iii) substitution, and (iv) rearrangement. Hydration and dehydration are classic examples of addition and elimination reactions, respectively whereas tautomerization or isomerization belongs to a class of rearrangement reactions. Atmospheric acids and water typically mediate these reactions. Organic and inorganic acids are present in appreciable levels in the atmosphere and are capable of facilitating two-point hydrogen bonding interactions with oxygenates possessing an hydroxyl and/or carbonyl-type functionality. As a result, acids influence the reactivity of oxygenates and, thus, the energetics and kinetics of their HAT-based chemistries. The steric and electronic effects of acids play an important role in determining the efficacy of acid catalysis. Acids that reduce the steric strain of 1:1 substrate···acid complex are generally better catalysts. Among a family of monocarboxylic acids, the electronic effects become important; barrier to the catalyzed reaction correlates strongly with the pKa of the acid. Under acid catalysis, the hydration of carbonyl compounds leads to the barrierless formation of diols, which can serve as seed particles for atmospheric aerosol growth. The hydration of sulfur trioxide, which is the principle mechanism for atmospheric sulfuric acid formation, also becomes barrierless under acid catalysis

  1. Heat capacity measurements of atoms and molecules adsorbed on evaporated metal films

    SciTech Connect

    Kenny, T.W.

    1989-05-01

    Investigations of the properties of absorbed monolayers have received great experimental and theoretical attention recently, both because of the importance of surface processes in practical applications such as catalysis, and the importance of such systems to the understanding of the fundamentals of thermodynamics in two dimensions. We have adapted the composite bolometer technology to the construction of microcalorimeters. For these calorimeters, the adsorption substrate is an evaporated film deposited on one surface of an optically polished sapphire wafer. This approach has allowed us to make the first measurements of the heat capacity of submonolayer films of /sup 4/He adsorbed on metallic films. In contrast to measurements of /sup 4/He adsorbed on all other insulating substrates, we have shown that /sup 4/He on silver films occupies a two-dimensional gas phase over a broad range of coverages and temperatures. Our apparatus has been used to study the heat capacity of Indium flakes. CO multilayers, /sup 4/He adsorbed on sapphire and on Ag films and H/sub 2/ adsorbed on Ag films. The results are compared with appropriate theories. 68 refs., 19 figs.

  2. Thermal hydrogen-atom transfer from methane: A mechanistic exercise

    NASA Astrophysics Data System (ADS)

    Schwarz, Helmut

    2015-06-01

    Hydrogen-atom transfer (HAT) constitutes a key process in a broad range of chemical transformations as it covers heterogeneous, homogeneous, and enzymatic reactions. While open-shell metal oxo species [MO]rad are no longer regarded as being involved in the heterogeneously catalyzed oxidative coupling of methane (2CH4 + → C2H6 + H2O), these reagents are rather versatile in bringing about (gas-phase) hydrogen-atom transfer, even from methane at ambient conditions. In this mini-review, various mechanistic scenarios will be presented, and it will be demonstrated how these are affected by the composition of the metal-oxide cluster ions. Examples will be discussed, how 'doping' the clusters permits the control of the charge and spin situation at the active site and, thus, the course of the reaction. Also, the interplay between supposedly inert support material and the active site - the so-called 'aristocratic atoms' - of the gas-phase catalyst will be addressed. Finally, gas-phase HAT from methane will be analyzed in the broader context of thermal activation of inert Csbnd H bonds by metal-oxo species.

  3. Pt atoms adsorbed on TiO2(110 ) -(1 ×1 ) studied with noncontact atomic force microscopy and first-principles simulations

    NASA Astrophysics Data System (ADS)

    Fernández-Torre, Delia; Yurtsever, Ayhan; Onoda, Jo; Abe, Masayuki; Morita, Seizo; Sugimoto, Yoshiaki; Pérez, Rubén

    2015-02-01

    We have studied the local properties of single Pt atoms adsorbed on hydroxylated TiO2(110 ) -(1 ×1 ) by combining noncontact atomic force microscopy (nc-AFM) and first-principles calculations. Room-temperature high-resolution nc-AFM images for the most frequently observed contrast modes reveal bright and elongated protrusions that can be traced back to the Pt atoms, and that are centered on the fivefold coordinated titanium rows, confined between two bridging oxygen rows. These observations are in line with the theoretical results, as the lowest energy sites for the Pt atom on the TiO2(110 ) surface are in the neighborhood of the titanium rows, and high energy barriers have to be overcome to displace the Pt atom over the bridging oxygen rows. Single Pt atoms can be distinguished from H adsorbates (OH defects) due to their characteristic shape and binding site and, because they appear as the brightest surface features in all of the contrast modes. Force spectroscopy data over the protrusion and hole imaging modes and the corresponding tip-sample forces, simulated with O and OH terminated TiO2 nanoclusters, provide an explanation for this puzzling result in terms of the intrinsic strength of the interaction with the Pt adatom and the adatom and tip apex relaxations induced by the tip-sample interaction. These imaging mechanisms can be extended to other electropositive metal dopants and support the use of nc-AFM not only to characterize their adsorption structure but also to directly probe their chemical reactivity.

  4. Kinetic modeling of α-hydrogen abstractions from unsaturated and saturated oxygenate compounds by hydrogen atoms.

    PubMed

    Paraskevas, Paschalis D; Sabbe, Maarten K; Reyniers, Marie-Françoise; Papayannakos, Nikos G; Marin, Guy B

    2014-10-01

    Hydrogen-abstraction reactions play a significant role in thermal biomass conversion processes, as well as regular gasification, pyrolysis, or combustion. In this work, a group additivity model is constructed that allows prediction of reaction rates and Arrhenius parameters of hydrogen abstractions by hydrogen atoms from alcohols, ethers, esters, peroxides, ketones, aldehydes, acids, and diketones in a broad temperature range (300-2000 K). A training set of 60 reactions was developed with rate coefficients and Arrhenius parameters calculated by the CBS-QB3 method in the high-pressure limit with tunneling corrections using Eckart tunneling coefficients. From this set of reactions, 15 group additive values were derived for the forward and the reverse reaction, 4 referring to primary and 11 to secondary contributions. The accuracy of the model is validated upon an ab initio and an experimental validation set of 19 and 21 reaction rates, respectively, showing that reaction rates can be predicted with a mean factor of deviation of 2 for the ab initio and 3 for the experimental values. Hence, this work illustrates that the developed group additive model can be reliably applied for the accurate prediction of kinetics of α-hydrogen abstractions by hydrogen atoms from a broad range of oxygenates. PMID:25209711

  5. Electron structure of AgCl nanocrystal with silver ion adsorbed on atomic-rough surface and quantum transitions

    NASA Astrophysics Data System (ADS)

    Timoshenko, Yury K.; Shunina, Valentina A.

    2009-08-01

    Adsorption was considered as on the atomically-rough surface (near the step and step fracture) as on the smooth surface. The electron structure of AgCl nanocrystals with the adsorbed silver ion were calculated by semiempirical tight-binding method relying on a self-consistent approach for the effective charges and dipole moments of the ions and in frame of DFT method B3LYP/HW. The quantum transitions were investigated in semiempirical approach. Visualization of the wave functions was performed for the localized states. Basing on the obtained data a conclusion is specically made that one can expect an enhancement of photoelectron localization with a decrease of the anions number in the substrate nearest to the adsorbed ion. It means that the most ecient trapping of photoelectron should occur under adsorption on a smooth surface rather than near the steps and their fractures as it was assumed previously. Also probabilities of quantum transitions for AgCl : J nanocrystal with the adsorbed silver ion were been discussed. This work is a continuation of paper [1].

  6. The confined hydrogen atom: a linear variational approach

    NASA Astrophysics Data System (ADS)

    Aquino, N.; Rojas, R. A.

    2016-01-01

    We study the size effect on the confinement of a hydrogen atom in a spherical box of impenetrable walls. We compute the energy of the ground and a few excited states as a function of the box radius R c . To obtain the energy eigenvalues and eigenfunctions we utilize the linear variational method via a basis set of free-particle-in-a-box wave functions. For small values of R c convergence is attained with a small number of basis set functions, whereas for R c ≥ 5.0 au, it is necessary to use over 100 terms in the expansion.

  7. Electron-impact-ionization cross section for the hydrogen atom

    NASA Astrophysics Data System (ADS)

    Hu, W.; Fang, D.; Wang, Y.; Yang, F.

    1994-02-01

    A distorted-wave Born exchange approximation was used to calculate the cross section for electron-impact ionization of the hydrogen atoms. Both the integral and energy-differential cross section were calculated. The results were compared with the latest experimental data and other theoretical calculations. Comparison shows that the calculations agree with differential cross-section measurements in general. For integral cross sections the calculation shows a better agreement with an earlier measurement [M.B. Shah, D. S. Elliott, and H. B. Gilbody, J. Phys. B 20, 3501 (1987)] in which the cross sections are normalized to the first Born approximation.

  8. Atomic hydrogen cleaning of GaAS Photocathodes

    SciTech Connect

    M. Poelker; J. Price; C. Sinclair

    1997-01-01

    It is well known that surface contaminants on semiconductors can be removed when samples are exposed to atomic hydrogen. Atomic H reacts with oxides and carbides on the surface, forming compounds that are liberated and subsequently pumped away. Experiments at Jefferson lab with bulk GaAs in a low-voltage ultra-high vacuum H cleaning chamber have resulted in the production of photocathodes with high photoelectron yield (i.e., quantum efficiency) and long lifetime. A small, portable H cleaning apparatus also has been constructed to successfully clean GaAs samples that are later removed from the vacuum apparatus, transported through air and installed in a high-voltage laser-driven spin-polarized electron source. These results indicate that this method is a versatile and robust alternative to conventional wet chemical etching procedures usually employed to clean bulk GaAs.

  9. Microwave ionization of hydrogen atoms: Experiment vs classical dynamics

    SciTech Connect

    van Leeuwen, K.A.H.; Oppen, G.V.; Renwick, S.; Bowlin, J.B.; Koch, P.M.; Jensen, R.V.; Rath, O.; Richards, D.; Leopold, J.G.

    1985-11-18

    Ionization of hydrogen atoms with principal quantum number n = 32, 40, and 51--74 by a 9.92-GHz electric field F(t)zF0 cos t was studied with a superimposed static electric field F-bar/sub s/ = 0,2,5,8 V/cm. The measured field strengths F0(10%) at which 10% of the atoms were ionized are in excellent agreement with classical calculations in both one and two spatial dimensions. Covering finer detail as well as gross structure of the n dependence of F0(10%), the agreement supports the application of classical dynamics to the analysis of this strongly perturbed quantum system.

  10. Classical and quantum dynamics of the impulsively driven hydrogen atom

    SciTech Connect

    Melles, M.; Reinhold, C.O.; Burgdoerfer, J. |

    1992-12-01

    We investigate the classical and quantum dynamics of the hydrogen atom in a Rydberg state subject to a sequence of periodic and random pulses. One goal of this study is to test the validity of classical electron transport theories. We analyze the critical momentum transfer for which 10% of the Rydberg atoms are ionized after a large number of pulses as a function of the frequency of the perturbation. The quantum mechanical results for a periodic sequence of pulses exhibit clear structures which are not present in a classical simulation. These structures are shown to vanish for the case of stochastic pulses for which agreement is obtained between the classical and quantum mechanical results. The dynamics of the quantum mechanical periodic system is analyzed in terms of quasi-eigenstates of the period-one time evolution operator.

  11. Classical and quantum dynamics of the impulsively driven hydrogen atom

    SciTech Connect

    Melles, M.; Reinhold, C.O.; Burgdoerfer, J. Oak Ridge National Lab., TN )

    1992-01-01

    We investigate the classical and quantum dynamics of the hydrogen atom in a Rydberg state subject to a sequence of periodic and random pulses. One goal of this study is to test the validity of classical electron transport theories. We analyze the critical momentum transfer for which 10% of the Rydberg atoms are ionized after a large number of pulses as a function of the frequency of the perturbation. The quantum mechanical results for a periodic sequence of pulses exhibit clear structures which are not present in a classical simulation. These structures are shown to vanish for the case of stochastic pulses for which agreement is obtained between the classical and quantum mechanical results. The dynamics of the quantum mechanical periodic system is analyzed in terms of quasi-eigenstates of the period-one time evolution operator.

  12. Ionization of atomic hydrogen by 30 1000 keV antiprotons

    SciTech Connect

    Knudsen, H.; Mikkelsen, U.; Paludan, K.; Kirsebom, K.; Moller, S.P.; Uggerhoj, E.; Slevin, J.; Charlton, M.; Morenzoni, E.

    1995-06-05

    Ionization in collisions between antiprotons and atomic hydrogen is perhaps the least complicated and most fundamental process that can be treated by atomic-collision theory. We present measurements of the ionization cross section for 30--1000 keV antiprotons colliding with atomic hydrogen.

  13. 1,2-shifts of hydrogen atoms in aryl radicals

    SciTech Connect

    Brooks, M.A.; Scott, L.T.

    1999-06-16

    An energy barrier on the order of 60 kcal/mol is predicted for the 1,2-shift of hydrogen atoms in aryl radicals. Such rearrangements are, therefore, not expected to occur under ordinary laboratory conditions, but they should be prevalent in the aryl radicals formed during combustion, flash vacuum pyrolysis, and other high-temperature gas-phase processes. As a demonstration of this rearrangement, the 2-benzo[c]phenanthryl radical (1) was generated by flash vacuum pyrolysis of the corresponding aryl bromide. A 1,2-shift of hydrogen out of the sterically congested cover region of 1, followed by cyclization and rearomatization of the resulting radical, is proposed to explain the observation of benzo[ghi]fluoranthene as the dominant monomeric product formed. Under the same conditions, [1,3,4,5-{sup 2}H{sub 4}]-2-bromobenzo[c]phenanthrene gives [1,2,3,4-{sup 2}H{sub 4}]-benzo[ghi]fluoranthene as the dominant monomeric product, in accord with the expectation of a deuterium atom 1,2-shift.

  14. Hydrogen-like atom with nonnegative quantum distribution function

    SciTech Connect

    Zorin, A. V. Sevastianov, L. A.

    2007-04-15

    Among numerous approaches to probabilistic interpretation of conventional quantum mechanics (CQM), the closest to N. Bohr's idea of the correspondence principle is the Blokhintzev-Terletsky approach of the quantum distribution function (QDF) on the coordinate-momentum (q, p) phase space. The detailed investigation of this approach has led to the correspondence rule of V.V. Kuryshkin parametrically dependent on a set of auxiliary functions. According to investigations of numerous authors, the existence and the explicit form of QDF depends on the correspondence rule between classical functions A(q, p) and quantum operator A. At the same time, the QDF corresponding to all known quantization rules turns out to be alternating in sign or overly complex valued. Finally nonexistence of nonnegative QDF in CQM was proved. On the other hand, from this follows the possibility to construct quantum mechanics where a nonnegative QDF exists. We consider a certain set of auxiliary functions to construct explicit expressions for operators O(H) for the hydrogen atom. Naturally, these operators differ from the related operator H in CQM, so that spherical coordinates are no longer separable for a hydrogen-like atom in quantum mechanics with nonnegative QDF.

  15. Hot hydrogen atom reactions moderated by H2 and He

    NASA Technical Reports Server (NTRS)

    Aronowitz, S.; Scattergood, T.; Flores, J.; Chang, S.

    1986-01-01

    Photolysis experiments were performed on the H2-CD4-NH3 and He-CD4-NH3 systems. The photolysis (1849 A) involved only NH3. Mixtures of H2:CD4:NH3 included all combinations of the ratios (200,400,800):(10,20,40):4. Two He:CD4:NH3 mixtures were examined where the ratios equalled the combinations 100:(10,20):4. Abstraction of a D from CD4 by the photolytically produced hot hydrogen from ammonia was monitored by mass spectrometric determination of HD. Both experiment and semiempirical hot-atom theory show that H2 is a very poor thermalizer of hot hydrogens with excess kinetic energy of about 2 eV. Applications of the hard-sphere collision model to the H2-CD4-NH3 system resulted in predicted ratios of net HD production to NH3 decomposition that were two orders of magnitude smaller than the experimental ratios. On the other hand, helium is found to be a very efficient thermalizer; here, the classical model yields reasonable agreement with experiments. Application of a semiempirical hot-atom program gave quantitative agreement with experiment for either system.

  16. Atomic hydrogen for low temperature atomic hydrogen masers and in-vacuum dissociators for VLG-11 series masers

    NASA Technical Reports Server (NTRS)

    Vessot, R. F. C.

    1984-01-01

    The operation of a cryogenically-cooled hydrogen maser using an RF plasma dissociator operating at liquid nitrogen temperature (77K) in confunction with a state selector magnet whose dimensions are suitable for slow atoms is studied. The focusing characteristics for a hexapole state selector magnet with maximum fields at the pole tips, provide a maximum acceptance angle for atoms at the most probable velocity in the beam. By thermally isolating the RF circuitry from the dissociator glassware, only dielectric losses in the glass and the energy coupled to the plasma will result in the boil-off of liquid nitrogen. It is estimated that this is about one watt and thus a loss rate of approximately .022 liters pr hour is anticipated.

  17. Plasma Effects on the Metastable Neutral HYDROGEN(2S) Atom.

    NASA Astrophysics Data System (ADS)

    Benage, John Ferns, Jr.

    Atomic radiative processes which occur in plasmas have long been of interest of plasma physicists. The process we are investigating is atomic dipole transitions, specifically transitions from the metastable 2s to the 2p in hydrogen, which are induced by processes which occur in the plasma. An experiment was done to measure the rate of transitions from 2s to 2p in hydrogen. This experiment was divided into two sections. The first was to measure the transition rate in a near equilibrium plasma. The second section measured the transition rate when RF oscillations were imposed on the plasma. The results of the first part of the experiment show that microscopic fluctuating electric fields which are produced by the motions of the charged particles induce transitions from 2s to 2p in hydrogen. The magnitude of this effect is compared to predicted transition rates due to collisions with electrons and ions and to rates predicted for an equilibrium plasma. In the second part of the experiment, the plasma was shown to act as a filter, preventing transitions from being caused by the RF unless the RF was in the range where plasma waves could be launched. The interpretation we give for this effect is that when the oscillations are inducing transitions, it is because plasma waves are being launched in the plasma and it is these waves which are inducing the transitions. These results have a couple of important applications. The results for the equilibrium part of the experiment can be used to explain a limit in the current which is produced by the Lamb-shift polarized ion source. The other important application is the possible use of the effect seen in the RF case as a non-perturbing diagnostic for plasma waves. Since dipole transition rates are proportional to E('2) and very sensitive near resonance, this effect could prove to be more accurate and more sensitive than methods currently used.

  18. Infrared spectroscopy of water clusters co-adsorbed with hydrogen molecules on a sodium chloride film

    NASA Astrophysics Data System (ADS)

    Yamakawa, Koichiro; Fukutani, Katsuyuki

    2016-06-01

    Hydrogen gas containing a trace of water vapor was dosed on a vacuum-evaporated sodium chloride film at 13 K, and water clusters formed on the substrate were investigated by infrared absorption spectroscopy. Absorption bands due to (H2O)n clusters with n = 3-6 and an induced absorption band due to hydrogen were clearly observed. With increasing gas dosage, the intensities of the cluster bands increased linearly while the intensity of the hydrogen band was constant. This suggests that the water clusters were formed in two-dimensional matrices of hydrogen. We found that the water clusters did exist on the surface upon heating even after the hydrogen molecules had desorbed. A further rise of the substrate temperature up to 27 K yielded the formation of larger clusters, (H2O)n with n > 6 . We also discuss the origins of the two bands of the trimer in terms of pseudorotation and a metastable isomer.

  19. Evaluation of Hydrogen Isotope Exchange Methodology on Adsorbents for Tritium Removal

    DOE PAGES

    Morgan, Gregg A.; Xiao, S. Xin

    2015-03-06

    The Savannah River National Laboratory has demonstrated a potential process that can be used to remove tritium from tritiated water using Pt-catalyzed molecular sieves. The process is an elemental isotope exchange process in which H2 (when flowed through the molecular sieves) will exchange with the adsorbed water, D2O, leaving H2O adsorbed on the molecular sieves. Various formulations of catalyzed molecular sieve material were prepared using two different techniques, Pt-implantation and Pt-ion exchange. This technology has been demonstrated for a protium (H) and deuterium (D) system, but can also be used for the removal of tritium from contaminated water (T2O, HTO,more » and DTO) using D2 (or H2)« less

  20. Evaluation of Hydrogen Isotope Exchange Methodology on Adsorbents for Tritium Removal

    SciTech Connect

    Morgan, Gregg A.; Xiao, S. Xin

    2015-03-06

    The Savannah River National Laboratory has demonstrated a potential process that can be used to remove tritium from tritiated water using Pt-catalyzed molecular sieves. The process is an elemental isotope exchange process in which H2 (when flowed through the molecular sieves) will exchange with the adsorbed water, D2O, leaving H2O adsorbed on the molecular sieves. Various formulations of catalyzed molecular sieve material were prepared using two different techniques, Pt-implantation and Pt-ion exchange. This technology has been demonstrated for a protium (H) and deuterium (D) system, but can also be used for the removal of tritium from contaminated water (T2O, HTO, and DTO) using D2 (or H2)

  1. Evaluation of hydrogen isotope exchange methodology on adsorbents for tritium removal

    SciTech Connect

    Morgan, G.A.; Xin Xiao, S.

    2015-03-15

    The Savannah River National Laboratory has demonstrated a potential process that can be used to remove tritium from tritiated water using Pt-catalyzed molecular sieves. The process is an elemental isotope exchange process in which H{sub 2} (when flowed through the molecular sieves) will exchange with the adsorbed water, D{sub 2}O, leaving H{sub 2}O adsorbed on the molecular sieves. Various formulations of catalyzed molecular sieve material were prepared using two different techniques, Pt-implantation and Pt-ion exchange. This technology has been demonstrated for a protium (H) and deuterium (D) system, but can also be used for the removal of tritium from contaminated water (T{sub 2}O, HTO, and DTO) using D{sub 2} (or H{sub 2}). (authors)

  2. Structural, electronic, and magnetic properties of transition-metal atom adsorbed two-dimensional GaAs nanosheet

    NASA Astrophysics Data System (ADS)

    Luo, Jia; Xiang, Gang; Yu, Tian; Lan, Mu; Zhang, Xi

    2016-09-01

    By using first-principles calculations within the framework of density functional theory, the electronic and magnetic properties of 3d transitional metal (TM) atoms (from Sc to Zn) adsorbed monolayer GaAs nanosheets (GaAsNSs) are systematically investigated. Upon TM atom adsorption, GaAsNS, which is a nonmagnetic semiconductor, can be tuned into a magnetic semiconductor (Sc, V, and Fe adsorption), a half-metal (Mn adsorption), or a metal (Co and Cu adsorption). Our calculations show that the strong p–d hybridization between the 3d orbit of TM atoms and the 4p orbit of neighboring As atoms is responsible for the formation of chemical bonds and the origin of magnetism in the GaAsNSs with Sc, V, and Fe adsorption. However, the Mn 3d orbit with more unpaired electrons hybridizes not only with the As 4p orbit but also with the Ga 4p orbit, resulting in a stronger exchange interaction. Our results may be useful for electronic and magnetic applications of GaAsNS-based materials. Project supported by the National Natural Science Foundation of China (Grant No. 11174212).

  3. Gold atom and dimer adsorbed on perfect and defective graphene and boron nitride monolayer: A first-principles study

    NASA Astrophysics Data System (ADS)

    Li, Guihua; Li, Feng; Wang, Xiaopeng; Zhao, Mingwen; Liu, Xiangdong

    2014-05-01

    Energetic and structural properties of gold atom (Au) and gold dimer (Au dimer) adsorbed on pristine and defective graphene (Gra) and boron nitride monolayer (BN) are investigated using density functional theory. Substitutional doping models in the neutral charge state are considered by replacing the C site in graphene with B or N atom impurities (Gra-CB and Gra-CN) or by doping the B or N sites in the BN sheet by a C atom (BN-BC and BN-NC). It is shown that while the binding of Au/Au-dimer to a pristine support is weak, stronger binding could be achieved by introducing a defect in the surface indicating that defects can trap metal atoms. It is found that Gra-CB and BN-NC support Au/Au-dimer well and BN-NC is more preferable from aspect of adsorption energy. Interaction between Au/Au-dimer and the BN-NC substrates is explained by assigning appropriate partial charge densities of the valence band maximum (VBM) and conduction band minimum (CBM) at the Г point and projected densities of states (PDOS). The results demonstrate that both pristine and defective BN surfaces can no longer be treated as inert supports for Au/Au-dimer.

  4. Structural, electronic, and magnetic properties of transition-metal atom adsorbed two-dimensional GaAs nanosheet

    NASA Astrophysics Data System (ADS)

    Luo, Jia; Xiang, Gang; Yu, Tian; Lan, Mu; Zhang, Xi

    2016-09-01

    By using first-principles calculations within the framework of density functional theory, the electronic and magnetic properties of 3d transitional metal (TM) atoms (from Sc to Zn) adsorbed monolayer GaAs nanosheets (GaAsNSs) are systematically investigated. Upon TM atom adsorption, GaAsNS, which is a nonmagnetic semiconductor, can be tuned into a magnetic semiconductor (Sc, V, and Fe adsorption), a half-metal (Mn adsorption), or a metal (Co and Cu adsorption). Our calculations show that the strong p-d hybridization between the 3d orbit of TM atoms and the 4p orbit of neighboring As atoms is responsible for the formation of chemical bonds and the origin of magnetism in the GaAsNSs with Sc, V, and Fe adsorption. However, the Mn 3d orbit with more unpaired electrons hybridizes not only with the As 4p orbit but also with the Ga 4p orbit, resulting in a stronger exchange interaction. Our results may be useful for electronic and magnetic applications of GaAsNS-based materials. Project supported by the National Natural Science Foundation of China (Grant No. 11174212).

  5. The ground state properties of spin-aligned atomic hydrogen, deuterium, and tritium

    NASA Technical Reports Server (NTRS)

    Etters, R. D.; Dugan, J. V., Jr.; Palmer, R. W.

    1975-01-01

    The internal energy, pressure, and compressibility of ground-state, spin-aligned atomic hydrogen, deuterium, and tritium are calculated assuming that all pair interactions occur via the atomic triplet (spin-aligned) potential. The conditions required to obtain atomic hydrogen and its isotopes in bulk are discussed; such a development would be of value in propulsion systems because of the light mass and energetic recombination of atomic hydrogen. Results show that atomic triplet hydrogen and deuterium remain gaseous at 0 K, and that tritium forms a liquid with a binding energy of approximately -0.75 K per atom at a molar volume of 130 cu cm per mole. The pair distribution function for these systems is calculated, and the predicted superfluid behavior of atomic triplet hydrogen and tritium is briefly discussed.

  6. Changes in the morphology of interstellar ice analogues after hydrogen atom exposure.

    PubMed

    Accolla, Mario; Congiu, Emanuele; Dulieu, François; Manicò, Giulio; Chaabouni, Henda; Matar, Elie; Mokrane, Hakima; Lemaire, Jean Louis; Pirronello, Valerio

    2011-05-01

    The morphology of water ice in the interstellar medium is still an open question. Although accretion of gaseous water could not be the only possible origin of the observed icy mantles covering dust grains in cold molecular clouds, it is well known that water accreted from the gas phase on surfaces kept at 10 K forms ice films that exhibit a very high porosity. It is also known that in the dark clouds H(2) formation occurs on the icy surface of dust grains and that part of the energy (4.48 eV) released when adsorbed atoms react to form H(2) is deposited in the ice. The experimental study described in the present work focuses on how relevant changes of the ice morphology result from atomic hydrogen exposure and subsequent recombination. Using the temperature-programmed desorption (TPD) technique and a method of inversion analysis of TPD spectra, we show that there is an exponential decrease in the porosity of the amorphous water ice sample following D-atom irradiation. This decrease is inversely proportional to the thickness of the ice and has a value of ϕ(0) = 2 × 10(16) D-atoms cm(-2) per layer of H(2)O. We also use a model which confirms that the binding sites on the porous ice are destroyed regardless of their energy depth, and that the reduction of the porosity corresponds in fact to a reduction of the effective area. This reduction appears to be compatible with the fraction of D(2) formation energy transferred to the porous ice network. Under interstellar conditions, this effect is likely to be efficient and, together with other compaction processes, provides a good argument to believe that interstellar ice is amorphous and non-porous.

  7. Atomic interactions and phase transition in hydrogen metal systems

    SciTech Connect

    Shirley, A.I.

    1985-01-01

    The statistical mechanical behavior of H in pure metals and metal alloys is investigated using elasticity theory and lattice-gas models. The interactions between H atoms are separated into elastic and electronic contributions, and only the elastic contributions are evaluated. Three studies are reported: trapping of H by interstitial and substitutional impurities in bbc metals; modeling of H in impure metals; and modeling of H in concentration metal hydrides. The elastic interactions between H and interstitial and substitutional impurities in bbc metals are calculated using the method of lattice statics. Comparison with experimentally-measured trapping energies indicates that trapping by interstitial impurities is due solely to elastic energy, whereas both elastic and electronic interactions contribute to trapping by substitutional impurities. To include the effect of substitutional trapping on the phase transitions of H in metal alloys, the random-field lattice-gas model is developed. Interactions between H atoms are determined using the effective metal atom approximation. Hydrogen-impurity interactions are treated as a random field, in analogy with the random-field Ising model. Phase diagrams of the Nb/sub .95/Mo/sub .05/-H and Nb/sub .85/Mo/sub .15/-H systems are calculated by Monte Carlo simulation using the random-field model. The model gives qualitatively correct predictions of the phase behavior when the random field is included.

  8. Hydrogen atom abstraction from organometallic hydrogen sources: First kinetics of H atom abstraction by benzyl radical from `Mo-S-H`

    SciTech Connect

    Birbaum, J.C.; Franz, J.A.; Linehan, J.C.

    1997-12-31

    Hydrogen transfers are very important in catalytic and stoichiometric organometallic reaction schemes, yet few kinetic studies of the transfers from a metal hydride to an organic radical have been performed. To our knowledge there are no kinetic studies of hydrogen atom transfers from atoms attached to metals such as sulfur or oxygen. We present the first study with the extremely fast hydrogen atom transfer from (CpMoSSH){sub 2} to benzyl radical. The rate constant for this reaction was found to be greater than 10{sup 6} M{sup -1}s{sup -1} at room temperature.

  9. Atomic-scale observation of hydrogen-induced crack growth by atom-probe FIM. [Fe-0. 29% Ti

    SciTech Connect

    Kuk, Y.; Pickering, H.W.; Sakurai, T.

    1980-01-01

    Formation and propagation of a microcrack due to hydrogen in a Fe-0.29 wt.% Ti alloy was observed at the atomic scale by field ion microscopy. A microcrack (-20 nm in length) formed and became noticeably large when the tip was heated at 950/sup 0/C in the presence of about 1 torr of Hg. Propagation was reported several times by reheating, until a portion of the tip ruptured and became detached from the tip. Compositional analysis, performed in situ using a high performance atom-probe, identified atomic hydrogen in quantity and some hydrogen molecules and FEH in the crack, but not elsewhere on the surface.

  10. Positron impact excitations of hydrogen atom embedded in weakly coupled plasmas: Formation of Rydberg atoms

    SciTech Connect

    Rej, Pramit; Ghoshal, Arijit

    2014-09-15

    Formation of Rydberg atoms due to 1s→nlm excitations of hydrogen, for arbitrary n, l, m, by positron impact in weakly coupled plasma has been investigated using a distorted-wave theory in the momentum space. The interactions among the charged particles in the plasma have been represented by Debye-Huckel potentials. Making use of a simple variationally determined wave function for the hydrogen atom, it has been possible to obtain the distorted-wave scattering amplitude in a closed analytical form. A detailed study has been made on the effects of plasma screening on the differential and total cross sections in the energy range 20–300 eV of incident positron. For the unscreened case, our results agree nicely with some of the most accurate results available in the literature. To the best of our knowledge, such a study on the differential and total cross sections for 1s→nlm inelastic positron-hydrogen collisions for arbitrary n, l, m in weakly coupled plasmas is the first reported in the literature.

  11. The role of vdW interactions in coverage dependent adsorption energies of atomic adsorbates on Pt(111) and Pd(111)

    NASA Astrophysics Data System (ADS)

    Thirumalai, Hari; Kitchin, John R.

    2016-08-01

    Adsorption, a fundamental process in heterogeneous catalysis is known to be dependent on the adsorbate-adsorbate and surface-adsorbate bonds. van der Waals (vdW) interactions are one of the types of interactions that have not been examined thoroughly as a function of adsorbate coverage. In this work we quantify the vdW interactions for atomic adsorbates on late transition metal surfaces, and determine how these long range forces affect the coverage dependent adsorption energies. We calculate the adsorption energies of carbon, nitrogen, oxygen, sulfur, fluorine, bromine and chlorine species on Pt(111) and Pd(111) at coverages ranging from 1/4 to 1 ML using the BEEF-vdW functional. We observe that adsorption energies remain coverage dependent, and this coverage dependence is shown to be statistically significant. vdW interactions are found to be coverage dependent, but more significantly, they are found to be dependent on molecular properties such as adsorbate size, and consequently, correlate with the adsorbate effective nuclear charge. We observe that these interactions account for a reduction in the binding energy of the system, due to the destabilizing attractive interactions between the adsorbates which weaken its bond with the surface.

  12. Theory of catalytic dissociation of hydrogen atoms on a metal surface

    SciTech Connect

    Konstantinov, O. V. Dymnikov, V. D.; Mittsev, M. A.

    2008-08-15

    The model of hydrogen atom ionization near a metal surface is discussed on the basis of a comparison between the metal work function and the atom ionization energy. In the theoretical calculation, it is shown that the hydrogen atom ionization energy decreases when the atom approaches the metal surface. The ionization energy vanishes when the distance between proton and the metal surface is somewhat less than the Bohr radius.

  13. X-ray emission spectroscopy applied to glycine adsorbed on Cu(110): An atom and symmetry projected view

    SciTech Connect

    Hasselstroem, J.; Karis, O.; Weinelt, M.

    1997-04-01

    When a molecule is adsorbed on a metal surface by chemical bonding new electronic states are formed. For noble and transition metals these adsorption-induced states overlap with the much more intense metal d-valence band, making them difficult to probe by for instance direct photoemission. However, it has recently been shown that X-ray emission spectroscopy (XES) can be applied to adsorbate systems. Since the intermediate state involves a core hole, this technique has the power to project out the partial density of states around each atomic site. Both the excitation and deexcitation processes are in general governed by the dipole selection rules. For oriented system, it is hence possible to obtain a complete separation into 2p{sub x}, 2p{sub y} and 2p{sub z} contributions using angular resolved measurements. The authors have applied XES together with other core level spectroscopies to glycine adsorption on Cu(110). Glycine (NH{sub 2}CH{sub 2}COOH) is the smallest amino acid and very suitable to study by core level spectroscopy since it has several functional groups, all well separated in energy by chemical shifts. Its properties are futhermore of biological interest. In summary, the authors have shown that it is possible to apply XES to more complicated molecular adsorbates. The assignment of different electronic states is however not as straight forward as for simple diatomic molecules. For a complete understanding of the redistribution and formation of new electronic states associated with the surface chemical bond, experimental data must be compared to theoretical calculations.

  14. Two-photon photoemission investigation of electronic and dynamical properties of alkali atoms adsorbed on noble metal surfaces

    NASA Astrophysics Data System (ADS)

    Sametoglu, Vahit

    We present a systematic time-resolved two-photon photoemission study of the electronic and dynamical properties of Li through Cs adsorbed on Cu(111) and Ag(111) surfaces. A fundamental problem in surface science is how to describe the electronic structure of a chemisorption interface based on the intrinsic properties of the interacting materials. Because of their simple s-electron structure, elements of the alkali atom group comprise paradigmatic adsorbates in many theories of chemisorption, whereas the complementary experimental studies are sparse and incomplete. Through a combination of spectroscopic and femtosecond time-resolved surface measurements, we are able to probe systematically the binding energies, symmetries, and electron and nuclear relaxation dynamics of the initially unoccupied alkali atom resonances. As a prelude, we study the two-photon photoemission process occurring at the bare Ag(111) surface. We develop a quantitative model for two-photon photoemission process, where the nonresonant and k-dependent two-photon absorption between the lower and upper sp-bands is modeled by the optical Bloch equations, and the angle-dependent intensities are described by the Fresnel equations. Our two-photon photoemission spectra of Li through Cs chemisorbed Cu(111) and Ag(111) surfaces reveal two resonances with the m = 0 and m = +/-1 symmetry ('m' is the projection of the orbital angular momentum 'l' onto the surface plane). For the m = 0 resonance, which is derived from the hybridization of the ns and npz orbitals of alkali atoms, we find a binding energy of 1.84--1.99 eV below the vacuum level, which is independent of the alkali atom period, and tunes with coverage in a universal manner. At 0.3--0.7 eV higher energy, we discover and identify the m = +/-1 resonance by its characteristic angular intensity distribution, which derives from the antisymmetry of the npx and npy orbitals. We implement a quantitative model for the alkali atom chemisorption based on the

  15. Entropy and complexity analysis of hydrogenic Rydberg atoms

    NASA Astrophysics Data System (ADS)

    López-Rosa, S.; Toranzo, I. V.; Sánchez-Moreno, P.; Dehesa, J. S.

    2013-05-01

    The internal disorder of hydrogenic Rydberg atoms as contained in their position and momentum probability densities is examined by means of the following information-theoretic spreading quantities: the radial and logarithmic expectation values, the Shannon entropy, and the Fisher information. As well, the complexity measures of Crámer-Rao, Fisher-Shannon, and López Ruiz-Mancini-Calvet types are investigated in both reciprocal spaces. The leading term of these quantities is rigorously calculated by use of the asymptotic properties of the concomitant entropic functionals of the Laguerre and Gegenbauer orthogonal polynomials which control the wavefunctions of the Rydberg states in both position and momentum spaces. The associated generalized Heisenberg-like, logarithmic and entropic uncertainty relations are also given. Finally, application to linear (l = 0), circular (l = n - 1), and quasicircular (l = n - 2) states is explicitly done.

  16. Phase Space Structures Explain Hydrogen Atom Roaming in Formaldehyde Decomposition.

    PubMed

    Mauguière, Frédéric A L; Collins, Peter; Kramer, Zeb C; Carpenter, Barry K; Ezra, Gregory S; Farantos, Stavros C; Wiggins, Stephen

    2015-10-15

    We re-examine the prototypical roaming reaction--hydrogen atom roaming in formaldehyde decomposition--from a phase space perspective. Specifically, we address the question "why do trajectories roam, rather than dissociate through the radical channel?" We describe and compute the phase space structures that define and control all possible reactive events for this reaction, as well as provide a dynamically exact description of the roaming region in phase space. Using these phase space constructs, we show that in the roaming region, there is an unstable periodic orbit whose stable and unstable manifolds define a conduit that both encompasses all roaming trajectories exiting the formaldehyde well and shepherds them toward the H2···CO well.

  17. Inelastic cross sections for positron scattering from atomic hydrogen

    SciTech Connect

    Weber, M.; Hofmann, A.; Raith, W.; Sperber, W.; Jacobsen, F.; Lynn, K.G.

    1994-12-31

    Positronium formation (Ps) cross sections for positrons impinging on atomic hydrogen were measured in the impact energy range from 13eV to 255eV at the High Intensity Positron (HIP) beam at Brookhaven National Laboratory (BNL). The Ps-formation cross section was found to rise rapidly from the threshold at 6.8eV to a maximum value of (2.98 {plus_minus} 0.18) {times} 10{sup {minus}16} cm{sup 2} for {approx} 15eV positrons. By 75eV it drops below the detection limit of 0.17 {times} 10{sup {minus}16} cm{sup 2} which is the present level of statistical uncertainty. The experiment was modified to enable the measurement of doubly differential scattering cross sections.

  18. Ionization of atomic hydrogen in strong infrared laser fields

    SciTech Connect

    Grum-Grzhimailo, Alexei N.; Abeln, Brant; Bartschat, Klaus; Weflen, Daniel; Urness, Timothy

    2010-04-15

    We have used the matrix iteration method of Nurhuda and Faisal [Phys. Rev. A 60, 3125 (1999)] to treat ionization of atomic hydrogen by a strong laser pulse. After testing our predictions against a variety of previous calculations, we present ejected-electron spectra as well as angular distributions for few-cycle infrared laser pulses with peak intensities of up to 10{sup 15} W/cm{sup 2}. It is shown that the convergence of the results with the number of partial waves is a serious issue, which can be managed in a satisfactory way by using the velocity form of the electric dipole operator in connection with an efficient time-propagation scheme.

  19. Entropy and complexity analysis of hydrogenic Rydberg atoms

    SciTech Connect

    Lopez-Rosa, S.; Toranzo, I. V.; Dehesa, J. S.; Sanchez-Moreno, P.

    2013-05-15

    The internal disorder of hydrogenic Rydberg atoms as contained in their position and momentum probability densities is examined by means of the following information-theoretic spreading quantities: the radial and logarithmic expectation values, the Shannon entropy, and the Fisher information. As well, the complexity measures of Cramer-Rao, Fisher-Shannon, and Lopez Ruiz-Mancini-Calvet types are investigated in both reciprocal spaces. The leading term of these quantities is rigorously calculated by use of the asymptotic properties of the concomitant entropic functionals of the Laguerre and Gegenbauer orthogonal polynomials which control the wavefunctions of the Rydberg states in both position and momentum spaces. The associated generalized Heisenberg-like, logarithmic and entropic uncertainty relations are also given. Finally, application to linear (l= 0), circular (l=n- 1), and quasicircular (l=n- 2) states is explicitly done.

  20. Cold collisions of atomic hydrogen with antihydrogen atoms: An optical potential approach

    SciTech Connect

    Zygelman, B.; Saenz, Alejandro; Froelich, P.; Jonsell, S.

    2004-04-01

    We present a theory that describes the interaction of hydrogen atoms with antihydrogen at subkelvin temperatures. The formalism includes a nonlocal complex optical potential, whose imaginary component describes the breakup of the H-H-bar complex into positronium and protonium fragments. Using ab inito methods, we construct the imaginary part of the optical potential and calculate the cross sections for fragmentation in ultracold collisions of H and H-bar. We find a 35% reduction in the value of the scattering length from that obtained in the Born-Oppenheimer approximation. We estimate the lifetimes for quasibound states of this complex to fragment into a protonium-positronium pair.

  1. Bonding Configurations and Collective Patterns of Ge Atoms Adsorbed on Si(111)-(7×7)

    SciTech Connect

    Wang, Y.; Gao, H.; Guo, H. M.; Wang, Sanwu; Pantelides, Sokrates T

    2005-01-01

    We report scanning tunneling microscopy observations of Ge deposited on the Si(111)-(7 x 7) surface for a sequence of submonolayer coverages. We demonstrate that Ge atoms replace so-called Si adatoms. Initially, the replacements are random, but distinct patterns emerge and evolve with increasing coverage, until small islands begin to form. Corner adatom sites in the faulted half unit cells are preferred. First-principles density functional calculations find that adatom substitution competes energetically with a high-coordination bridge site, but atoms occupying the latter sites are highly mobile. Thus, the observed structures are indeed more thermodynamically stable.

  2. Transient absorption spectra of the laser-dressed hydrogen atom

    NASA Astrophysics Data System (ADS)

    Murakami, Mitsuko; Chu, Shih-I.

    2013-10-01

    We present a theoretical study of transient absorption spectra of laser-dressed hydrogen atoms, based on numerical solutions of the time-dependent Schrödinger equation. The timing of absorption is controlled by the delay between an extreme ultra violet (XUV) pulse and an infrared (IR) laser field. The XUV pulse is isolated and several hundred attoseconds in duration, which acts as a pump to drive the ground-state electron to excited p states. The subsequent interaction with the IR field produces dressed states, which manifest as sidebands between the 1s-np absorption spectra separated by one IR-photon energy. We demonstrate that the population of dressed states is maximized when the timing of the XUV pulse coincides with the zero crossing of the IR field, and that their energies can be manipulated in a subcycle time scale by adding a chirp to the IR field. An alternative perspective to the problem is to think of the XUV pulse as a probe to detect the dynamical ac Stark shifts. Our results indicate that the accidental degeneracy of the hydrogen excited states is removed while they are dressed by the IR field, leading to large ac Stark shifts. Furthermore, we observe the Autler-Townes doublets for the n=2 and 3 levels using the 656 nm dressing field, but their separation does not agree with the prediction by the conventional three-level model that neglects the dynamical ac Stark shifts.

  3. Positron scattering from hydrogen atom embedded in dense quantum plasma

    SciTech Connect

    Bhattacharya, Arka; Kamali, M. Z. M.; Ghoshal, Arijit; Ratnavelu, K.

    2013-08-15

    Scattering of positrons from the ground state of hydrogen atoms embedded in dense quantum plasma has been investigated by applying a formulation of the three-body collision problem in the form of coupled multi-channel two-body Lippmann-Schwinger equations. The interactions among the charged particles in dense quantum plasma have been represented by exponential cosine-screened Coulomb potentials. Variationally determined hydrogenic wave function has been employed to calculate the partial-wave scattering amplitude. Plasma screening effects on various possible mode of fragmentation of the system e{sup +}+H(1s) during the collision, such as 1s→1s and 2s→2s elastic collisions, 1s→2s excitation, positronium formation, elastic proton-positronium collisions, have been reported in the energy range 13.6-350 eV. Furthermore, a comparison has been made on the plasma screening effect of a dense quantum plasma with that of a weakly coupled plasma for which the plasma screening effect has been represented by the Debye model. Our results for the unscreened case are in fair agreement with some of the most accurate results available in the literature.

  4. Quantum dynamics of hydrogen atoms on graphene. II. Sticking

    SciTech Connect

    Bonfanti, Matteo; Jackson, Bret; Hughes, Keith H.; Burghardt, Irene

    2015-09-28

    Following our recent system-bath modeling of the interaction between a hydrogen atom and a graphene surface [Bonfanti et al., J. Chem. Phys. 143, 124703 (2015)], we present the results of converged quantum scattering calculations on the activated sticking dynamics. The focus of this study is the collinear scattering on a surface at zero temperature, which is treated with high-dimensional wavepacket propagations with the multi-configuration time-dependent Hartree method. At low collision energies, barrier-crossing dominates the sticking and any projectile that overcomes the barrier gets trapped in the chemisorption well. However, at high collision energies, energy transfer to the surface is a limiting factor, and fast H atoms hardly dissipate their excess energy and stick on the surface. As a consequence, the sticking coefficient is maximum (∼0.65) at an energy which is about one and half larger than the barrier height. Comparison of the results with classical and quasi-classical calculations shows that quantum fluctuations of the lattice play a primary role in the dynamics. A simple impulsive model describing the collision of a classical projectile with a quantum surface is developed which reproduces the quantum results remarkably well for all but the lowest energies, thereby capturing the essential physics of the activated sticking dynamics investigated.

  5. Quantum dynamics of hydrogen atoms on graphene. II. Sticking.

    PubMed

    Bonfanti, Matteo; Jackson, Bret; Hughes, Keith H; Burghardt, Irene; Martinazzo, Rocco

    2015-09-28

    Following our recent system-bath modeling of the interaction between a hydrogen atom and a graphene surface [Bonfanti et al., J. Chem. Phys. 143, 124703 (2015)], we present the results of converged quantum scattering calculations on the activated sticking dynamics. The focus of this study is the collinear scattering on a surface at zero temperature, which is treated with high-dimensional wavepacket propagations with the multi-configuration time-dependent Hartree method. At low collision energies, barrier-crossing dominates the sticking and any projectile that overcomes the barrier gets trapped in the chemisorption well. However, at high collision energies, energy transfer to the surface is a limiting factor, and fast H atoms hardly dissipate their excess energy and stick on the surface. As a consequence, the sticking coefficient is maximum (∼0.65) at an energy which is about one and half larger than the barrier height. Comparison of the results with classical and quasi-classical calculations shows that quantum fluctuations of the lattice play a primary role in the dynamics. A simple impulsive model describing the collision of a classical projectile with a quantum surface is developed which reproduces the quantum results remarkably well for all but the lowest energies, thereby capturing the essential physics of the activated sticking dynamics investigated. PMID:26429029

  6. Quantum effects of hydrogen atoms on the dynamical rearrangement of hydrogen-bond networks in liquid water.

    PubMed

    Hyeon-Deuk, Kim; Ando, Koji

    2010-04-28

    Quantum effects such as zero-point energy and delocalization of wave packets (WPs) representing water hydrogen atoms are essential to understand anomalous energetics and dynamics in water. Since quantum calculations of many-body dynamics are highly complicated, no one has yet directly viewed the quantum WP dynamics of hydrogen atoms in liquid water. Our semiquantum molecular dynamics simulation made it possible to observe the hydrogen WP dynamics in liquid water. We demonstrate that the microscopic WP dynamics are closely correlated with and actually play key roles in the dynamical rearrangement in the hydrogen-bond network (HBN) of bulk water. We found the quantum effects of hydrogen atoms on liquid water dynamics such as the rearrangement of HBN and the concomitant fluctuation and relaxation. Our results provide new physical insights on HBN dynamics in water whose significance is not limited to pure liquid dynamics but also a greater understanding of chemical and biological reactions in liquid water.

  7. Schrodinger Equation Solutions that Lead to the Solution for the Hydrogen Atom

    ERIC Educational Resources Information Center

    Newhouse, Paul F.; McGill, K.C.

    2004-01-01

    Two exercises that would provide beginning quantum theory students with an introduction to more advanced quantum mechanical treatments, especially the hydrogen atom are given. The exercises are stepwise in difficulty, leading naturally to the full hydrogen atom development and greatly extend the pedagogy of most multidimensional Cartesian systems…

  8. Which hydrogen atom of toluene protonates PAH molecules in (+)-mode APPI MS analysis?

    PubMed

    Ahmed, Arif; Ghosh, Manik Kumer; Choi, Myung Chul; Choi, Cheol Ho; Kim, Sunghwan

    2013-03-01

    A previous study (Ahmed, A. et al., Anal. Chem. 84, 1146-1151( 2012) reported that toluene used as a solvent was the proton source for polyaromatic hydrocarbon compounds (PAHs) that were subjected to (+)-mode atmospheric-pressure photoionization. In the current study, the exact position of the hydrogen atom in the toluene molecule (either a methyl hydrogen or an aromatic ring hydrogen) involved in the formation of protonated PAH ions was investigated. Experimental analyses of benzene and anisole demonstrated that although the aromatic hydrogen atom of toluene did not contribute to the formation of protonated anthracene, it did contribute to the formation of protonated acridine. Thermochemical data and quantum mechanical calculations showed that the protonation of anthracene by an aromatic ring hydrogen atom of toluene is endothermic, while protonation by a methyl hydrogen atom is exothermic. However, protonation of acridine by either an aromatic ring hydrogen or a methyl hydrogen atom of toluene is exothermic. The different behavior of acridine and anthracene was attributed to differences in gas-phase basicity. It was concluded that both types of hydrogen in toluene can be used for protonation of PAH compounds, but a methyl hydrogen atom is preferred, especially for non-basic compounds.

  9. The structures and dynamics of atomic and molecular adsorbates on metal surfaces by scanning tunneling microscopy and low energy electron diffraction

    SciTech Connect

    Yoon, Hyungsuk Alexander

    1996-12-01

    Studies of surface structure and dynamics of atoms and molecules on metal surfaces are presented. My research has focused on understanding the nature of adsorbate-adsorbate and adsorbate-substrate interactions through surface studies of coverage dependency and coadsorption using both scanning tunneling microscopy (STM) and low energy electron diffraction (LEED). The effect of adsorbate coverage on the surface structures of sulfur on Pt(111) and Rh(111) was examined. On Pt(111), sulfur forms p(2x2) at 0.25 ML of sulfur, which transforms into a more compressed ({radical}3x{radical}3)R30{degrees} at 0.33 ML. On both structures, it was found that sulfur adsorbs only in fcc sites. When the coverage of sulfur exceeds 0.33 ML, it formed more complex c({radical}3x7)rect structure with 3 sulfur atoms per unit cell. In this structure, two different adsorption sites for sulfur atoms were observed - two on fcc sites and one on hcp site within the unit cell.

  10. Positron impact excitations of hydrogen atom embedded in dense quantum plasmas: Formation of Rydberg atoms

    SciTech Connect

    Rej, Pramit; Ghoshal, Arijit

    2014-11-15

    Formation of Rydberg atoms due to 1 s → nlm excitations of hydrogen by positron impact, for arbitrary n, l, m, in dense quantum plasma has been investigated using a distorted wave theory which includes screened dipole polarization potential. The interactions among the charged particles in the plasma have been represented by exponential cosine-screened Coulomb potentials. Making use of a simple variationally determined hydrogen wave function, it has been possible to obtain the distorted wave scattering amplitude in a closed analytical form. A detailed study has been made to explore the structure of differential and total cross sections in the energy range 20–300 eV of incident positron. For the unscreened case, our results agree nicely with some of the most accurate results available in the literature. To the best of our knowledge, such a study on the differential and total cross sections for 1 s → nlm inelastic positron-hydrogen collisions in dense quantum plasma is the first reported in the literature.

  11. Magnetic Properties of High-Surface-Area Carbons and Their Effect on Adsorbed Hydrogen

    NASA Astrophysics Data System (ADS)

    Romanos, Jimmy; Beckner, Matthew; Kraus, Michael; Burress, Jacob; Pfeifer, Peter

    2009-03-01

    We report the discovery that a large number of nanoporous carbon samples, made from corn cob and exhibiting high hydrogen storage capacities (Pfeifer et al, Mater. Res. Soc. Symp. Proc. 1041 R02-02 (2008)), show unexpected magnetic properties, due to iron impurities in the samples. Magnetization curves are consistent with ferromagnetic and/or super-paramagnetic behavior. Magnetic susceptibilities, saturation magnetizations, coercivities and remanence magnetizations, from measurements on a SQUID magnetometer, will be presented, and their temperature dependence will be discussed. Results will be presented regarding the presence of small iron clusters, magnetic properties of iron-leached samples, and hydrogen binding energies as a function of iron leaching. This material is based on work supported by the U.S. Department of Energy under Award No. DE-FG-08GO18142.

  12. New horizons in chemical propulsion. [processes using free radicals, atomic hydrogen, excited species, etc

    NASA Technical Reports Server (NTRS)

    Cohen, W.

    1973-01-01

    After a review of the work of the late-Fifties on free radicals for propulsion, it is concluded that atomic hydrogen would provide a potentially large increase in specific impulse. Work conducted to find an approach for isolating atomic hydrogen is considered. Other possibilities for obtaining propellants of greatly increased capability might be connected with the technology for the generation of activated states of gases, metallic hydrogen, fuels obtained from other planets, and laser transfer of energy.

  13. Adsorption isotherms and structure of cationic surfactants adsorbed on mineral oxide surfaces prepared by atomic layer deposition.

    PubMed

    Wangchareansak, Thipvaree; Craig, Vincent S J; Notley, Shannon M

    2013-12-01

    The adsorption isotherms and aggregate structures of adsorbed surfactants on smooth thin-film surfaces of mineral oxides have been studied by optical reflectometry and atomic force microscopy (AFM). Films of the mineral oxides of titania, alumina, hafnia, and zirconia were produced by atomic layer deposition (ALD) with low roughness. We find that the surface strongly influences the admicelle organization on the surface. At high concentrations (2 × cmc) of cetyltrimethylammonium bromide (CTAB), the surfactant aggregates on a titania surface exhibit a flattened admicelle structure with an average repeat distance of 8.0 ± 1.0 nm whereas aggregates on alumina substrates exhibit a larger admicelle with an average separation distance of 10.5 ± 1.0 nm. A wormlike admicelle structure with an average separation distance of 7.0 ± 1.0 nm can be observed on zirconia substrates whereas a bilayered aggregate structure on hafnia substrates was observed. The change in the surface aggregate structure can be related to an increase in the critical packing parameter through a reduction in the effective headgroup area of the surfactant. The templating strength of the surfaces are found to be hafnia > alumina > zirconia > titania. Weakly templating surfaces are expected to have superior biocompatibility.

  14. Atomic force microscopy compatible device for stretching cells and adsorbed proteins

    NASA Astrophysics Data System (ADS)

    De Jong, K. L.; MacLeod, H. C.; Norton, P. R.; Petersen, N. O.; Jasnin, M. F.

    2006-02-01

    A device that we term a "microrack" was designed to provide a means to stretch cells and proteins and to permit the measurement of any changes in adhesion forces that might occur as a result of the strain, with an atomic force microscope. The device requires an elastic material that allows adsorption of proteins and attachment of cells. The elastomer polydimethylsiloxane (PDMS) was chosen, and its suitability for short-term cell studies was tested by comparing cell morphology and fiber distribution on PDMS with cells grown on glass, a conventional substrate for cell study. Atomic force microscopy (AFM) images and section analysis of beads and scrape marks on the PDMS surface before and after stretching indicate that the microrack can provide up to 21%-29% deformation of PDMS. AFM images of cells grown on PDMS show that material attached to the surface is also affected by stretching of the microrack. The rupture of the cell after stretching and rippling of the cell under compression can be attributed to the fixation treatment, but indicates that the cell morphology is significantly affected by the movement of the substrate on the microrack.

  15. Apparatus for trapping and thermal detection of atomic hydrogen in high magnetic fields at low temperatures

    NASA Technical Reports Server (NTRS)

    Woollam, J. A.

    1980-01-01

    An apparatus is described in which hydrogen atoms were trapped at temperatures down to 1.1 K in the 11 T field of a large volume superconducting magnet. A high sensitivity thermal detector was used to study trapping and recombination of atoms on the detector surface. The apparatus permits the application of extremely high steady state magnetic fields to study the potential effects of electron spin polarization on the stabilization of hydrogen atoms.

  16. Subharmonic excitation in amplitude modulation atomic force microscopy in the presence of adsorbed water layers

    SciTech Connect

    Santos, Sergio; Barcons, Victor; Verdaguer, Albert; Chiesa, Matteo

    2011-12-01

    In ambient conditions, nanometric water layers form on hydrophilic surfaces covering them and significantly changing their properties and characteristics. Here we report the excitation of subharmonics in amplitude modulation atomic force microscopy induced by intermittent water contacts. Our simulations show that there are several regimes of operation depending on whether there is perturbation of water layers. Single period orbitals, where subharmonics are never induced, follow only when the tip is either in permanent contact with the water layers or in pure noncontact where the water layers are never perturbed. When the water layers are perturbed subharmonic excitation increases with decreasing oscillation amplitude. We derive an analytical expression which establishes whether water perturbations compromise harmonic motion and show that the predictions are in agreement with numerical simulations. Empirical validation of our interpretation is provided by the observation of a range of values for apparent height of water layers when subharmonic excitation is predicted.

  17. Hydrogen abstraction from the hydrazine molecule by an oxygen atom.

    PubMed

    Spada, Rene F K; Ferrão, Luiz F A; Rocha, Roberta J; Iha, Koshun; Rocco, José A F F; Roberto-Neto, Orlando; Lischka, Hans; Machado, Francisco B C

    2015-03-01

    Thermochemical and kinetics properties of the hydrogen abstraction from the hydrazine molecule (N2H4) by an oxygen atom were computed using high-level ab initio methods and the M06-2X DFT functional with aug-cc-pVXZ (X = T, Q) and maug-cc-pVTZ basis sets, respectively. The properties along the reaction path were obtained using the dual-level methodology to build the minimum energy path with the potential energy surface obtained with the M06-2X method and thermochemical properties corrected with the CCSD(T)/CBS//M06-2X/maug-cc-pVTZ results. The thermal rate constants were calculated in the framework of variational transition-state theory. Wells on both sides of the reaction (reactants and products) were found and considered in the chemical kinetics calculations. Additionally, the product yields were investigated by means of a study of the triplet and singlet surfaces of the N2H4 + O → N2H2 + H2O reaction.

  18. Charge exchange and ionization in hydrogen atom-fully stripped ion collisions in Debye plasmas

    SciTech Connect

    Zhang, H.; Wang, J. G.; He, B.; Qiu, Y. B.; Janev, R. K.

    2007-05-15

    The processes of charge exchange and ionization in collisions of ground state hydrogen atom with fully stripped ions in a weakly coupled plasma are studied by the classical trajectory Monte Carlo method in the collision energy range 10-900 keV/amu. The interparticle interactions are described by the Debye-Hueckel model with inclusion of dynamical effects associated with the projectile velocity. The microcanonical distribution of initial state electronic coordinates and momenta has been determined by inclusion of plasma screening effects. The cross section dependencies on plasma parameters and ion charge and velocity are investigated. It is shown that plasma effects on charge exchange and ionization cross sections are significant and particularly pronounced at low collision velocities. The results of systematic cross section calculations for different values of Debye screening length (in the range 1-50a{sub 0}) and ion charges (in the range 1-14) are presented.

  19. Application of KrCI excilamp for cleaning GaAs surfaces using atomic hydrogen

    NASA Astrophysics Data System (ADS)

    Tarasenko, Victor F.; Kagadei, Valerii A.; Lomaev, Mikhail I.; Panchenko, Alexei N.; Proskurovsky, Dmitrii I.

    1998-06-01

    Novel single block process facility including UV excilamp and sources of atomic hydrogen is described. Circular sealed-off KrCl* excilamp emitting two intensive bands at 195 and 222 nm was used. The source of atomic hydrogen on the base of reflecting Penning arc discharge was placed in line with the lamp. Semiconducting structures were treated in an expanding effusion jet of atomic hydrogen. The possibility to realize the process of cleaning GaAs surface under joint action of atomic hydrogen and UV radiation has been investigated. Effect of UV radiation on the rate of removing oxide layer is found at low temperature (18 - 100 degree(s)C). The mechanism providing an explanation for this event is suggested. The possibility to realize GaAs surface cleaning using successive performing the procedures of the surface treatment by atomic hydrogen, its oxidation with UV- stimulation and additional treatment by atomic hydrogen was also studied. The sources of atomic hydrogen and UV radiation developed allows to improve cleaning control and provides a way of producing the surface with specified properties.

  20. HAAD: A quick algorithm for accurate prediction of hydrogen atoms in protein structures.

    PubMed

    Li, Yunqi; Roy, Ambrish; Zhang, Yang

    2009-08-20

    Hydrogen constitutes nearly half of all atoms in proteins and their positions are essential for analyzing hydrogen-bonding interactions and refining atomic-level structures. However, most protein structures determined by experiments or computer prediction lack hydrogen coordinates. We present a new algorithm, HAAD, to predict the positions of hydrogen atoms based on the positions of heavy atoms. The algorithm is built on the basic rules of orbital hybridization followed by the optimization of steric repulsion and electrostatic interactions. We tested the algorithm using three independent data sets: ultra-high-resolution X-ray structures, structures determined by neutron diffraction, and NOE proton-proton distances. Compared with the widely used programs CHARMM and REDUCE, HAAD has a significantly higher accuracy, with the average RMSD of the predicted hydrogen atoms to the X-ray and neutron diffraction structures decreased by 26% and 11%, respectively. Furthermore, hydrogen atoms placed by HAAD have more matches with the NOE restraints and fewer clashes with heavy atoms. The average CPU cost by HAAD is 18 and 8 times lower than that of CHARMM and REDUCE, respectively. The significant advantage of HAAD in both the accuracy and the speed of the hydrogen additions should make HAAD a useful tool for the detailed study of protein structure and function. Both an executable and the source code of HAAD are freely available at http://zhang.bioinformatics.ku.edu/HAAD.

  1. Metastable-atom deexcitation spectroscopy of clean and Ag-adsorbed Si (111) surfaces

    NASA Astrophysics Data System (ADS)

    Nishigaki, S.; Takao, K.; Yamada, T.; Arimoto, M.; Komatsu, T.

    1985-07-01

    Electron energy spectra upon incidence of He ∗ metastables on a clean Si(111)7 × 7 surface are obtained, which demonstrate the operation of the surface Penning ionization mechanism for the metastable-atom deexcitation (MD). Dangling bond orbitals are detected at about -0.5 and -1.5 eV below EF in the MD spectra. They are compared with previous UPS results. The adsorption process of Ag on Si(111) is studied by MDS and AES. In a MD spectrum for a Ag-deposited surface at room temperature with θ = {2}/{3} a peak appears at -5.2 below EF which belongs to Ag 4d orbitals. For a surface with the 3× 3 structure (deposited at 300°C with θ = {2}/{3}), however, the intensity of the Ag 4d peak is rather weak and its energy shifts by about -0.4 eV from the room-temperature value. These results support the embedded-Ag model for the Si(111) 3Ag structure.

  2. Modeling of Transmittance Degradation Caused by Optical Surface Contamination by Atomic Oxygen Reaction with Adsorbed Silicones

    NASA Technical Reports Server (NTRS)

    Snyder, Aaron; Banks, Bruce; Miller, Sharon; Stueber, Thomas; Sechkar, Edward

    2001-01-01

    A numerical procedure is presented to calculate transmittance degradation caused by contaminant films on spacecraft surfaces produced through the interaction of orbital atomic oxygen (AO) with volatile silicones and hydrocarbons from spacecraft components. In the model, contaminant accretion is dependent on the adsorption of species, depletion reactions due to gas-surface collisions, desorption, and surface reactions between AO and silicone producing SiO(x), (where x is near 2). A detailed description of the procedure used to calculate the constituents of the contaminant layer is presented, including the equations that govern the evolution of fractional coverage by specie type. As an illustrative example of film growth, calculation results using a prototype code that calculates the evolution of surface coverage by specie type is presented and discussed. An example of the transmittance degradation caused by surface interaction of AO with deposited contaminant is presented for the case of exponentially decaying contaminant flux. These examples are performed using hypothetical values for the process parameters.

  3. Platinum nanoparticle during electrochemical hydrogen evolution: Adsorbate distribution, active reaction species, and size effect

    SciTech Connect

    Tan, Teck L.; Wang, Lin -Lin; Zhang, Jia; Johnson, Duane D.; Bai, Kewu

    2015-03-02

    For small Pt nanoparticles (NPs), catalytic activity is, as observed, adversely affected by size in the 1–3 nm range. We elucidate, via first-principles-based thermodynamics, the operation H* distribution and cyclic voltammetry (CV) during the hydrogen evolution reaction (HER) across the electrochemical potential, including the underpotential region (U ≤ 0) that is difficult to assess in experiment. We consider multiple adsorption sites on a 1 nm Pt NP model and show that the characteristic CV peaks from different H* species correspond well to experiment. We next quantify the activity contribution from each H* species to explain the adverse effect of size. From the resolved CV peaks at the standard hydrogen electrode potential (U = 0), we first deduce that the active species for the HER are the partially covered (100)-facet bridge sites and the (111)-facet hollow sites. Upon evaluation of the reaction barriers at operation H* distribution and microkinetic modeling of the exchange current, we find that the nearest-neighbor (100)-facet bridge site pairs have the lowest activation energy and contribute to ~75% of the NP activity. Edge bridge sites (fully covered by H*) per se are not active; however, they react with neighboring (100)-facet H* to account for ~18% of the activity, whereas (111)-facet hollow sites contribute little. As a result, extrapolating the relative contributions to larger NPs in which the ratio of facet-to-edge sites increases, we show that the adverse size effect of Pt NP HER activity kicks in for sizes below 2 nm.

  4. Platinum nanoparticle during electrochemical hydrogen evolution: Adsorbate distribution, active reaction species, and size effect

    DOE PAGES

    Tan, Teck L.; Wang, Lin -Lin; Zhang, Jia; Johnson, Duane D.; Bai, Kewu

    2015-03-02

    For small Pt nanoparticles (NPs), catalytic activity is, as observed, adversely affected by size in the 1–3 nm range. We elucidate, via first-principles-based thermodynamics, the operation H* distribution and cyclic voltammetry (CV) during the hydrogen evolution reaction (HER) across the electrochemical potential, including the underpotential region (U ≤ 0) that is difficult to assess in experiment. We consider multiple adsorption sites on a 1 nm Pt NP model and show that the characteristic CV peaks from different H* species correspond well to experiment. We next quantify the activity contribution from each H* species to explain the adverse effect of size.more » From the resolved CV peaks at the standard hydrogen electrode potential (U = 0), we first deduce that the active species for the HER are the partially covered (100)-facet bridge sites and the (111)-facet hollow sites. Upon evaluation of the reaction barriers at operation H* distribution and microkinetic modeling of the exchange current, we find that the nearest-neighbor (100)-facet bridge site pairs have the lowest activation energy and contribute to ~75% of the NP activity. Edge bridge sites (fully covered by H*) per se are not active; however, they react with neighboring (100)-facet H* to account for ~18% of the activity, whereas (111)-facet hollow sites contribute little. As a result, extrapolating the relative contributions to larger NPs in which the ratio of facet-to-edge sites increases, we show that the adverse size effect of Pt NP HER activity kicks in for sizes below 2 nm.« less

  5. Ab initio calculations on etching of graphite and diamond surfaces by atomic hydrogen

    SciTech Connect

    Kanai, C.; Watanabe, K.; Takakuwa, Y.

    2001-06-15

    Etching of graphite and hydrogenated diamond C(100) 2{times}1 surfaces by irradiating atomic hydrogen, which is one of the key reactions to promote epitaxial diamond growth by chemical vapor deposition, has been investigated by ab initio pseudopotential calculations. We demonstrate the reaction pathways and determine the activation energies for breaking C-C bonds on the surfaces by irradiating hydrogen atoms. The activation energy for C-C bond breaking on graphite is found to be only one-half of that on the hydrogenated diamond surface. This indicates that graphite, which is a typical nondiamond phase unnecessarily generated on the diamond surface during epitaxial growth, can be selectively eliminated by atomic hydrogen, resulting in methane desorption. Our result supports the growth rate enhancement in diamond epitaxy observed in a recent experiment by gas-source molecular beam epitaxy under hydrogen beam irradiation.

  6. In situ x-ray photoelectron spectroscopic and density-functional studies of Si atoms adsorbed on a C60 film

    NASA Astrophysics Data System (ADS)

    Onoe, Jun; Nakao, Aiko; Hara, Toshiki

    2004-12-01

    The interaction between C60 and Si atoms has been investigated for Si atoms adsorbed on a C60 film using in situ x-ray photoelectron spectroscopy (XPS) and density-functional (DFT) calculations. Analysis of the Si 2p core peak identified three kinds of Si atoms adsorbed on the film: silicon suboxides (SiOx), bulk Si crystal, and silicon atoms bound to C60. Based on the atomic percent ratio of silicon to carbon, we estimated that there was approximately one Si atom bound to each C60 molecule. The Si 2p peak due to the Si-C60 interaction demonstrated that a charge transfer from the Si atom to the C60 molecule takes place at room temperature, which is much lower than the temperature of 670 K at which the charge transfer was observed for C60 adsorbed on Si(001) and (111) clean surfaces [Sakamoto et al., Phys. Rev. B 60, 2579 (1999)]. The number of electrons transferred between the C60 molecule and Si atom was estimated to be 0.59 based on XPS results, which is in good agreement with the DFT result of 0.63 for a C60Si with C2v symmetry used as a model cluster. Furthermore, the shift in binding energy of both the Si 2p and C 1s core peaks before and after Si-atom deposition was experimentally obtained to be +2.0 and -0.4 eV, respectively. The C60Si model cluster provides the shift of +2.13 eV for the Si 2p core peak and of -0.28 eV for the C 1s core peak, which are well corresponding to those experimental results. The covalency of the Si-C60 interaction was also discussed in terms of Mulliken overlap population between them.

  7. In situ x-ray photoelectron spectroscopic and density-functional studies of Si atoms adsorbed on a C60 film.

    PubMed

    Onoe, Jun; Nakao, Aiko; Hara, Toshiki

    2004-12-01

    The interaction between C(60) and Si atoms has been investigated for Si atoms adsorbed on a C(60) film using in situ x-ray photoelectron spectroscopy (XPS) and density-functional (DFT) calculations. Analysis of the Si 2p core peak identified three kinds of Si atoms adsorbed on the film: silicon suboxides (SiO(x)), bulk Si crystal, and silicon atoms bound to C(60). Based on the atomic percent ratio of silicon to carbon, we estimated that there was approximately one Si atom bound to each C(60) molecule. The Si 2p peak due to the Si-C(60) interaction demonstrated that a charge transfer from the Si atom to the C(60) molecule takes place at room temperature, which is much lower than the temperature of 670 K at which the charge transfer was observed for C(60) adsorbed on Si(001) and (111) clean surfaces [Sakamoto et al., Phys. Rev. B 60, 2579 (1999)]. The number of electrons transferred between the C(60) molecule and Si atom was estimated to be 0.59 based on XPS results, which is in good agreement with the DFT result of 0.63 for a C(60)Si with C(2v) symmetry used as a model cluster. Furthermore, the shift in binding energy of both the Si 2p and C 1s core peaks before and after Si-atom deposition was experimentally obtained to be +2.0 and -0.4 eV, respectively. The C(60)Si model cluster provides the shift of +2.13 eV for the Si 2p core peak and of -0.28 eV for the C 1s core peak, which are well corresponding to those experimental results. The covalency of the Si-C(60) interaction was also discussed in terms of Mulliken overlap population between them.

  8. Hydrogen diffusion and stabilization in single-crystal VO2 micro/nanobeams by direct atomic hydrogenation.

    PubMed

    Lin, Jian; Ji, Heng; Swift, Michael W; Hardy, Will J; Peng, Zhiwei; Fan, Xiujun; Nevidomskyy, Andriy H; Tour, James M; Natelson, Douglas

    2014-09-10

    We report measurements of the diffusion of atomic hydrogen in single crystalline VO2 micro/nanobeams by direct exposure to atomic hydrogen, without catalyst. The atomic hydrogen is generated by a hot filament, and the doping process takes place at moderate temperature (373 K). Undoped VO2 has a metal-to-insulator phase transition at ∼340 K between a high-temperature, rutile, metallic phase and a low-temperature, monoclinic, insulating phase with a resistance exhibiting a semiconductor-like temperature dependence. Atomic hydrogenation results in stabilization of the metallic phase of VO2 micro/nanobeams down to 2 K, the lowest point we could reach in our measurement setup. Optical characterization shows that hydrogen atoms prefer to diffuse along the c axis of rutile (a axis of monoclinic) VO2, along the oxygen "channels". Based on observing the movement of the hydrogen diffusion front in single crystalline VO2 beams, we estimate the diffusion constant for hydrogen along the c axis of the rutile phase to be 6.7 × 10(-10) cm(2)/s at approximately 373 K, exceeding the value in isostructural TiO2 by ∼38×. Moreover, we find that the diffusion constant along the c axis of the rutile phase exceeds that along the equivalent a axis of the monoclinic phase by at least 3 orders of magnitude. This remarkable change in kinetics must originate from the distortion of the "channels" when the unit cell doubles along this direction upon cooling into the monoclinic structure. Ab initio calculation results are in good agreement with the experimental trends in the relative kinetics of the two phases. This raises the possibility of a switchable membrane for hydrogen transport.

  9. Scanning tunneling microscopy study: From clean surface to surfaces adsorbed with atom/cluster or metallic island

    NASA Astrophysics Data System (ADS)

    Zhang, Xieqiu

    2007-12-01

    Nanostructures, namely materials in the nanometer or sub-nanometer scales, can possess completely diRTMerent properties from their bulk counterparts. Due to the potential applications in different disciplines, the study of nanostructures has attracted extensive attention worldwide in recent years. Metal nanostructures grown on semiconductor substrates are a special group of nanostructures. Since these nanostructures can be prepared in ultrahigh vacuum with high controllability, one can use low-temperature scanning tunneling microscopy (STM) to obtain information in situ on both the structural and electronic properties of these nanostructures simultaneously. In this thesis, I will present the growth behavior of metal or semiconductor nanostructures at the initial stage and the novel electronic properties of some of these nanostructures. The study of single Ge atoms adsorbed on the Si(111)-7x7 surface shows that different deposition temperatures result in diRTMerent adsorption structures. We find Ge substitution for the Si adatoms during high temperature growth and simple Ge adsorption above the Si atoms during low temperature growth. Small Ag clusters, formed on the Si(111)-7x7 surface at controlled coverages, show a strong rectification effect, which is an indication of the initial stage of Schottky barrier formation and possibly the smallest Schottky diode. On the surfaces of heavily n-doped and p-doped Si substrates, although the 7x7 is metallic at room temperature, an energy gap opens at low temperatures. This energy gap is correlated well with the electronic localization induced by the doping impurities. For Pb nanoislands, a pseudogap was discovered at temperatures higher than the superconducting transition temperature. The strength of the pseudogap depends on the lateral size and temperature, which is speculated to originate from the weak electronic localization induced by structural disorder.

  10. FTIR spectroscopy and thermodynamics of hydrogen adsorbed in a cross-linked polymer.

    PubMed

    Spoto, Giuseppe; Vitillo, Jenny G; Cocina, Donato; Damin, Alessandro; Bonino, Francesca; Zecchina, Adriano

    2007-09-28

    The adsorption of H(2) in a cross-linked poly(styrene-co-divinylbenzene) (St-DVB) microporous polymer (BET surface area 920 m(2) g(-1)) is studied by volumetric and gravimetric methods, FTIR spectroscopy at variable temperature (300-14 K) and ab initio calculations. At 77 K the polymer reversibly stores up to 1.3 mass% H(2) at a pressure of 1 bar and 1.8 mass% at 10 bar. The adsorption process involves the specific interaction of H(2) with the structural phenyl rings through weak dispersive forces. The interacting molecules become IR active and give rise to vibrational and rotational-vibrational manifestations which are affected by the temperature, the contact time and the H(2) equilibrium pressure. The spectra of the H(2)/St-DVB system reported here represent the first IR evidence of the adsorption of hydrogen on unsaturated molecules. The adsorption enthalpy is evaluated by the VTIR (variable temperature IR spectroscopy) method (C. Otero Areán et al., Phys. Chem. Chem. Phys., 2007, DOI: 10.1039/b615535a) and compared with the results of ab initio calculations for the H(2)/benzene interaction and with literature data.

  11. Ab Initio Vibrational Levels For HO2 and Vibrational Splittings for Hydrogen Atom Transfer

    NASA Technical Reports Server (NTRS)

    Barclay, V. J.; Dateo, Christopher E.; Hamilton, I. P.; Arnold, James O. (Technical Monitor)

    1994-01-01

    We calculate vibrational levels and wave functions for HO2 using the recently reported ab initio potential energy surface of Walch and Duchovic. There is intramolecular hydrogen atom transfer when the hydrogen atom tunnels through a T-shaped saddle point separating two equivalent equilibrium geometries, and correspondingly, the energy levels are split. We focus on vibrational levels and wave functions with significant splitting. The first three vibrational levels with splitting greater than 2/cm are (15 0), (0 7 1) and (0 8 0) where V(sub 2) is the O-O-H bend quantum number. We discuss the dynamics of hydrogen atom transfer; in particular, the O-O distances at which hydrogen atom transfer is most probable for these vibrational levels. The material of the proposed presentation was reviewed and the technical content will not reveal any information not already in the public domain and will not give any foreign industry or government a competitive advantage.

  12. Simulation of diffusion of hydrogen atoms in the lattice of tungsten

    NASA Astrophysics Data System (ADS)

    Degtyarenko, N. N.; Pisarev, A. A.

    2016-09-01

    Results of DFT calculations of the activation energy for diffusion and vibrational spectra of interstitial hydrogen atoms in the lattice of tungsten are presented. The temperature dependences of the diffusion coefficient are calculated and compared with experimental data.

  13. Direct observation of hydrogen atom dynamics and interactions by ultrahigh resolution neutron protein crystallography.

    PubMed

    Chen, Julian C-H; Hanson, B Leif; Fisher, S Zoë; Langan, Paul; Kovalevsky, Andrey Y

    2012-09-18

    The 1.1 Å, ultrahigh resolution neutron structure of hydrogen/deuterium (H/D) exchanged crambin is reported. Two hundred ninety-nine out of 315, or 94.9%, of the hydrogen atom positions in the protein have been experimentally derived and resolved through nuclear density maps. A number of unconventional interactions are clearly defined, including a potential O─H…π interaction between a water molecule and the aromatic ring of residue Y44, as well as a number of potential C─H…O hydrogen bonds. Hydrogen bonding networks that are ambiguous in the 0.85 Å ultrahigh resolution X-ray structure can be resolved by accurate orientation of water molecules. Furthermore, the high resolution of the reported structure has allowed for the anisotropic description of 36 deuterium atoms in the protein. The visibility of hydrogen and deuterium atoms in the nuclear density maps is discussed in relation to the resolution of the neutron data.

  14. Quantum beats in hydrogen and antihydrogen atoms in an external electric field.

    PubMed

    Labzowsky, L; Sharipov, V

    2004-04-01

    An effect of quantum beats that arises due to the coherent excitation of 2s and 2p states of hydrogen and antihydrogen atoms in an external electric field is described. It is shown that the quantum beat signal contains terms linear in electric field, i.e., is of opposite sign for the hydrogen and antihydrogen atoms. The conditions for the observation of this effect are discussed.

  15. Erwin Schrödinger, Wave Mechanics, and the Hydrogen Atom

    NASA Astrophysics Data System (ADS)

    de Lange, Owen L.

    1996-06-01

    A brief account is given of some of the main events in Erwin Schrödinger's life, the circumstances leading to his discovery of wave mechanics in 1925-1926, and the application of this mechanics to a model of the hydrogen atom. Two methods of solving this model are outlined, namely, Sommerfeld's polynomial method and Schrödinger's shift operator method. The relation to Pauli's analysis of the quantum-mechanical hydrogen atom is also discussed.

  16. Evidence of wave-particle duality for single fast hydrogen atoms.

    PubMed

    Schmidt, H T; Fischer, D; Berenyi, Z; Cocke, C L; Gudmundsson, M; Haag, N; Johansson, H A B; Källberg, A; Levin, S B; Reinhed, P; Sassenberg, U; Schuch, R; Simonsson, A; Støchkel, K; Cederquist, H

    2008-08-22

    We report the direct observation of interference effects in a Young's double-slit experiment where the interfering waves are two spatially separated components of the de Broglie wave of single 1.3 MeV hydrogen atoms formed close to either target nucleus in H++H2 electron-transfer collisions. Quantum interference strongly influences the results even though the hydrogen atoms have a de Broglie wavelength, lambda_{dB}, as small as 25 fm.

  17. Enhancement of electrical conductivity and electrochemical activity of hydrogenated amorphous carbon by incorporating boron atoms

    NASA Astrophysics Data System (ADS)

    Naragino, Hiroshi; Yoshinaga, Kohsuke; Nakahara, Akira; Tanaka, Sakuya; Honda, Kensuke

    2013-06-01

    Conductive boron-doped hydrogenated amorphous carbon (B-DLC) thin films were successfully synthesized with RF plasma-enhanced CVD method. By incorporating boron atoms in amorphous carbon, conduction types were changed from n- to p-type, and volume resistivity was decreased from 30.4 (non-doped) to 6.36 × 10-2 Ω cm (B/C = 2.500 atom%). B-DLC film with sp2/(sp2 + sp3) carbons of 75 atom% exhibited high resistance to electrochemically-induced corrosion in strong acid solution. Furthermore, it was clarified that boron atoms in DLC could enhance kinetics of hydrogen evolution during water electrolysis at B-DLC surface. B-DLC is, therefore, a promising electrode material for hydrogen production by increasing the concentration of boron atoms in B-DLC and enhancing the reactivity of H2 evolution.

  18. Atomic-Scale Mechanism for Hydrogenation of o-Cresol on Pt Catalysis

    NASA Astrophysics Data System (ADS)

    Li, Yaping; Liu, Zhimin; Xue, Wenhua; Crossley, Steven; Jentoft, Friederike; Wang, Sanwu

    Biofuels derived from lignocellulosic biomass have received significant attention lately due to increasing environmental concerns. With first-principles density-functional theory and ab initio molecular dynamic simulations, we investigated the atomic-scale mechanism of o-cresol hydrogenation on the Pt(111) surface. The formation of 2-methyl-cyclohexanone (the intermediate product) was found to involve two steps. The first step is the dehydrogenation, that is, the H atom in the hydroxyl group moves to the Pt surface. The second step is the hydrogenation, that is, the H atoms on Pt react with the carbon atoms in the aromatic ring. The first step involves a smaller barrier, suggesting that dehydrogenation occurs first, followed by hydrogenation of the ring. In particular, tautomerization is found to occur via a two-step process over the catalyst. On the other hand, 2-methyl-cyclohexanol (the final product) is produced through two paths. One is direct hydrogenation of the aromatic ring. Another pathway includes partial hydrogenation of the ring, dehydrogenation of -OH group, finally hydrogenation of remaining C atoms and the O atom. Our theoretical results agree well with the experimental observations. Supported by DOE (DE-SC0004600). This research used the supercomputer resources of NERSC, XSEDE, TACC.

  19. Fluorescence (TALIF) measurement of atomic hydrogen concentration in a coplanar surface dielectric barrier discharge

    NASA Astrophysics Data System (ADS)

    Mrkvičková, M.; Ráheľ, J.; Dvořák, P.; Trunec, D.; Morávek, T.

    2016-10-01

    Spatially and temporally resolved measurements of atomic hydrogen concentration above the dielectric of coplanar barrier discharge are presented for atmospheric pressure in 2.2% H2/Ar. The measurements were carried out in the afterglow phase by means of two-photon absorption laser-induced fluorescence (TALIF). The difficulties of employing the TALIF technique in close proximity to the dielectric surface wall were successfully addressed by taking measurements on a suitable convexly curved dielectric barrier, and by proper mathematical treatment of parasitic signals from laser-surface interactions. It was found that the maximum atomic hydrogen concentration is situated closest to the dielectric wall from which it gradually decays. The maximum absolute concentration was more than 1022 m-3. In the afterglow phase, the concentration of atomic hydrogen above the dielectric surface stays constant for a considerable time (10 μs-1 ms), with longer times for areas situated farther from the dielectric surface. The existence of such a temporal plateau was explained by the presented 1D model: the recombination losses of atomic hydrogen farther from the dielectric surface are compensated by the diffusion of atomic hydrogen from regions close to the dielectric surface. The fact that a temporal plateau exists even closest to the dielectric surface suggests that the dielectric surface acts as a source of atomic hydrogen in the afterglow phase.

  20. The simplicity of perfect atoms: Degeneracies in supersymmetric hydrogen

    DOE PAGES

    Rube, Tomas; Wacker, Jay G.

    2011-06-07

    In this study, supersymmetric QED hydrogen-like bound states are remarkably similar to nonsupersymmetric hydrogen, including an accidental degeneracy of the fine structure and is broken by the Lamb shift. This article classifies the states, calculates the leading order spectrum, and illustrates the results in several limits. The relation to other nonrelativistic bound states is explored.

  1. The simplicity of perfect atoms: Degeneracies in supersymmetric hydrogen

    SciTech Connect

    Rube, Tomas; Wacker, Jay G.

    2011-06-15

    Supersymmetric QED hydrogen-like bound states are remarkably similar to nonsupersymmetric hydrogen, including an accidental degeneracy of the fine structure and is broken by the Lamb shift. This article classifies the states, calculates the leading order spectrum, and illustrates the results in several limits. The relation to other nonrelativistic bound states is explored.

  2. ATOMIC AND MOLECULAR PHYSICS: Multiphoton ionization of the hydrogen atom exposed to circularly or linearly polarized laser pulses

    NASA Astrophysics Data System (ADS)

    Wang, Pei-Jie; He, Feng

    2009-12-01

    This paper studies the multiphoton ionization of the hydrogen atom exposed to the linearly or circularly polarized laser pulses by solving the time-dependent Schrödinger equation. It finds that the ratio of the ionization probabilities by linearly and circularly polarized laser pulses varies with the numbers of absorbing photons. With the same laser intensity, the circularly polarized laser pulse favors to ionize the atom with more ease than the linearly polarized laser pulse if only two or three photons are necessary to be absorbed. For the higher order multiphoton ionization, the linearly polarized laser pulse has the advantage over circularly polarized laser pulse to ionize the atom.

  3. Hydrogen atoms can be located accurately and precisely by x-ray crystallography

    PubMed Central

    Woińska, Magdalena; Grabowsky, Simon; Dominiak, Paulina M.; Woźniak, Krzysztof; Jayatilaka, Dylan

    2016-01-01

    Precise and accurate structural information on hydrogen atoms is crucial to the study of energies of interactions important for crystal engineering, materials science, medicine, and pharmacy, and to the estimation of physical and chemical properties in solids. However, hydrogen atoms only scatter x-radiation weakly, so x-rays have not been used routinely to locate them accurately. Textbooks and teaching classes still emphasize that hydrogen atoms cannot be located with x-rays close to heavy elements; instead, neutron diffraction is needed. We show that, contrary to widespread expectation, hydrogen atoms can be located very accurately using x-ray diffraction, yielding bond lengths involving hydrogen atoms (A–H) that are in agreement with results from neutron diffraction mostly within a single standard deviation. The precision of the determination is also comparable between x-ray and neutron diffraction results. This has been achieved at resolutions as low as 0.8 Å using Hirshfeld atom refinement (HAR). We have applied HAR to 81 crystal structures of organic molecules and compared the A–H bond lengths with those from neutron measurements for A–H bonds sorted into bonds of the same class. We further show in a selection of inorganic compounds that hydrogen atoms can be located in bridging positions and close to heavy transition metals accurately and precisely. We anticipate that, in the future, conventional x-radiation sources at in-house diffractometers can be used routinely for locating hydrogen atoms in small molecules accurately instead of large-scale facilities such as spallation sources or nuclear reactors. PMID:27386545

  4. Hydrogen atoms can be located accurately and precisely by x-ray crystallography.

    PubMed

    Woińska, Magdalena; Grabowsky, Simon; Dominiak, Paulina M; Woźniak, Krzysztof; Jayatilaka, Dylan

    2016-05-01

    Precise and accurate structural information on hydrogen atoms is crucial to the study of energies of interactions important for crystal engineering, materials science, medicine, and pharmacy, and to the estimation of physical and chemical properties in solids. However, hydrogen atoms only scatter x-radiation weakly, so x-rays have not been used routinely to locate them accurately. Textbooks and teaching classes still emphasize that hydrogen atoms cannot be located with x-rays close to heavy elements; instead, neutron diffraction is needed. We show that, contrary to widespread expectation, hydrogen atoms can be located very accurately using x-ray diffraction, yielding bond lengths involving hydrogen atoms (A-H) that are in agreement with results from neutron diffraction mostly within a single standard deviation. The precision of the determination is also comparable between x-ray and neutron diffraction results. This has been achieved at resolutions as low as 0.8 Å using Hirshfeld atom refinement (HAR). We have applied HAR to 81 crystal structures of organic molecules and compared the A-H bond lengths with those from neutron measurements for A-H bonds sorted into bonds of the same class. We further show in a selection of inorganic compounds that hydrogen atoms can be located in bridging positions and close to heavy transition metals accurately and precisely. We anticipate that, in the future, conventional x-radiation sources at in-house diffractometers can be used routinely for locating hydrogen atoms in small molecules accurately instead of large-scale facilities such as spallation sources or nuclear reactors. PMID:27386545

  5. Hydrogen atoms can be located accurately and precisely by x-ray crystallography.

    PubMed

    Woińska, Magdalena; Grabowsky, Simon; Dominiak, Paulina M; Woźniak, Krzysztof; Jayatilaka, Dylan

    2016-05-01

    Precise and accurate structural information on hydrogen atoms is crucial to the study of energies of interactions important for crystal engineering, materials science, medicine, and pharmacy, and to the estimation of physical and chemical properties in solids. However, hydrogen atoms only scatter x-radiation weakly, so x-rays have not been used routinely to locate them accurately. Textbooks and teaching classes still emphasize that hydrogen atoms cannot be located with x-rays close to heavy elements; instead, neutron diffraction is needed. We show that, contrary to widespread expectation, hydrogen atoms can be located very accurately using x-ray diffraction, yielding bond lengths involving hydrogen atoms (A-H) that are in agreement with results from neutron diffraction mostly within a single standard deviation. The precision of the determination is also comparable between x-ray and neutron diffraction results. This has been achieved at resolutions as low as 0.8 Å using Hirshfeld atom refinement (HAR). We have applied HAR to 81 crystal structures of organic molecules and compared the A-H bond lengths with those from neutron measurements for A-H bonds sorted into bonds of the same class. We further show in a selection of inorganic compounds that hydrogen atoms can be located in bridging positions and close to heavy transition metals accurately and precisely. We anticipate that, in the future, conventional x-radiation sources at in-house diffractometers can be used routinely for locating hydrogen atoms in small molecules accurately instead of large-scale facilities such as spallation sources or nuclear reactors.

  6. A spectroscopic study of hydrogen atom and molecule collision. Final report

    SciTech Connect

    Kielkopf, John F.

    2002-07-01

    The fundamental processes which occur in low-energy collisions of excited states of the hydrogen atom with other neutral atoms, protons, and electrons in dense plasmas were investigated in this project. Theoretical and experimental results for the Lyman and Balmer series are described here, including references to recent publications resulting from this project.

  7. Path integral Monte Carlo simulations of H2 adsorbed to lithium-doped benzene: A model for hydrogen storage materials

    NASA Astrophysics Data System (ADS)

    Lindoy, Lachlan P.; Kolmann, Stephen J.; D'Arcy, Jordan H.; Crittenden, Deborah L.; Jordan, Meredith J. T.

    2015-11-01

    Finite temperature quantum and anharmonic effects are studied in H2-Li+-benzene, a model hydrogen storage material, using path integral Monte Carlo (PIMC) simulations on an interpolated potential energy surface refined over the eight intermolecular degrees of freedom based upon M05-2X/6-311+G(2df,p) density functional theory calculations. Rigid-body PIMC simulations are performed at temperatures ranging from 77 K to 150 K, producing both quantum and classical probability density histograms describing the adsorbed H2. Quantum effects broaden the histograms with respect to their classical analogues and increase the expectation values of the radial and angular polar coordinates describing the location of the center-of-mass of the H2 molecule. The rigid-body PIMC simulations also provide estimates of the change in internal energy, ΔUads, and enthalpy, ΔHads, for H2 adsorption onto Li+-benzene, as a function of temperature. These estimates indicate that quantum effects are important even at room temperature and classical results should be interpreted with caution. Our results also show that anharmonicity is more important in the calculation of U and H than coupling—coupling between the intermolecular degrees of freedom becomes less important as temperature increases whereas anharmonicity becomes more important. The most anharmonic motions in H2-Li+-benzene are the "helicopter" and "ferris wheel" H2 rotations. Treating these motions as one-dimensional free and hindered rotors, respectively, provides simple corrections to standard harmonic oscillator, rigid rotor thermochemical expressions for internal energy and enthalpy that encapsulate the majority of the anharmonicity. At 150 K, our best rigid-body PIMC estimates for ΔUads and ΔHads are -13.3 ± 0.1 and -14.5 ± 0.1 kJ mol-1, respectively.

  8. Path integral Monte Carlo simulations of H2 adsorbed to lithium-doped benzene: A model for hydrogen storage materials.

    PubMed

    Lindoy, Lachlan P; Kolmann, Stephen J; D'Arcy, Jordan H; Crittenden, Deborah L; Jordan, Meredith J T

    2015-11-21

    Finite temperature quantum and anharmonic effects are studied in H2-Li(+)-benzene, a model hydrogen storage material, using path integral Monte Carlo (PIMC) simulations on an interpolated potential energy surface refined over the eight intermolecular degrees of freedom based upon M05-2X/6-311+G(2df,p) density functional theory calculations. Rigid-body PIMC simulations are performed at temperatures ranging from 77 K to 150 K, producing both quantum and classical probability density histograms describing the adsorbed H2. Quantum effects broaden the histograms with respect to their classical analogues and increase the expectation values of the radial and angular polar coordinates describing the location of the center-of-mass of the H2 molecule. The rigid-body PIMC simulations also provide estimates of the change in internal energy, ΔUads, and enthalpy, ΔHads, for H2 adsorption onto Li(+)-benzene, as a function of temperature. These estimates indicate that quantum effects are important even at room temperature and classical results should be interpreted with caution. Our results also show that anharmonicity is more important in the calculation of U and H than coupling-coupling between the intermolecular degrees of freedom becomes less important as temperature increases whereas anharmonicity becomes more important. The most anharmonic motions in H2-Li(+)-benzene are the "helicopter" and "ferris wheel" H2 rotations. Treating these motions as one-dimensional free and hindered rotors, respectively, provides simple corrections to standard harmonic oscillator, rigid rotor thermochemical expressions for internal energy and enthalpy that encapsulate the majority of the anharmonicity. At 150 K, our best rigid-body PIMC estimates for ΔUads and ΔHads are -13.3 ± 0.1 and -14.5 ± 0.1 kJ mol(-1), respectively.

  9. Path integral Monte Carlo simulations of H2 adsorbed to lithium-doped benzene: A model for hydrogen storage materials.

    PubMed

    Lindoy, Lachlan P; Kolmann, Stephen J; D'Arcy, Jordan H; Crittenden, Deborah L; Jordan, Meredith J T

    2015-11-21

    Finite temperature quantum and anharmonic effects are studied in H2-Li(+)-benzene, a model hydrogen storage material, using path integral Monte Carlo (PIMC) simulations on an interpolated potential energy surface refined over the eight intermolecular degrees of freedom based upon M05-2X/6-311+G(2df,p) density functional theory calculations. Rigid-body PIMC simulations are performed at temperatures ranging from 77 K to 150 K, producing both quantum and classical probability density histograms describing the adsorbed H2. Quantum effects broaden the histograms with respect to their classical analogues and increase the expectation values of the radial and angular polar coordinates describing the location of the center-of-mass of the H2 molecule. The rigid-body PIMC simulations also provide estimates of the change in internal energy, ΔUads, and enthalpy, ΔHads, for H2 adsorption onto Li(+)-benzene, as a function of temperature. These estimates indicate that quantum effects are important even at room temperature and classical results should be interpreted with caution. Our results also show that anharmonicity is more important in the calculation of U and H than coupling-coupling between the intermolecular degrees of freedom becomes less important as temperature increases whereas anharmonicity becomes more important. The most anharmonic motions in H2-Li(+)-benzene are the "helicopter" and "ferris wheel" H2 rotations. Treating these motions as one-dimensional free and hindered rotors, respectively, provides simple corrections to standard harmonic oscillator, rigid rotor thermochemical expressions for internal energy and enthalpy that encapsulate the majority of the anharmonicity. At 150 K, our best rigid-body PIMC estimates for ΔUads and ΔHads are -13.3 ± 0.1 and -14.5 ± 0.1 kJ mol(-1), respectively. PMID:26590532

  10. In situ study of erosion and deposition of amorphous hydrogenated carbon films by exposure to a hydrogen atom beam

    SciTech Connect

    Markelj, Sabina; Pelicon, Primoz; Cadez, Iztok; Schwarz-Selinger, Thomas; Jacob, Wolfgang

    2012-07-15

    This paper reports on the first dual-beam experiment employing a hydrogen atom beam for sample exposure and an ion beam for analysis, enabling in situ and real-time studies of hydrogen atom interaction with materials. The erosion of an amorphous hydrogenated carbon (a-C:H) layer by deuterium atoms at 580 K sample temperature was studied and the uptake of deuterium during the erosion process was measured in real time. The deuterium areal density increased at the beginning to 7.3 Multiplication-Sign 10{sup 15} D cm{sup -2}, but then stabilized at a constant value of 5.5 Multiplication-Sign 10{sup 15} D cm{sup -2}. Formation of a polymer-like deposit on an a-C:H layer held at room temperature and subjected to the deuterium atom beam was observed and also studied in situ. For both erosion and deposition studies an a-{sup 13}C:H layer on top of an Si substrate was used as a sample, making the experiments isotopically fully specified and thereby differentiating the deposited from the original layer and the interacting D atoms from H atoms present in the layer and in the residual vacuum. From the deposition study it was shown that carbon in the deposited layer originates from carbon-carrying species in the background vacuum that interact with hydrogen atoms. The areal density of the carbon at the surface was determined from the energy shift of the Si edge in the Rutherford backscattering spectrum. The cross section for {sup 7}Li on D at 4.3 MeV Li ion energy and at a recoil angle of 30 Degree-Sign was also determined to be (236 {+-} 16) Multiplication-Sign 10{sup -27} cm{sup 2}/sr. This is a factor of 3 {+-} 0.2 times higher than the Rutherford elastic cross section.

  11. Trapping of hydrogen atoms inside small beryllium clusters and their ions

    NASA Astrophysics Data System (ADS)

    Naumkin, F. Y.; Wales, D. J.

    2016-08-01

    Structure, stability and electronic properties are evaluated computationally for small Ben (n = 5-9) cluster cages accommodating atomic H inside and forming core-shell species. These parameters are predicted to vary significantly upon insertion of H, for ionic derivatives, and with the system size. In particular, the energy barrier for H-atom exit from the cage changes significantly for ions compared to the neutral counterparts. The corresponding effects predicted for cage assemblies suggest the possibility of efficient charge-control of hydrogen release. This, together with a high capacity for storing hydrogen in extended such assemblies might indicate a possible way towards feasible hydrogen-storage solutions.

  12. Hydrogen atom scrambling in ion-molecule reactions of methane and ethylene.

    NASA Technical Reports Server (NTRS)

    Huntress, W. T., Jr.

    1972-01-01

    The extent of hydrogen atom exchange in the reaction, CH3(+) + CH4 yields C2H5(+) + H2, is determined by examining the product distribution for the reactions CH3(+) + CD4 and CD3(+) + CH4 as a function of relative kinetic energy from thermal energies to 10 eV. It is found that the reaction of CH4(+) with the parent neutral proceeds both via proton transfer and hydrogen abstraction accompanied by approximately 10% hydrogen atom exchange during the reaction.

  13. Identification of titanium-hydrogen complexes with up to four hydrogen atoms in silicon

    SciTech Connect

    Scheffler, L.; Kolkovsky, Vl. Weber, J.

    2015-02-28

    Using high-resolution Laplace deep level transient spectroscopy studies, several TiH-related complexes (E40′, E170, E170′, and E260) were observed in wet-chemically etched and H-plasma treated n-type Si. We assign E40′ and E170 to two different configurations of Ti with one H atom. Both of them are shown to behave as single donor states with an activation enthalpy of E{sub C} − 0.07 eV (E40′) and E{sub C} − 0.34 eV (E170) in the upper half of Si. E170′ with an activation energy of E{sub C} − 0.37 eV is correlated with the donor state of the Ti{sub i}H{sub 2} defect, whereas E260 is attributed to the donor state of Ti{sub i}H{sub 3}. Besides the TiH defects, the presence of electrically inactive TiH{sub 4} is reported. No titanium-hydrogen-related levels were observed in p-type Si.

  14. Optical radiation and ionization of hydrogen atoms in heterogeneous exothermal reactions proceeding in an electric field

    NASA Astrophysics Data System (ADS)

    Blashenkov, N. M.; Lavrent'ev, G. Ya.

    2009-09-01

    Optical radiation related to the Balmer series (Hα, Hβ, Hγ) of hydrogen atoms is discovered when studying the isothermal reaction of trimeric acetone peroxide decomposition on the surface of oxidized tungsten in a static electric field with a strength of up to 4 × 106 V/cm at T = 300 K. The distance from the surface over which desorbing excited hydrogen atoms radiate is determined from the Stark splitting of the lines. Electronically excited atoms remaining on the surface ionize according to the surface ionization mechanism.

  15. 2s Hyperfine splitting in light hydrogen-like atoms: Theory and experiment

    SciTech Connect

    Karshenboim, S. G. Kolachevsky, N. N.; Ivanov, V. G.; Fischer, M.; Fendel, P.; Haensch, T. W.

    2006-03-15

    Since the combination D{sub 21} = 8f{sub HFS}(2s)-f{sub HFS}(1s) of hyperfine intervals in hydrogen and light two-body hydrogen-like atomic systems weakly depends on the nuclear structure, comparison between theory and experiment can be sensitive to high order QED corrections. New theoretical and experimental results are presented. Calculations have been performed for the hydrogen and deuterium atoms and for the helium-3 ion. Experiments on the 2s hyperfine splitting (responsible for the dominant contribution to the error in D{sub 21}) have been conducted for hydrogen and deuterium. The theory and experiment are in good agreement, and their accuracy is comparable to that attained in verifying the QED theory of the hyperfine splitting in leptonic atoms (muonium and positronium)

  16. Hydrogen trapped in Ben cluster cages: The atomic encapsulation option

    NASA Astrophysics Data System (ADS)

    Naumkin, Fedor Y.; Wales, David J.

    2012-08-01

    Core-shell (kH)@Ben (k = 1-3, n = 6-11) systems are studied computationally. The smallest system with endohedral hydrogen is H@Be6 with a central H anion, thermodynamically stable to dissociation into H + Be6. Larger structures are constructed by merging a few such units and have reduced stability. Potential energy barriers to hydrogen exit from the cage assemblies are estimated. Face- and edge-sharing combinations of the structural units are considered. The extrapolated upper bound for the potential 'nanofoam' material storage capacity is 10 weight-% of hydrogen. The changes in shape and electronic properties of the Ben cages upon insertion of hydrogen are also analyzed.

  17. An improved atomic hydrogen frequency and time standard

    NASA Technical Reports Server (NTRS)

    Mc Gunigal, T. E.; Peters, H. E.

    1969-01-01

    Use of a large bulb, long-multipole magnet, automatic tuner and aluminum cavity provides an improved hydrogen maser which is accurate over long periods of time and suitable for tracking station environments.

  18. Characterization of hot hydrogen-atom reactions by kinetic spectrography.

    NASA Technical Reports Server (NTRS)

    Tomalesky, R. E.; Sturm, J. E.

    1971-01-01

    The flash photolysis of hydrogen iodide in the presence of nitrous oxide, carbon dioxide, and water has been investigated by kinetic spectroscopy. Although the fraction of hydrogen iodide dissociated was very large, the only observable intermediate was imidogen. It was demonstrated that the rapid removal of imidogen and the apparent absence of hydroxyl radicals in each case is a result of the following two reactions, respectively: (1) NH + HI yields NH2 + I; and (2) OH + HI yields H2O + I.

  19. Atomically isolated nickel species anchored on graphitized carbon for efficient hydrogen evolution electrocatalysis.

    PubMed

    Fan, Lili; Liu, Peng Fei; Yan, Xuecheng; Gu, Lin; Yang, Zhen Zhong; Yang, Hua Gui; Qiu, Shilun; Yao, Xiangdong

    2016-01-01

    Hydrogen production through electrochemical process is at the heart of key renewable energy technologies including water splitting and hydrogen fuel cells. Despite tremendous efforts, exploring cheap, efficient and durable electrocatalysts for hydrogen evolution still remains as a great challenge. Here we synthesize a nickel-carbon-based catalyst, from carbonization of metal-organic frameworks, to replace currently best-known platinum-based materials for electrocatalytic hydrogen evolution. This nickel-carbon-based catalyst can be activated to obtain isolated nickel atoms on the graphitic carbon support when applying electrochemical potential, exhibiting highly efficient hydrogen evolution performance with high exchange current density of 1.2 mA cm(-2) and impressive durability. This work may enable new opportunities for designing and tuning properties of electrocatalysts at atomic scale for large-scale water electrolysis. PMID:26861684

  20. Atomically isolated nickel species anchored on graphitized carbon for efficient hydrogen evolution electrocatalysis

    PubMed Central

    Fan, Lili; Liu, Peng Fei; Yan, Xuecheng; Gu, Lin; Yang, Zhen Zhong; Yang, Hua Gui; Qiu, Shilun; Yao, Xiangdong

    2016-01-01

    Hydrogen production through electrochemical process is at the heart of key renewable energy technologies including water splitting and hydrogen fuel cells. Despite tremendous efforts, exploring cheap, efficient and durable electrocatalysts for hydrogen evolution still remains as a great challenge. Here we synthesize a nickel–carbon-based catalyst, from carbonization of metal-organic frameworks, to replace currently best-known platinum-based materials for electrocatalytic hydrogen evolution. This nickel-carbon-based catalyst can be activated to obtain isolated nickel atoms on the graphitic carbon support when applying electrochemical potential, exhibiting highly efficient hydrogen evolution performance with high exchange current density of 1.2 mA cm−2 and impressive durability. This work may enable new opportunities for designing and tuning properties of electrocatalysts at atomic scale for large-scale water electrolysis. PMID:26861684

  1. The elastic, electronic and magnetism structure of the MAl and M3Al (M=Fe and Ni) alloy with and without hydrogen atoms

    NASA Astrophysics Data System (ADS)

    Mubarak, A. A.

    2016-03-01

    The energetic stability, electronic and magnetism of the MAl, M3Al alloy (M=Fe, Ni) and variant surfaces of MAl (001) with and without hydrogen atoms are investigated by utilizing DFT and GGA as the exchange-correlation potential. All presented alloys with and without the H atom absorption is found elastically and thermodynamically stable. The calculated absorption energy shows that H is more energetically stable in the bridge and octahedral site in MAl and M3Al alloys, respectively. Hydrogen atoms absorption is expanded and brittle the studied host alloys. The ability of absorption of H atom at more than one site in the MAl alloy is found energetically and thermodynamically stable. The H adsorption on the variant surfaces of MAl (001) is predicted too. Fourfold and top sites are found more energetically stable to adsorbed the H atom on the above surface layer of H/MAl-M and H/MAl-Al, respectively. The obvious changes are observed in the interlayer spacing for studied surfaces which yields to decrease the LDOS and magnetic moments of the surface and subsurface layers.

  2. Interaction of alkali atoms with water multilayers adsorbed on TiO 2(1 1 0): a study with MIES and UPS

    NASA Astrophysics Data System (ADS)

    Krischok, S.; Höfft, O.; Kempter, V.

    2003-06-01

    The chemistry of alkali atoms (Li, Na, K, Cs) embedded in a multilayer aqueous environment was studied with metastable impact electron spectroscopy (MIES) and ultraviolet photoemission spectroscopy (UPS) (HeI and II) under ultra high vacuum (UHV) conditions. The water multilayers were grown at 130 K on a rutile, 1×1 reconstructed, TiO 2(1 1 0) single crystal. The behavior of the multilayer system was investigated as a function of the temperature (130-500 K). Due to the relatively large escape depth of the emitted electrons UPS provides spectroscopic information about several layers in contrast to MIES which is only sensitive to the outermost layer. This allows us to discriminate between species adsorbed at the water multilayer and species, which are embedded in the solvent or at the substrate-solvent interface. Furthermore, MIES is, in contrast to UPS, very sensitive to the outermost s-states of adsorbed alkali atoms, which are considered to be responsible for the high reactivity of these metals. The present study gives insight into the complicated chemistry of alkali atoms added to an aqueous multilayer system. The chosen combination of MIES and UPS allows us to distinguish clearly between various phases depending on the amount of offered alkali atoms. For low alkali concentrations the alkali atoms penetrate the water surface whereby they dissociate some water. With increasing exposure more and more water molecules become dissociated, whereby the outermost water layer remains intact. Finally, the chemistry between water and alkali atoms takes place at the outermost surface too, which is manifested by the formation of OH-groups at the surface. With further increasing alkali concentration the atoms start to adsorb as neutral atoms; whereby the spectrum of the alkali species is then strongly influenced by the underlying solvent system. For very high exposure the observed spectra are not influenced by the underlying aqueous system anymore; the formation of an alkali

  3. Symmetry in chemistry from the hydrogen atom to proteins

    PubMed Central

    Kellman, Michael E.

    1996-01-01

    The last 2 decades have seen discoveries in highly excited states of atoms and molecules of phenomena that are qualitatively different from the “planetary” model of the atom, and the near-rigid model of molecules, characteristic of these systems in their low-energy states. A unified view is emerging in terms of approximate dynamical symmetry principles. Highly excited states of two-electron atoms display “molecular” behavior of a nonrigid linear structure undergoing collective rotation and vibration. Highly excited states of molecules described in the “standard molecular model” display normal mode couplings, which induce bifurcations on the route to molecular chaos. New approaches such as rigid–nonrigid correlation, vibrons, and quantum groups suggest a unified view of collective electronic motion in atoms and nuclear motion in molecules. PMID:8962040

  4. Positron scattering from hydrogen atom with screened Coulomb potentials

    SciTech Connect

    Ghoshal, Arijit; Nayek, Sujay; Kamali, M. Z. M.; Ratnavelu, K.

    2014-03-05

    Elastic positron-hydrogen collisions with screened Coulomb potentials have been investigated using a second-order distorted wave Born approximation in the momentum space. Two types of potentials have been considered, namely, static screened Coulomb potential and exponential cosine-screened Coulomb potential. Using a simple variationally determined hydrogenic wave function it has been possible to obtain the scattering amplitude in a closed form. A detailed study has been made on the differential and total cross sections in the energy range 20–300 eV.

  5. Hydrogen bond cooperativity in water hexamers: atomic energy perspective of local stabilities.

    PubMed

    Albrecht, Laura; Chowdhury, Saptarshi; Boyd, Russell J

    2013-10-17

    Atomic energies are used to describe local stability in eight low-lying water hexamers: prism, cage, boat 1, boat 2, bag, chair, book 1, and book 2. The energies are evaluated using the quantum theory of atoms in molecules (QTAIM) at MP2/aug-cc-pVTZ geometries. It is found that the simple, stabilizing cooperativity observed in linear hydrogen-bonded water systems is diminished as clusters move from nearly planar to three-dimensional structures. The prism, cage, and bag clusters can have local water stabilities differing up to 5 kcal mol(-1) as a result of mixed cooperative and anticooperative interactions. At the atomic level, in many cases a water may have a largely stabilized oxygen atom but the net water stability will be diminished due to strong destabilization of the water's hydrogen atoms. Analysis of bond critical point (BCP) electron densities shows that the reduced cooperativity results in a decrease in hydrogen bond strength and an increase in covalent bond strength, most evident in the prism. The chair, with the greatest cooperativity, has the largest average electron density at the BCP per hydrogen bond, whereas the cage has the largest total value for BCP density at all hydrogen bonds. The cage also has the second largest value (after the prism) for covalent bond critical point densities and an oxygen-oxygen BCP which may factor into the experimentally observed stability of the structure.

  6. Hydrogen-induced atomic rearrangement in MgPd{sub 3}

    SciTech Connect

    Kohlmann, H. . E-mail: h.kohlmann@mx.uni-saarland.de; Renaudin, G.; Yvon, K.; Wannek, C.; Harbrecht, B.

    2005-04-15

    The hydrogenation behavior of MgPd{sub 3} has been studied by in situ X-ray powder diffraction and by neutron powder diffraction. At room temperature and p {approx}500kPa hydrogen pressure its structure is capable of incorporating up to one hydrogen atom per formula unit ({alpha}-MgPd{sub 3}H{sub {approx}}{sub 1}), thereby retaining a tetragonal ZrAl{sub 3}-type metal atom arrangement. Upon heating to 750K in a hydrogen atmosphere of 610kPa it transforms into a cubic modification with AuCu{sub 3}-type metal atom arrangement ({beta}-MgPd{sub 3}H{sub {approx}}{sub 0.7}). Neutron diffraction on the deuteride reveals an anion deficient anti-perovskite-type structure ({beta}-MgPd{sub 3}D{sub 0.67}, a=398.200(7)pm) in which octahedral sites surrounded exclusively by palladium atoms are occupied by deuterium. Complete removal of hydrogen (480K, 1Pa) stabilizes a new binary modification ({beta}-MgPd{sub 3}, a=391.78(2)pm) crystallizing with a primitive cubic AuCu{sub 3}-type structure. Mechanical treatment (grinding) transforms both {alpha} and {beta} modifications of MgPd{sub 3} into a cubic face-centered solid solution Mg{sub 0.25}Pd{sub 0.75} showing a random distribution of magnesium and palladium atoms.

  7. Hydrogen Atom Reactivity toward Aqueous tert-Butyl Alcohol

    SciTech Connect

    Lymar S. V.; Schwarz, H.A.

    2012-02-09

    Through a combination of pulse radiolysis, purification, and analysis techniques, the rate constant for the H + (CH{sub 3}){sub 3}COH {yields} H{sub 2} + {sm_bullet}CH{sub 2}C(CH{sub 3}){sub 2}OH reaction in aqueous solution is definitively determined to be (1.0 {+-} 0.15) x 10{sup 5} M{sup -1} s{sup -1}, which is about half of the tabulated number and 10 times lower than the more recently suggested revision. Our value fits on the Polanyi-type, rate-enthalpy linear correlation ln(k/n) = (0.80 {+-} 0.05){Delta}H + (3.2 {+-} 0.8) that is found for the analogous reactions of other aqueous aliphatic alcohols with n equivalent abstractable H atoms. The existence of such a correlation and its large slope are interpreted as an indication of the mechanistic similarity of the H atom abstraction from {alpha}- and {beta}-carbon atoms in alcohols occurring through the late, product-like transition state. tert-Butyl alcohol is commonly contaminated by much more reactive secondary and primary alcohols (2-propanol, 2-butanol, ethanol, and methanol), whose content can be sufficient for nearly quantitative scavenging of the H atoms, skewing the H atom reactivity pattern, and explaining the disparity of the literature data on the H + (CH{sub 3}){sub 3}COH rate constant. The ubiquitous use of tert-butyl alcohol in pulse radiolysis for investigating H atom reactivity and the results of this work suggest that many other previously reported rate constants for the H atom, particularly the smaller ones, may be in jeopardy.

  8. A New Time-Dependent Scattering Theory: Application to the Capture of Antiprotons by Hydrogen Atoms and Helium Atoms

    SciTech Connect

    Tong, X. M.; Hino, K.; Toshima, N.

    2008-08-08

    We present a theoretical method for Coulomb three-body rearrangement collisions solving a Chew-Goldberger-type integral equation directly. The scattering boundary condition is automatically satisfied by adiabatically switching on the interaction between the projectile and target. Hence the outgoing wave function is obtained without the tedious procedure of adjusting the total wave function in the asymptotic region. All the dynamical information can be derived from the scattering wave function obtained on pseudo-spectral grids numerically. Using this method, we obtained the state-specified capture cross sections when antiprotons collide with hydrogen atoms or helium atoms. Differing from the capture processes of antiprotons by hydrogen atoms, the anomalous bumpy structures are revealed in the total angular momentum dependent capture cross sections by helium atoms. Further analysis shows that the bumps arise from the partial channel closing due to the removal of the energy degeneracy in the antiprotonic helium atom. The ejected electron energy distributions are also provided for the comparison with future experiments.

  9. Recombination of 5-eV O(3P) atoms with surface-adsorbed NO - Spectra and their dependence on surface material and temperature

    NASA Technical Reports Server (NTRS)

    Orient, O. J.; Martus, K. E.; Chutjian, A.; Murad, E.

    1992-01-01

    Measurements have been conducted of the 300-850 nm recombination spectra associated with 5-eV collisions of O(3P) atoms with NO adsorbed on surfaces of MgF2, Ni, and Ti. Attention is given to the dependence of chemiluminescence intensity on surface temperature over the 240-340 K range. While all three materials tend to emit at the lower temperatures, MgF2 exhibits the greatest tendency to chemiluminescence. Both results are reflective of the greater packing density of surface-adsorbed NO at the lower temperatures for each surface. The activation energy for each surface is independent of emission wavelength, so that the same species is emitting throughout the wavelength range.

  10. Adsorptive Removal of Pharmaceuticals and Personal Care Products from Water with Functionalized Metal-organic Frameworks: Remarkable Adsorbents with Hydrogen-bonding Abilities

    PubMed Central

    Seo, Pill Won; Bhadra, Biswa Nath; Ahmed, Imteaz; Khan, Nazmul Abedin; Jhung, Sung Hwa

    2016-01-01

    Adsorption of typical pharmaceuticals and personal care products (PPCPs) (such as naproxen, ibuprofen and oxybenzone) from aqueous solutions was studied by using the highly porous metal-organic framework (MOF) MIL-101 with and without functionalization. Adsorption results showed that MIL-101s with H-donor functional groups such as –OH and –NH2 were very effective for naproxen adsorption, despite a decrease in porosity, probably because of H-bonding between O atoms on naproxen and H atoms on the adsorbent. For this reason, MIL-101 with two functional groups capable of H-bonding (MIL-101-(OH)2) exhibited remarkable adsorption capacity based on adsorbent surface area. The favorable contributions of –OH and –(OH)2 on MIL-101 in the increased adsorption of ibuprofen and oxybenzone (especially based on porosity) confirmed again the importance of H-bonding mechanism. The adsorbent with the highest adsorption capacity, MIL-101-OH, was very competitive when compared with carbonaceous materials, mesoporous materials, and pristine MIL-101. Moreover, the MIL-101-OH could be recycled several times by simply washing with ethanol, suggesting potential application in the adsorptive removal of PPCPs from water. PMID:27695005

  11. Adsorptive Removal of Pharmaceuticals and Personal Care Products from Water with Functionalized Metal-organic Frameworks: Remarkable Adsorbents with Hydrogen-bonding Abilities

    NASA Astrophysics Data System (ADS)

    Seo, Pill Won; Bhadra, Biswa Nath; Ahmed, Imteaz; Khan, Nazmul Abedin; Jhung, Sung Hwa

    2016-10-01

    Adsorption of typical pharmaceuticals and personal care products (PPCPs) (such as naproxen, ibuprofen and oxybenzone) from aqueous solutions was studied by using the highly porous metal-organic framework (MOF) MIL-101 with and without functionalization. Adsorption results showed that MIL-101s with H-donor functional groups such as –OH and –NH2 were very effective for naproxen adsorption, despite a decrease in porosity, probably because of H-bonding between O atoms on naproxen and H atoms on the adsorbent. For this reason, MIL-101 with two functional groups capable of H-bonding (MIL-101-(OH)2) exhibited remarkable adsorption capacity based on adsorbent surface area. The favorable contributions of –OH and –(OH)2 on MIL-101 in the increased adsorption of ibuprofen and oxybenzone (especially based on porosity) confirmed again the importance of H-bonding mechanism. The adsorbent with the highest adsorption capacity, MIL-101-OH, was very competitive when compared with carbonaceous materials, mesoporous materials, and pristine MIL-101. Moreover, the MIL-101-OH could be recycled several times by simply washing with ethanol, suggesting potential application in the adsorptive removal of PPCPs from water.

  12. Experimental investigations of electron capture from atomic hydrogen and deuterium by alpha particles

    SciTech Connect

    Gay, T.J.; Park, J.T.

    1992-01-01

    We report progress made during the period 15 September 1991--14 September 1992 on the project Experimental Investigations of Electron Capture from Atomic Hydrogen and Deuterium by Alpha Particles''. In the past year we have developed reliable, narrow energy spread, high-current sources of He[sup ++] based on direct-current magentron and electron-cyclotron resonance discharges. These sources have been proven on our test bench accelerator which has been upgraded to also allow us to test atomic hydrogen effusive targets. We have thus made substantial progress toward our goal of studying single electron capture from atomic hydrogen by doubly-ionized helium. A research plan for the upcoming year is also presented.

  13. Hydrogen atom wave function and eigen energy in the Rindler space

    NASA Astrophysics Data System (ADS)

    Dai, De-Chang

    2016-10-01

    We study the hydrogen atom eigenstate energy and wave function in the Rindler space. The probability distribution is tilted because the electric field of the nucleus is no longer spherically symmetric. The hydrogen atom therefore cannot be treated exactly in the same way as what it is in an inertial frame. We also find that if the external force accelerates only the nucleus and then the nucleus accelerates its surrounding electrons through electromagnetic force, the electrons can tunnel through the local energy gap and split the hydrogen atom into an ion. This is similar to what one expects from the Stark effect. However, the critical acceleration is about 3 ×1022 m /s2. It is well beyond the gravitational acceleration on a regular star surface.

  14. A massive cloud of cold atomic hydrogen in the outer Galaxy.

    PubMed

    Knee, L B; Brunt, C M

    2001-07-19

    A large fraction of the mass of the interstellar medium in our Galaxy is in the form of warm (103-104 K) and cool (50-100 K) atomic hydrogen (H i) gas. Cold (10-30 K) regions are thought to be dominated by dense clouds of molecular hydrogen. Cold H i is difficult to observe, and therefore our knowledge of its abundance and distribution in the interstellar medium is poor. The few known clouds of cold H i are much smaller in size and mass than typical molecular clouds. Here we report the discovery that the H i supershell GSH139-03-69 is very cold (10 K). It is about 2 kiloparsecs in size and as massive as the largest molecular complexes. The existence of such an immense structure composed of cold atomic hydrogen in the interstellar medium runs counter to the prevailing view that cold gas resides almost exclusively in clouds dominated by molecular hydrogen.

  15. Lewis acid-water/alcohol complexes as hydrogen atom donors in radical reactions.

    PubMed

    Povie, Guillaume; Renaud, Philippe

    2013-01-01

    Water or low molecular weight alcohols are, due to their availability, low price and low toxicity ideal reagents for organic synthesis. Recently, it was reported that, despite the very strong BDE of the O-H bond, they can be used as hydrogen atom donors in place of expensive and/or toxic group 14 metal hydrides when boron and titanium(III) Lewis acids are present. This finding represents a considerable innovation and uncovers a new perspective on the paradigm of hydrogen atom transfers to radicals. We discuss here the influence of complex formation and other association processes on the efficacy of the hydrogen transfer step. A delicate balance between activation by complex formation and deactivation by further hydrogen bonding is operative.

  16. Performance evaluation of the SAO VLG-11 atomic hydrogen masers

    NASA Technical Reports Server (NTRS)

    Levine, M. W.; Vessot, R. F.; Mattison, E. M.

    1978-01-01

    A new generation of frequency standards, the VLG-11 hydrogen maser, has been designed and built at the Smithsonian Astrophysical Observatory (SAO). A comprehensive series of environmental and short-term stability tests on three VLG-11 masers has been completed and evaluated. The test results reported here show substantial improvements over previous hydrogen masers in measured sensitivity to variations in ambient temperature, barometric pressure, and magnetic fields. The maser frequency stability, as represented by the two-sample (Allan) variance, has been measured for averaging times ranging from 1 to 100,00 seconds. The variance is lower than 1 x 10 to the -15th for averaging intervals between 1400 and 20,000 seconds. For times shorter than 4000 seconds, the measured stability data agree remarkably well with theoretical values calculated from thermal noise mechanisms and the 'noise within the linewidth' regime is clearly discernable in the data.

  17. Atomic force microscopy study of the interaction between adsorbed poly(ethylene oxide) layers: effects of surface modification and approach velocity.

    PubMed

    McLean, Scott C; Lioe, Hadi; Meagher, Laurence; Craig, Vincent S J; Gee, Michelle L

    2005-03-15

    The interaction forces between layers of the triblock copolymer Pluronic F108 adsorbed onto hydrophobic radio frequency glow discharge (RFGD) thin film surfaces and hydrophilic silica, in polymer-free 0.15 M NaCl solution, have been measured using the atomic force microscope (AFM) colloid probe technique. Compression of Pluronic F108 layers adsorbed on the hydrophobic RFGD surfaces results in a purely repulsive force due to the steric overlap of the layers, the form of which suggests that the PEO chains adopt a brush conformation. Subsequent fitting of these data to the polymer brush models of Alexander-de Gennes and Milner, Witten, and Cates confirms that the adsorbed Pluronic F108 adsorbs onto hydrophobic surfaces as a polymer brush with a parabolic segment density profile. In comparison, the interaction between Pluronic F108 layers adsorbed on silica exhibits a long ranged shallow attractive force and a weaker steric repulsion. The attractive component is reasonably well described by van der Waals forces, but polymer bridging cannot be ruled out. The weaker steric component of the force suggests that the polymer is less densely packed on the surface and is less extended into solution, existing as polymeric isolated mushrooms. When the surfaces are driven together at high piezo ramp velocities, an additional repulsive force is measured, attributable to hydrodynamic drainage forces between the surfaces. In comparing theoretical predictions of the hydrodynamic force to the experimentally obtained data, agreement could only be obtained if the flow profile of the aqueous solution penetrated significantly into the polymer brush. This finding is in line with the theoretical predictions of Milner and provides further evidence that the segment density profile of the adsorbed polymer brush is parabolic. A velocity dependent additional stepped repulsive force, reminiscent of a solvation oscillatory force, is also observed when the adsorbed layers are compressed under high

  18. Atomic Hydrogen Measurements in a Fusion-Relevant Plasma

    NASA Astrophysics Data System (ADS)

    Samuell, Cameron; Corr, Cormac

    2012-10-01

    Critical to the success of large-scale fusion reactors is the development of new materials that can withstand the extreme conditions at the plasma-surface boundary. The materials required for plasma-facing components will need to withstand a very aggressive environment that is characterized by both a high heat load and high ion flux produced by the hydrogen isotope plasma. As such, investigating the ways in which hydrogen plasmas interact with a range of materials is an important area for research and development and is vital to the future success of fusion. A new experimental reactor, the MAGnetized Plasma Interaction Experiment (MAGPIE), has been constructed at the Australian National University to help resolve some of the critical issues surrounding the choice of fusion reactor materials. MAGPIE is a linear system with a 2.5kW, 13.56MHz helicon source that operates in a magnetic hill configuration with field strengths up to 0.19T. Densities up to 10^19m-3 at temperatures < 5eV have been achieved. The focus of this presentation is the interaction between a magnetized hydrogen plasma and tungsten and graphite targets in MAGPIE. Results from two-photon absorption laser induced fluorescence (TALIF), optical emission spectroscopy (OES) and probe diagnostics will be presented.

  19. Cooper-type minima in multipole cross sections of atomic hydrogen

    SciTech Connect

    Fazio, P.M.; Copeland, G.E.

    1984-07-09

    The quadrupole photoionization cross sections for hydrogen are shown to contain minima at kinetic energies of the free electron that are less than 2 eV. These minima are the result of zeros that occur in some of the quadrupole transition strengths between bound excited (Vertical Barn,l>) and continuum (Vertical BarW,l+2>) states for atomic hydrogen. These minima are compared with Cooper minima which occur in the photoionization cross sections for some multielectron systems.

  20. Resonant Coherent Excitation of Fast Hydrogen Atoms in Front of a LiF(001) Surface

    SciTech Connect

    Auth, C.; Mertens, A.; Winter, H.; Borisov, A.G.; Garcia de Abajo, F.J.

    1997-12-01

    We have scattered protons and hydrogen atoms with energies of some keV from a LiF(001) surface under a grazing angle of incidence. From the intensity of Lyman-{alpha} radiation (transition from n=2 to n=1, {lambda}=121.6 nm ) as a function of projectile energy for different azimuthal orientations of the crystal surface, we find clear evidence for a resonant coherent excitation of n=2 states of hydrogen atoms in the oscillating electric field in front of the insulator surface. {copyright} {ital 1997} {ital The American Physical Society}

  1. Deformylation Reaction by a Nonheme Manganese(III)-Peroxo Complex via Initial Hydrogen-Atom Abstraction.

    PubMed

    Barman, Prasenjit; Upadhyay, Pranav; Faponle, Abayomi S; Kumar, Jitendra; Nag, Sayanta Sekhar; Kumar, Devesh; Sastri, Chivukula V; de Visser, Sam P

    2016-09-01

    Metal-peroxo intermediates are key species in the catalytic cycles of nonheme metalloenzymes, but their chemical properties and reactivity patterns are still poorly understood. The synthesis and characterization of a manganese(III)-peroxo complex with a pentadentate bispidine ligand system and its reactivity with aldehydes was studied. Manganese(III)-peroxo can react through hydrogen-atom abstraction reactions instead of the commonly proposed nucleophilic addition reaction. Evidence of the mechanism comes from experiments which identify a primary kinetic isotope effect of 5.4 for the deformylation reaction. Computational modeling supports the established mechanism and identifies the origin of the reactivity preference of hydrogen-atom abstraction over nucleophilic addition.

  2. Deuterium removal from radiation damage in tungsten by isotopic exchange with hydrogen atomic beam

    NASA Astrophysics Data System (ADS)

    Ogorodnikova, O. V.; Markelj, S.; Efimov, V. S.; Gasparyan, Yu M.

    2016-09-01

    The tungsten samples were pre-irradiated with self-ions to create radiation-induced defects and then exposed to the deuterium atomic beam. The deuterium removal was studied by isotopic exchange with atomic hydrogen beam. Modification of the deuterium depth profile in self-ion irradiated tungsten under isotopic exchange up to a depth of 6 μm was measured in- situ by nuclear reaction analysis. The total deuterium retention after isotopic exchange was measured by thermal desorption spectroscopy. It is shown that the efficiency of the deuterium removal increases with increasing of the hydrogen incident flux, incident energy and temperature of the tungsten sample.

  3. Reduction of uranium hexafluoride to tetrafluoride by using the hydrogen atoms

    NASA Astrophysics Data System (ADS)

    Aleksandrov, B. P.; Gordon, E. B.; Ivanov, A. V.; Kotov, A. A.; Smirnov, V. E.

    2016-09-01

    We consider the reduction of UF6 to UF4 by chemical reaction with hydrogen atoms originated in the powerful chemical generator. The principal design of such a chemical convertor is described. The results of the mathematical modeling of the thermodynamics and kinetics of the UF6 to UF4 reduction process are analyzed. The few options for the hydrogen atom generator design are proposed. A layout of the experimental setup with the chemical reactor is presented. The high efficiency together with the ability of the process scaling without loss of its efficiency makes this approach to the uranium hexafluoride depletion into tetrafluoride promising for its application in the industry.

  4. Atomic hydrogen beam source: a convenient, extended cavity, microwave discharge design.

    PubMed

    Murphy, E J; Brophy, J H

    1979-05-01

    An extended cavity design of a microwave discharge source for production of intense beams of atomic, radical, and metastable species in vacuo is described. The extended cavity enables the discharge to be run at the beam source nozzle while the power connection and tuning elements remain conveniently outside the apparatus. This design minimizes wall recombination losses to produce intense atomic hydrogen beams with considerably less engineering than previous discharge sources.

  5. Ground state properties of solid and liquid spin-aligned atomic hydrogen

    NASA Technical Reports Server (NTRS)

    Danilowicz, R. L.; Dugan, J. V., Jr.; Etters, R. D.

    1976-01-01

    Calculations of the ground state energy in the solid phase were performed with the aid of a variational approach. The Morse potential form of the atomic triple potential computed by Kolos and Wolniewicz (1965) was employed for the calculations. The ground state energies of both the liquid and solid phases of spin-aligned atomic hydrogen around the volume of the transition are presented in a graph.

  6. Role of hydrogen in the chemical vapor deposition growth of MoS2 atomic layers

    NASA Astrophysics Data System (ADS)

    Li, Xiao; Li, Xinming; Zang, Xiaobei; Zhu, Miao; He, Yijia; Wang, Kunlin; Xie, Dan; Zhu, Hongwei

    2015-04-01

    Hydrogen plays a crucial role in the chemical vapor deposition (CVD) growth of graphene. Here, we have revealed the roles of hydrogen in the two-step CVD growth of MoS2. Our study demonstrates that hydrogen acts as the following: (i) an inhibitor of the thermal-induced etching effect in the continuous film growth process; and (ii) a promoter of the desulfurization reaction by decreasing the S/Mo atomic ratio and the oxidation reaction of the obtained MoSx (0 < x < 2) films. A high hydrogen content of more than 100% in argon forms nano-sized circle-like defects and damages the continuity and uniformity of the film. Continuous MoS2 films with a high crystallinity and a nearly perfect S/Mo atomic ratio were finally obtained after sulfurization annealing with a hydrogen content in the range of 20%-80%. This insightful understanding reveals the crucial roles of hydrogen in the CVD growth of MoS2 and paves the way for the controllable synthesis of two-dimensional materials.Hydrogen plays a crucial role in the chemical vapor deposition (CVD) growth of graphene. Here, we have revealed the roles of hydrogen in the two-step CVD growth of MoS2. Our study demonstrates that hydrogen acts as the following: (i) an inhibitor of the thermal-induced etching effect in the continuous film growth process; and (ii) a promoter of the desulfurization reaction by decreasing the S/Mo atomic ratio and the oxidation reaction of the obtained MoSx (0 < x < 2) films. A high hydrogen content of more than 100% in argon forms nano-sized circle-like defects and damages the continuity and uniformity of the film. Continuous MoS2 films with a high crystallinity and a nearly perfect S/Mo atomic ratio were finally obtained after sulfurization annealing with a hydrogen content in the range of 20%-80%. This insightful understanding reveals the crucial roles of hydrogen in the CVD growth of MoS2 and paves the way for the controllable synthesis of two-dimensional materials. Electronic supplementary

  7. Coupled Electron-Ion Monte Carlo calculations of atomic hydrogen

    NASA Astrophysics Data System (ADS)

    Holzmann, Markus; Pierleoni, Carlo; Ceperley, David M.

    2005-07-01

    We present a new Monte Carlo method which couples Path Integral for finite temperature protons with Quantum Monte Carlo for ground state electrons, and we apply it to metallic hydrogen for pressures beyond molecular dissociation. This method fills the gap between high temperature electron-proton Path Integral and ground state Diffusion Monte Carlo methods. Our data exhibit more structure and higher melting temperatures of the proton crystal than Car-Parrinello Molecular Dynamics results using LDA. We further discuss the quantum motion of the protons and the zero temperature limit.

  8. Nucleon polarizabilities: From Compton scattering to hydrogen atom

    NASA Astrophysics Data System (ADS)

    Hagelstein, Franziska; Miskimen, Rory; Pascalutsa, Vladimir

    2016-05-01

    We review the current state of knowledge of the nucleon polarizabilities and of their role in nucleon Compton scattering and in hydrogen spectrum. We discuss the basic concepts, the recent lattice QCD calculations and advances in chiral effective-field theory. On the experimental side, we review the ongoing programs aimed to measure the nucleon (scalar and spin) polarizabilities via the Compton scattering processes, with real and virtual photons. A great part of the review is devoted to the general constraints based on unitarity, causality, discrete and continuous symmetries, which result in model-independent relations involving nucleon polarizabilities. We (re-)derive a variety of such relations and discuss their empirical value. The proton polarizability effects are presently the major sources of uncertainty in the assessment of the muonic hydrogen Lamb shift and hyperfine structure. Recent calculations of these effects are reviewed here in the context of the "proton-radius puzzle". We conclude with summary plots of the recent results and prospects for the near-future work.

  9. Linear quadratic stochastic control of atomic hydrogen masers.

    PubMed

    Koppang, P; Leland, R

    1999-01-01

    Data are given showing the results of using the linear quadratic Gaussian (LQG) technique to steer remote hydrogen masers to Coordinated Universal Time (UTC) as given by the United States Naval Observatory (USNO) via two-way satellite time transfer and the Global Positioning System (GPS). Data also are shown from the results of steering a hydrogen maser to the real-time USNO mean. A general overview of the theory behind the LQG technique also is given. The LQG control is a technique that uses Kalman filtering to estimate time and frequency errors used as input into a control calculation. A discrete frequency steer is calculated by minimizing a quadratic cost function that is dependent on both the time and frequency errors and the control effort. Different penalties, chosen by the designer, are assessed by the controller as the time and frequency errors and control effort vary from zero. With this feature, controllers can be designed to force the time and frequency differences between two standards to zero, either more or less aggressively depending on the application.

  10. Use of Ni/NixB Nanoparticles as a Novel Adsorbent for the Preconcentration of Mercury Species prior to Cold Vapor-Atomic Fluorescence Spectrometric Determination.

    PubMed

    Yayayürük, Onur; Henden, Emür

    2016-01-01

    A selective matrix separation/enrichment method, utilizing a simple batch procedure with nickel/nickel boride (Ni/NixB) nanoparticles was proposed for the determination of inorganic mercury(II), Hg(2+) and methyl mercury(I), CH3Hg(+) in waters prior to cold vapor-atomic fluorescence spectrometry (CV-AFS). The Ni/NixB nanoparticles, were synthesized by the chemical reduction of Ni(II) to Ni/NixB. The novel adsorbent was selective to Hg(2+) and CH3Hg(+) species between pH values of 4 - 10. Both of the mercury species were recovered from the adsorbent using 1.0 mol L(-1) hot HNO3 with high efficiency. It was observed that the adsorbent selectively removed Hg(2+) and CH3Hg(+) from the bulk solution in the presence of several competitor ions (As(3+), Sb(3+), Pb(2+), Zn(2+), Cu(2+), Cd(2+) and Fe(3+)) with ≥96% adsorption. The limit of detection (3σ above blank) was found to be 1.8 ng L(-1) with a preconcentration factor of 20. The validation of the method was tested through spike recovery experiments with several water samples (tap and seawater) at μg L(-1) concentration levels, and all recovery values were found to vary between 95 and 105%. PMID:27506713

  11. Structural transformation of hydrogen-adsorbed Si(111)-√3×√3-Ag surfaces induced by electron-stimulated desorption

    NASA Astrophysics Data System (ADS)

    Watanabe, Heiji; Ichikawa, Masakazu

    1997-07-01

    Atomic hydrogen irradiated Si(111)-√3×√3-Ag surfaces, which involve nanometer size Ag clusters and hydrogen terminated regions, are studied by combined surface analysis with ultrahigh-vacuum scanning electron microscopy (UHV-SEM), scanning reflection electron microscopy (SREM), microprobe reflection high-energy electron diffration (μ-RHEED) and Auger electron spectroscopy (AES). Electron beam irradiation onto this surface results in disappearance of the Ag clusters, and subsequent low-temperature annealing at 275°C transforms the surface to the original √3×√3-Ag structure. Hydrogen removal from the Si surface induced by electron-stimulated desorption (ESD) and surface diffusion of Ag atoms on the bare regions by low-temperature annealing explain this structural transformation.

  12. Hydrogen transport diagnostics by atomic and molecular emission line profiles simultaneously measured for large helical device

    SciTech Connect

    Fujii, K.; Shikama, T.; Hasuo, M.; Goto, M.; Morita, S.

    2013-01-15

    We observe the Balmer-{alpha}, -{beta}, and -{gamma} lines of hydrogen atoms and Q branches of the Fulcher-{alpha} band of hydrogen molecules simultaneously with their polarization resolved for large helical device. From the fit including the line splits and the polarization dependences by the Zeeman effect, the emission locations, intensities, and the temperatures of the atoms and molecules are determined. The emission locations of the hydrogen atoms are determined outside but close to the last closed flux surface (LCFS). The results are consistent with a previous work (Phys. Plasmas 12, 042501 (2005)). On the other hand, the emission locations of the molecules are determined to be in the divertor legs, which is farer from those of the atoms. The kinetic energy of the atoms is 1 {approx} 20 eV, while the rotational temperature of molecules is {approx}0.04 eV. Additionally, substantial wings, which originate from high velocity atoms and are not reproduced by the conventional spectral analysis, are observed in the Balmer line profiles. We develop a one-dimensional model to simulate the transport of the atoms and molecules. The model reproduces the differences of the emission locations of the atoms and molecules when their initial temperatures are assumed to be 3 eV and 0.04 eV, respectively. From the model, the wings of the Balmer-{alpha} line is attributed to the high velocity atoms exist deep inside the LCFS, which are generated by the charge exchange collisions with hot protons there.

  13. Zirconium-nickel crystals—hydrogen accumulators: Dissolution and penetration of hydrogen atoms in alloys

    NASA Astrophysics Data System (ADS)

    Matysina, Z. A.; Zaginaichenko, S. Yu.; Shchur, D. V.; Gabdullin, M. T.; Kamenetskaya, E. A.

    2016-07-01

    The calculation of the free energy, thermodynamic equilibrium equations, and kinetic equations of the intermetallic compound Zr2NiH x has been carried out based on molecular-kinetic concepts. The equilibrium hydrogen concentration depending on the temperature, pressure, and energy parameters has been calculated. The absorption-desorption of hydrogen has been studied, and the possibility of the realization of the hysteresis effect has been revealed. The kinetics of the dissolution and permeability of hydrogen is considered, the time dependence of these values has been found, and conditions for the extremum character of their time dependence have been determined. Relaxation times of the dissolution and permeability of hydrogen into the alloy have been calculated. The calculation results are compared with the experimental data available in the literature.

  14. Cathodic reduction of oxygen and hydrogen peroxide at cobalt and iron crowned phthalocyanines adsorbed on highly oriented pyrolytic graphite electrodes

    SciTech Connect

    Kobayashi, N.; Janda, P.; Lever, A.B.P. )

    1992-12-09

    The surface electrochemistry of iron and cobalt crowned phthalocyanine (Fe[sup II]CRPc(-2) and Co[sup II]CRPc(-2)) adsorbed on a highly oriented pyrolytic graphite (HOPG) electrode has been explored under an argon atmosphere. The redox processes of surface bound Co[sup II]CRPc(-2)/[Co[sup I]CRPc(-2)][sup [minus

  15. STEM Imaging of Single Pd Atoms in Activated Carbon Fibers Considered for Hydrogen Storage

    SciTech Connect

    Van Benthem, Klaus; Bonifacio, Cecile S; Contescu, Cristian I; Pennycook, Stephen J; Gallego, Nidia C

    2011-01-01

    Aberration corrected scanning transmission electron microscopy was used to demonstrate the feasibility of imaging individual Pd atoms that are highly dispersed throughout the volume of activated carbon fibers. Simultaneous acquisition of high-angle annular dark-field and bright-field images allows correlation of the location of single Pd atoms with microstructural features of the carbon host material. Sub-Angstrom imaging conditions revealed that 18 wt% of the total Pd content is dispersed as single Pd atoms in three re-occurring local structural arrangements. The identified structural configurations may represent effective storage sites for molecular hydrogen through Kubas complex formation as discussed in detail in the preceding article.

  16. Continuous spectra of atomic hydrogen in a strong magnetic field

    NASA Astrophysics Data System (ADS)

    Zhao, L. B.; Zatsarinny, O.; Bartschat, K.

    2016-09-01

    We describe a theoretical method, developed in the coupled-channel formalism, to study photoionization of H atoms in a strong magnetic field of a size that is typical for magnetic white dwarfs. The coupled Schrödinger equations are solved numerically using the renormalized Numerov method proposed by Johnson [B. R. Johnson, J. Chem. Phys. 67, 4086 (1977), 10.1063/1.435384; B. R. Johnson, J. Chem. Phys. 69, 4678 (1978), 10.1063/1.436421]. The distinct advantage of this method is the fact that no overflow problems are encountered in the classically forbidden region, and hence the method exhibits excellent numerical stability. Photoionization cross sections are presented for magnetized H atoms in the ground and 2 p excited states. The calculated results are compared with those obtained by other theories. The present method is particularly useful for explaining the complex features of continuous spectra in a strong magnetic field and hence provides an efficient tool for modeling photoionization spectra observed in the atmosphere of magnetic white dwarfs.

  17. Detecting Hydrogen Atoms in Solid Parahydrogen Using FTIR Spectroscopy

    NASA Astrophysics Data System (ADS)

    Anderson, David T.; Ruzi, Mahmut

    2012-06-01

    Our group is currently studying the 193.3 nm photochemistry of a number of precursor molecules isolated in solid parahydrogen (pH_2) using high-resolution FTIR spectroscopy. In photochemical studies of formic acid and ammonia, right after the photolysis laser is turned off, we observe metastable satellite peaks in close proximity to the strong rovibrational transition out of the ground state of the respective monomer photoproducts H_2O and NH_3. In both cases, there are two satellite peaks near the R(0) monomer transition. We have assigned these satellite features to H-H_2O and H-NH_3 radical clusters that form via reactions of the photoproduct with the pH_2 host. We will present IR spectroscopic studies of these two H-atom cluster systems that we hope to use in future photochemical studies to measure the concentration of H-atoms in our sample using FTIR spectroscopy. K. A. Kufeld, W. R. Wonderly, L. O. Paulson, S. C. Kettwich, and D. T. Anderson, J. Phys. Chem. Lett. 3, 342-347 (2012).

  18. Dry soldering with hot filament produced atomic hydrogen

    DOEpatents

    Panitz, J.K.G.; Jellison, J.L.; Staley, D.J.

    1995-04-25

    A system is disclosed for chemically transforming metal surface oxides to metal that is especially, but not exclusively, suitable for preparing metal surfaces for dry soldering and solder reflow processes. The system employs one or more hot, refractory metal filaments, grids or surfaces to thermally dissociate molecular species in a low pressure of working gas such as a hydrogen-containing gas to produce reactive species in a reactive plasma that can chemically reduce metal oxides and form volatile compounds that are removed in the working gas flow. Dry soldering and solder reflow processes are especially applicable to the manufacture of printed circuit boards, semiconductor chip lead attachment and packaging multichip modules. The system can be retrofitted onto existing metal treatment ovens, furnaces, welding systems and wave soldering system designs. 1 fig.

  19. Dry soldering with hot filament produced atomic hydrogen

    DOEpatents

    Panitz, Janda K. G.; Jellison, James L.; Staley, David J.

    1995-01-01

    A system for chemically transforming metal surface oxides to metal that is especially, but not exclusively, suitable for preparing metal surfaces for dry soldering and solder reflow processes. The system employs one or more hot, refractory metal filaments, grids or surfaces to thermally dissociate molecular species in a low pressure of working gas such as a hydrogen-containing gas to produce reactive species in a reactive plasma that can chemically reduce metal oxides and form volatile compounds that are removed in the working gas flow. Dry soldering and solder reflow processes are especially applicable to the manufacture of printed circuit boards, semiconductor chip lead attachment and packaging multichip modules. The system can be retrofitted onto existing metal treatment ovens, furnaces, welding systems and wave soldering system designs.

  20. The distribution of atomic hydrogen in the magnetosphere of Saturn

    NASA Technical Reports Server (NTRS)

    Shemansky, D. E.; Hall, D. T.

    1992-01-01

    Three sets of previously unpublished Voyager ultraviolet spectrometer observations of the Saturn system conducted by Voyager 1 and 2 are presented. Voyager 1 observations during the postencounter period provided a map of the distribution looking down on the equatorial plane. The reduced data show a nonuniform distribution in local time with a preponderance of emission on the duskside. The emission extends radially inward to the top of the Saturn atmosphere with stronger signals appearing close to the planet, strongly suggesting that the principal source is the sunlit Saturn atmosphere. In the subsolar sector of the magnetosphere no excess emission in the vicinity of Titan's orbit is detectable. Voyager 1 and 2 preencounter observations also show H Ly-alpha emissions increasing monotonically toward the planet but with a distinctive dawnside excess. It is concluded that the preliminary results reporting a toroidal hydrogen distribution with a cavity inside 8 RS are invalid because of limited spatial resolution and poor statistics.

  1. The distribution of atomic hydrogen in the Jovian atmosphere

    NASA Technical Reports Server (NTRS)

    Killen, R. M.; Chamberlain, J. W.

    1986-01-01

    An analysis is presented of the Voyager and IUE lyman alpha spectra of the Jovian equatorial emission in which was derived a zonal asymmetry in the hydrogen column abundance. Using two estimates of the fraction of Lyman alpha which is due to direct excitation by charged particle precipitation from the ionosphere, upper and lower limits were derived to the H column abundance within and without the perturbed region. That the asymmetry in H abundance may be due to localized heating near the homopause with a consequent rise in scale height is shown. The derived exospheric temperature remains fairly constant with longitude. The required additional heat input over the bulge region, 0.02 erg/cm/s, is supplied by an additional flux of magnetospheric electrons due to Jupiter's magnetic anomaly.

  2. Compression experiments with spin-polarized atomic hydrogen

    NASA Astrophysics Data System (ADS)

    Sprik, R.; Walraven, J. T. M.; Silvera, Isaac F.

    1985-11-01

    Doubly polarized hydrogen has been produced up to densities of 2×1018 cm-3 with the use of a compression technique. Samples were compressed up to five orders of magnitude into small bubblelike volumes under a column of liquid helium. This technique enabled us to study the volume decay of a bubble at almost constant gas density for minutes. The analysis of the volume decay of such a bubble is discussed. A bulk three-body recombination process was observed with rate constant C3=[7(2)]×10-39 cm6 s-1, as well as bulk electronic b-->c relaxation with rate constant Gvbc↓=[12(4)]×10-16 cm3 s-1. The nature of the three-body process is analyzed with a set of extended rate equations. The samples were very delicate and rapid compressions could result in explosions.

  3. The role of Cu atoms on silver electrodes in surface enhanced Raman scattering from pyridine: Giant enhancement by a minority of adsorbed molecules

    NASA Astrophysics Data System (ADS)

    Moerl, Ludwig; Pettinger, Bruno

    1982-08-01

    Surface enhanced Raman scattering (SERS) has been studied for pyridine molecules adsorbed at Ag electrodes covered with submonolayers of Cu ( θ = 0.003 - 0.1). Depending on the amount of Cu coverage the frequencies of the breathing vibrations shift, and new breathing modes appear. Obviously two types of pyridine complexes are formed, differing in the nature of the bonding provided either by copper or silver surface atoms. The generation and quenching behaviour of SERS at rough electrodes evidence the importance of metastable atomic surface structures for SERS and indicate the cooperation of local and non-local enhancement processes. Since active sites can be stabilized with traces of Cu at the silver electrode, the enhancement factor on a molecular basis appears to be by one order of magnitude larger than earlier anticipated, and ranges from 2 × 10 6 to 1.6 × 10 7 for an exciting wavelength at 514.5 nm or 647.1 nm, respectively.

  4. Continuous vs. discrete models for the quantum harmonic oscillator and the hydrogen atom

    NASA Astrophysics Data System (ADS)

    Lorente, Miguel

    2001-07-01

    The Kravchuk and Meixner polynomials of discrete variable are introduced for the discrete models of the harmonic oscillator and hydrogen atom. Starting from Rodrigues formula we construct raising and lowering operators, commutation and anticommutation relations. The physical properties of discrete models are figured out through the equivalence with the continuous models obtained by limit process.

  5. Compensation of logarithmic corrections in calculating the fine structure of levels in hydrogen-like atoms

    SciTech Connect

    Boikova, N. A. Tyukhtyaev, Yu. N.; Faustov, R. N.

    2011-01-15

    Special features of the quasipotential approach to calculating logarithmic (in the fine-structure constant) contributions to the fine splitting of energy levels in hydrogen-like atoms are analyzed. The boundaries of the region of applicability of the Fell technique are indicated, and the order of corrections beyond this region is estimated.

  6. Moøller polarimetry with polarized atomic hydrogen at MESA

    SciTech Connect

    Bartolomé, P. Aguar; Aulenbacher, K.; Tyukin, V.

    2013-11-07

    A new generation of parity violation (PV) electron scattering experiments are planned to be carried out at the Institut für Kernphysik in Mainz. These experiments will be performed at low energies of 100-200 MeV using the new accelerator MESA (Mainz Energy recovering Superconducting Accelerator). One of the main challenges of such experiments is to achieve an accuracy in beam polarization measurements that must be below 0.5%. This very high accuracy can be reached using polarized atomic hydrogen gas, stored in an ultra-cold magnetic trap, as the target for electron beam polarimetry based on Mo/ller scattering. Electron spin-polarized atomic hydrogen can be stored at high densities of 10{sup 16} cm{sup −2}, over relatively long time periods, in a high magnetic field (8T) and at low temperatures (0.3K). The gradient force splits the ground state of the hydrogen into four states with different energies. Atoms in the low energy states are trapped in the strong magnetic field region whereas the high energy states are repelled and pumped away. The physics of ultra-cold atomic hydrogen in magnetic traps and the status of the Mainz Hydro-Mo/ller project will be presented.

  7. The Lamb shift in the hydrogen atom: Shift of s states

    SciTech Connect

    Karshenboim, S.G.

    1995-02-01

    A theoretical expression for the difference of the Lamb shifts of the 1s{sub 1/2} and 2s{sub 1/2} levels is obtained. The Lamb shift of the ground state in the hydrogen atom is recalculated and found to be 8172.898(26) MHz. 22 refs.

  8. Determination of the Relative Atomic Masses of Metals by Liberation of Molecular Hydrogen

    ERIC Educational Resources Information Center

    Waghorne, W. Earle; Rous, Andrew J.

    2009-01-01

    Students determine the relative atomic masses of calcium, magnesium, and aluminum by reaction with hydrochloric acid and measurement of the volume of hydrogen gas liberated. The experiment demonstrates stoichiometry and illustrates clearly that mass of the reagent is not the determinant of the amounts in chemical reactions. The experiment is…

  9. Learning about Regiochemistry from a Hydrogen-Atom Abstraction Reaction in Water

    ERIC Educational Resources Information Center

    Sears-Dundes, Christopher; Huon, Yoeup; Hotz, Richard P.; Pinhas, Allan R.

    2011-01-01

    An experiment has been developed in which the hydrogen-atom abstraction and the coupling of propionitrile, using Fenton's reagent, are investigated. Students learn about the regiochemistry of radical formation, the stereochemistry of product formation, and the interpretation of GC-MS data, in a safe reaction that can be easily completed in one…

  10. Effects of laser radiation field on energies of hydrogen atom in plasmas

    SciTech Connect

    Bahar, M. K.

    2015-09-15

    In this study, for the first time, the Schrödinger equation with more general exponential cosine screened Coulomb (MGECSC) potential is solved numerically in the presence of laser radiation field within the Ehlotzky approximation using the asymptotic iteration method. The MGECSC potential includes four different potential forms in consideration of different sets of the parameters in the potential. By applying laser field, the total interaction potential of hydrogen atom embedded in plasmas converts to double well-type potential. The plasma screening effects under the influence of laser field as well as confinement effects of laser field on hydrogen atom in Debye and quantum plasmas are investigated by solving the Schrödinger equation with the laser-dressed MGECSC potential. It is resulted that since applying a monochromatic laser field on hydrogen atom embedded in a Debye and quantum plasma causes to shift in the profile of the total interaction potential, the confinement effects of laser field on hydrogen atom in plasmas modeled by the MGECSC potential change localizations of energy states.

  11. Quantum dynamics of hydrogen atoms on graphene. I. System-bath modeling

    SciTech Connect

    Bonfanti, Matteo; Jackson, Bret; Hughes, Keith H.; Burghardt, Irene

    2015-09-28

    An accurate system-bath model to investigate the quantum dynamics of hydrogen atoms chemisorbed on graphene is presented. The system comprises a hydrogen atom and the carbon atom from graphene that forms the covalent bond, and it is described by a previously developed 4D potential energy surface based on density functional theory ab initio data. The bath describes the rest of the carbon lattice and is obtained from an empirical force field through inversion of a classical equilibrium correlation function describing the hydrogen motion. By construction, model building easily accommodates improvements coming from the use of higher level electronic structure theory for the system. Further, it is well suited to a determination of the system-environment coupling by means of ab initio molecular dynamics. This paper details the system-bath modeling and shows its application to the quantum dynamics of vibrational relaxation of a chemisorbed hydrogen atom, which is here investigated at T = 0 K with the help of the multi-configuration time-dependent Hartree method. Paper II deals with the sticking dynamics.

  12. Laboratory Measurements of Charge Transfer on Atomic Hydrogen at Thermal Energies

    NASA Technical Reports Server (NTRS)

    Havener, C. C.; Vane, C. R.; Krause, H. F.; Stancil, P. C.; Mroczkowski, T.; Savin, D. W.

    2002-01-01

    We describe our ongoing program to measure velocity dependent charge transfer (CT) cross sections for selected ions on atomic hydrogen using the ion-aloin merged-beams apparatus at Oak Ridge Natioiial Laboralory. Our focus is on those ions for which CT plays an important role in determining the ionization structure, line emis sion, and thermal structure of observed cosmic photoionized plasmas.

  13. Moøller polarimetry with polarized atomic hydrogen at MESA

    NASA Astrophysics Data System (ADS)

    Bartolomé, P. Aguar; Aulenbacher, K.; Tyukin, V.

    2013-11-01

    A new generation of parity violation (PV) electron scattering experiments are planned to be carried out at the Institut für Kernphysik in Mainz. These experiments will be performed at low energies of 100-200 MeV using the new accelerator MESA (Mainz Energy recovering Superconducting Accelerator). One of the main challenges of such experiments is to achieve an accuracy in beam polarization measurements that must be below 0.5%. This very high accuracy can be reached using polarized atomic hydrogen gas, stored in an ultra-cold magnetic trap, as the target for electron beam polarimetry based on Mo/ller scattering. Electron spin-polarized atomic hydrogen can be stored at high densities of 1016 cm-2, over relatively long time periods, in a high magnetic field (8T) and at low temperatures (0.3K). The gradient force splits the ground state of the hydrogen into four states with different energies. Atoms in the low energy states are trapped in the strong magnetic field region whereas the high energy states are repelled and pumped away. The physics of ultra-cold atomic hydrogen in magnetic traps and the status of the Mainz Hydro-Mo/ller project will be presented.

  14. Hydrogen atom formation from the photodissociation of water ice at 193 nm.

    PubMed

    Yabushita, Akihiro; Hashikawa, Yuichi; Ikeda, Atsushi; Kawasaki, Masahiro; Tachikawa, Hiroto

    2004-03-15

    The TOF spectra of photofragment hydrogen atoms from the 193 nm photodissociation of amorphous ice at 90-140 K have been measured. The spectra consist of both a fast and a slow components that are characterized by average translational energies of 2k(B)T(trans)=0.39+/-0.04 eV (2300+/-200 K) and 0.02 eV (120+/-20 K), respectively. The incident laser power dependency of the hydrogen atom production suggests one-photon process. The electronic excitation energy of a branched cluster, (H(2)O)(6+1), has been theoretically calculated, where (H(2)O)(6+1) is a (H(2)O)(6) cyclic cluster attached by a water molecule with the hydrogen bond. The photoabsorption of this branched cluster is expected to appear at around 200 nm. The source of the hydrogen atoms is attributed to the photodissociation of the ice surface that is attached by water molecules with the hydrogen bond. Atmospheric implications are estimated for the photodissociation of the ice particles (Noctilucent clouds) at 190-230 nm in the region between 80 and 85 km altitude.

  15. Self-interaction in Green's-function theory of the hydrogen atom

    SciTech Connect

    Nelson, W.; Bokes, P.; Rinke, Patrick; Godby, R. W.

    2007-03-15

    Atomic hydrogen provides a unique test case for computational electronic structure methods, since its electronic excitation energies are known analytically. With only one electron, hydrogen contains no electronic correlation and is therefore particularly susceptible to spurious self-interaction errors introduced by certain computational methods. In this paper we focus on many-body perturbation theory (MBPT) in Hedin's GW approximation. While the Hartree-Fock and the exact MBPT self-energy are free of self-interaction, the correlation part of the GW self-energy does not have this property. Here we use atomic hydrogen as a benchmark system for GW and show that the self-interaction part of the GW self-energy, while nonzero, is small. The effect of calculating the GW self-energy from exact wave functions and eigenvalues, as distinct from those from the local-density approximation, is also illuminating.

  16. The possibility of constructing the hydrogen scale of the absolute atomic masses of the elements

    NASA Astrophysics Data System (ADS)

    Kuz'min, I. I.

    2009-12-01

    The paper presents a scheme for the experimental-empirical construction of the existing chemical, physical, and carbon scales of the relative nonintegral atomic masses of the elements. The quantitative interrelation between the nonintegral relative atomic masses, their minimized fractional positive and negative natural deviations from integral numbers, and their integral parts are reproduced mathematically. Nonisotopic fractional deviations are shown to be a consequence of methodological side effects of the scheme for theoretical processing of the data of thorough physical and chemical measurements performed by Stas and Aston in constructing scales of relative atomic masses. In conformity with the Prout hypothesis, the absolute atomic mass unit and the corresponding Avogadro’s number value are suggested for the construction of the hydrogen scale of absolute atomic masses of nonisotopic elements, individual isotopes, and isotope-containing elements.

  17. Insights into the Electronic Structure of Ozone and Sulfur Dioxide from Generalized Valence Bond Theory: Addition of Hydrogen Atoms.

    PubMed

    Lindquist, Beth A; Takeshita, Tyler Y; Dunning, Thom H

    2016-05-01

    Ozone (O3) and sulfur dioxide (SO2) are valence isoelectronic species, yet their properties and reactivities differ dramatically. In particular, O3 is highly reactive, whereas SO2 is chemically relatively stable. In this paper, we investigate serial addition of hydrogen atoms to both the terminal atoms of O3 and SO2 and to the central atom of these species. It is well-known that the terminal atoms of O3 are much more amenable to bond formation than those of SO2. We show that the differences in the electronic structure of the π systems in the parent triatomic species account for the differences in the addition of hydrogen atoms to the terminal atoms of O3 and SO2. Further, we find that the π system in SO2, which is a recoupled pair bond dyad, facilitates the addition of hydrogen atoms to the sulfur atom, resulting in stable HSO2 and H2SO2 species.

  18. Production of Excited Atomic Hydrogen and Deuterium from HD Photodissociation

    NASA Astrophysics Data System (ADS)

    Machacek, J. R.; Bozek, J. D.; Furst, J. E.; Gay, T. J.; Gould, H.; Kilcoyne, A. L. D.; McLaughlin, K. W.

    2008-05-01

    We have measured the production of Lyα, Hα, and Hβ fluorescence from atomic H and D for the photodissociation of HD by linearly-polarized photons with energies between 20 and 66 eV. In this energy range, excited photofragments result primarily from the production of doubly-excited molecular species which promptly autoionize or dissociate into two neutrals. Theoretical calculation are not yet available for HD, but comparison between the relative cross sections for H2, D2 and HD targets and the available theory for H2 and D2 [1] allow for an estimate of the relative strength of each dissociation channel in this energy range. [1] J. D. Bozek et al., J. Phys. B 39, 4871 (2006). Support provided by the NSF (Grant PHY-0653379), DOE (LBNL/ALS) and ANSTO (Access to Major Research Facilities Programme).

  19. Hydrogen atom initiated chemistry. [chemical evolution in planetary atmospheres

    NASA Technical Reports Server (NTRS)

    Hong, J. H.; Becker, R. S.

    1979-01-01

    H Atoms have been created by the photolysis of H2S. These then initiated reactions in mixtures involving acetylene-ammonia-water and ethylene-ammonia-water. In the case of the acetylene system, the products consisted of two amino acids, ethylene and a group of primarily cyclic thio-compounds, but no free sulfur. In the case of the ethylene systems, seven amino acids, including an aromatic one, ethane, free sulfur, and a group of solely linear thio-compounds were produced. Total quantum yields for the production of amino acids were about 3 x 10 to the -5th and about 2 x 10 to the -4th with ethylene and acetylene respectively as carbon substrates. Consideration is given of the mechanism for the formation of some of the products and implications regarding planetary atmosphere chemistry, particularly that of Jupiter, are explored.

  20. Graphene oxide/metal nanocrystal multilaminates as the atomic limit for safe and selective hydrogen storage

    DOE PAGES

    Cho, Eun Seon; Ruminski, Anne M.; Aloni, Shaul; Liu, Yi-Sheng; Guo, Jinghua; Urban, Jeffrey J.

    2016-02-23

    Interest in hydrogen fuel is growing for automotive applications; however, safe, dense, solid-state hydrogen storage remains a formidable scientific challenge. Metal hydrides offer ample storage capacity and do not require cryogens or exceedingly high pressures for operation. However, hydrides have largely been abandoned because of oxidative instability and sluggish kinetics. We report a new, environmentally stable hydrogen storage material constructed of Mg nanocrystals encapsulated by atomically thin and gas-selective reduced graphene oxide (rGO) sheets. This material, protected from oxygen and moisture by the rGO layers, exhibits exceptionally dense hydrogen storage (6.5 wt% and 0.105 kg H2 per litre in themore » total composite). As rGO is atomically thin, this approach minimizes inactive mass in the composite, while also providing a kinetic enhancement to hydrogen sorption performance. In conclusion, these multilaminates of rGO-Mg are able to deliver exceptionally dense hydrogen storage and provide a material platform for harnessing the attributes of sensitive nanomaterials in demanding environments.« less

  1. Graphene oxide/metal nanocrystal multilaminates as the atomic limit for safe and selective hydrogen storage

    PubMed Central

    Cho, Eun Seon; Ruminski, Anne M.; Aloni, Shaul; Liu, Yi-Sheng; Guo, Jinghua; Urban, Jeffrey J.

    2016-01-01

    Interest in hydrogen fuel is growing for automotive applications; however, safe, dense, solid-state hydrogen storage remains a formidable scientific challenge. Metal hydrides offer ample storage capacity and do not require cryogens or exceedingly high pressures for operation. However, hydrides have largely been abandoned because of oxidative instability and sluggish kinetics. We report a new, environmentally stable hydrogen storage material constructed of Mg nanocrystals encapsulated by atomically thin and gas-selective reduced graphene oxide (rGO) sheets. This material, protected from oxygen and moisture by the rGO layers, exhibits exceptionally dense hydrogen storage (6.5 wt% and 0.105 kg H2 per litre in the total composite). As rGO is atomically thin, this approach minimizes inactive mass in the composite, while also providing a kinetic enhancement to hydrogen sorption performance. These multilaminates of rGO-Mg are able to deliver exceptionally dense hydrogen storage and provide a material platform for harnessing the attributes of sensitive nanomaterials in demanding environments. PMID:26902901

  2. Electrochemical removal of hydrogen atoms in Mg-doped GaN epitaxial layers

    SciTech Connect

    Lee, June Key E-mail: hskim7@jbnu.ac.kr; Hyeon, Gil Yong; Tawfik, Wael Z.; Choi, Hee Seok; Ryu, Sang-Wan; Jeong, Tak; Jung, Eunjin; Kim, Hyunsoo E-mail: hskim7@jbnu.ac.kr

    2015-05-14

    Hydrogen atoms inside of an Mg-doped GaN epitaxial layer were effectively removed by the electrochemical potentiostatic activation (EPA) method. The role of hydrogen was investigated in terms of the device performance of light-emitting diodes (LEDs). The effect of the main process parameters for EPA such as solution type, voltage, and time was studied and optimized for application to LED fabrication. In optimized conditions, the light output of 385-nm LEDs was improved by about 26% at 30 mA, which was caused by the reduction of the hydrogen concentration by ∼35%. Further removal of hydrogen seems to be involved in the breaking of Ga-H bonds that passivate the nitrogen vacancies. An EPA process with high voltage breaks not only Mg-H bonds that generate hole carriers but also Ga-H bonds that generate electron carriers, thus causing compensation that impedes the practical increase of hole concentration, regardless of the drastic removal of hydrogen atoms. A decrease in hydrogen concentration affects the current-voltage characteristics, reducing the reverse current by about one order and altering the forward current behavior in the low voltage region.

  3. Graphene oxide/metal nanocrystal multilaminates as the atomic limit for safe and selective hydrogen storage.

    PubMed

    Cho, Eun Seon; Ruminski, Anne M; Aloni, Shaul; Liu, Yi-Sheng; Guo, Jinghua; Urban, Jeffrey J

    2016-02-23

    Interest in hydrogen fuel is growing for automotive applications; however, safe, dense, solid-state hydrogen storage remains a formidable scientific challenge. Metal hydrides offer ample storage capacity and do not require cryogens or exceedingly high pressures for operation. However, hydrides have largely been abandoned because of oxidative instability and sluggish kinetics. We report a new, environmentally stable hydrogen storage material constructed of Mg nanocrystals encapsulated by atomically thin and gas-selective reduced graphene oxide (rGO) sheets. This material, protected from oxygen and moisture by the rGO layers, exhibits exceptionally dense hydrogen storage (6.5 wt% and 0.105 kg H2 per litre in the total composite). As rGO is atomically thin, this approach minimizes inactive mass in the composite, while also providing a kinetic enhancement to hydrogen sorption performance. These multilaminates of rGO-Mg are able to deliver exceptionally dense hydrogen storage and provide a material platform for harnessing the attributes of sensitive nanomaterials in demanding environments.

  4. Femtosecond real-time probing of reactions. IX. Hydrogen-atom transfer

    NASA Astrophysics Data System (ADS)

    Herek, J. L.; Pedersen, S.; Bañares, L.; Zewail, A. H.

    1992-12-01

    The real-time dynamics of hydrogen-atom-transfer processes under collisionless conditions are studied using femtosecond depletion techniques. The experiments focus on the methyl salicylate system, which exhibits ultrafast hydrogen motion between two oxygen atoms due to molecular tautomerization, loosely referred to as intramolecular ``proton'' transfer. To test for tunneling and mass effects on the excited potential surface, we also studied deuterium and methyl-group substitutions. We observe that the motion of the hydrogen, under collisionless conditions, takes place within 60 fs. At longer times, on the picosecond time scale, the hydrogen-transferred form decays with a threshold of 15.5 kJ/mol; this decay behavior was observed up to a total vibrational energy of ˜7200 cm-1. The observed dynamics provide the global nature of the motion, which takes into account bonding before and after the motion, and the evolution of the wave packet from the initial nonequilibrium state to the transferred form along the O-H—O reaction coordinate. The vibrational periods (2π/ω) of the relevant modes range from 13 fs (the OH stretch) to 190 fs (the low-frequency distortion) and the motion involves (in part) these coordinates. The intramolecular vibrational-energy redistribution dynamics at longer times are important to the hydrogen-bond dissociation and to the nonradiative decay of the hydrogen-transferred form.

  5. Graphene oxide/metal nanocrystal multilaminates as the atomic limit for safe and selective hydrogen storage

    NASA Astrophysics Data System (ADS)

    Cho, Eun Seon; Ruminski, Anne M.; Aloni, Shaul; Liu, Yi-Sheng; Guo, Jinghua; Urban, Jeffrey J.

    2016-02-01

    Interest in hydrogen fuel is growing for automotive applications; however, safe, dense, solid-state hydrogen storage remains a formidable scientific challenge. Metal hydrides offer ample storage capacity and do not require cryogens or exceedingly high pressures for operation. However, hydrides have largely been abandoned because of oxidative instability and sluggish kinetics. We report a new, environmentally stable hydrogen storage material constructed of Mg nanocrystals encapsulated by atomically thin and gas-selective reduced graphene oxide (rGO) sheets. This material, protected from oxygen and moisture by the rGO layers, exhibits exceptionally dense hydrogen storage (6.5 wt% and 0.105 kg H2 per litre in the total composite). As rGO is atomically thin, this approach minimizes inactive mass in the composite, while also providing a kinetic enhancement to hydrogen sorption performance. These multilaminates of rGO-Mg are able to deliver exceptionally dense hydrogen storage and provide a material platform for harnessing the attributes of sensitive nanomaterials in demanding environments.

  6. Stabilizing a Platinum1 Single-Atom Catalyst on Supported Phosphomolybdic Acid without Compromising Hydrogenation Activity.

    PubMed

    Zhang, Bin; Asakura, Hiroyuki; Zhang, Jia; Zhang, Jiaguang; De, Sudipta; Yan, Ning

    2016-07-11

    In coordination chemistry, catalytically active metal complexes in a zero- or low-valent state often adopt four-coordinate square-planar or tetrahedral geometry. By applying this principle, we have developed a stable Pt1 single-atom catalyst with a high Pt loading (close to 1 wt %) on phosphomolybdic acid(PMA)-modified active carbon. This was achieved by anchoring Pt on the four-fold hollow sites on PMA. Each Pt atom is stabilized by four oxygen atoms in a distorted square-planar geometry, with Pt slightly protruding from the oxygen planar surface. Pt is positively charged, absorbs hydrogen easily, and exhibits excellent performance in the hydrogenation of nitrobenzene and cyclohexanone. It is likely that the system described here can be extended to a number of stable SACs with superior catalytic activities.

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

    PubMed

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

    2015-08-19

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

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

    PubMed Central

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

    2015-01-01

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

  9. Dephenolization of stored olive-mill wastewater, using four different adsorbing matrices to attain a low-cost feedstock for hydrogen photo-production.

    PubMed

    Padovani, Giulia; Pintucci, Cristina; Carlozzi, Pietro

    2013-06-01

    This investigation deals with the conversion of olive-mill wastewater (OMW) into several feedstocks suitable for hydrogen photo-production. The goal was reached by means of two sequential steps: (i) a pre-treatment process of stored-OMW for the removal of polyphenols, which made it possible to obtain several effluents, and (ii) a photo-fermentative process for hydrogen production by means of Rhodopseudomonas palustris sp. Four different adsorbent matrices (Azolla, granular active carbon, resin, and zeolite) were used to dephenolize stored-OMW. The four liquid fractions attained by using the above process created the same number of effluents, and these were diluted with water and then used for hydrogen photo-production. The maximum hydrogen production rate (14.31 mL/L/h) was attained with the photo-fermenter containing 25% of the effluent, which came from the pre-treatment of stored-OMW using granular active carbon. Using the carbon effluent as feedstock, the greatest light conversion efficiency of 2.29% was achieved. PMID:23612177

  10. Benchmarking all-atom simulations using hydrogen exchange

    PubMed Central

    Skinner, John J.; Yu, Wookyung; Gichana, Elizabeth K.; Baxa, Michael C.; Hinshaw, James R.; Freed, Karl F.; Sosnick, Tobin R.

    2014-01-01

    Long-time molecular dynamics (MD) simulations are now able to fold small proteins reversibly to their native structures [Lindorff-Larsen K, Piana S, Dror RO, Shaw DE (2011) Science 334(6055):517–520]. These results indicate that modern force fields can reproduce the energy surface near the native structure. To test how well the force fields recapitulate the other regions of the energy surface, MD trajectories for a variant of protein G are compared with data from site-resolved hydrogen exchange (HX) and other biophysical measurements. Because HX monitors the breaking of individual H-bonds, this experimental technique identifies the stability and H-bond content of excited states, thus enabling quantitative comparison with the simulations. Contrary to experimental findings of a cooperative, all-or-none unfolding process, the simulated denatured state ensemble, on average, is highly collapsed with some transient or persistent native 2° structure. The MD trajectories of this protein G variant and other small proteins exhibit excessive intramolecular H-bonding even for the most expanded conformations, suggesting that the force fields require improvements in describing H-bonding and backbone hydration. Moreover, these comparisons provide a general protocol for validating the ability of simulations to accurately capture rare structural fluctuations. PMID:25349413

  11. Semiclassical study of the quenching of excited-state fluorine atom by hydrogen molecule - Comparison between reactive and nonreactive processes

    NASA Technical Reports Server (NTRS)

    Yuan, J.-M.; Skuse, B. M.; Jaffe, R. L.; Komornicki, A.; Morokuma, K.; George, T. F.

    1980-01-01

    Semiclassical calculations are carried out for the quenching of excited-state fluorine atom by collinear collisions with hydrogen molecule. The overall quenching probability is the sum of two contributions: the reactive quenching probability associated with the formation of hydrogen fluoride and the nonreactive quenching probability leading to ground-state fluorine atom and hydrogen molecule. The reactive probability is greater in the threshold region of the collision energy, whereas the nonreactive probability dominates for energies above the threshold region.

  12. Solid Hydrogen Experiments for Atomic Propellants: Particle Formation Energy and Imaging Analyses

    NASA Technical Reports Server (NTRS)

    Palaszewski, Bryan

    2002-01-01

    This paper presents particle formation energy balances and detailed analyses of the images from experiments that were conducted on the formation of solid hydrogen particles in liquid helium during the Phase II testing in 2001. Solid particles of hydrogen were frozen in liquid helium and observed with a video camera. The solid hydrogen particle sizes and the total mass of hydrogen particles were estimated. The particle formation efficiency is also estimated. Particle sizes from the Phase I testing in 1999 and the Phase II testing in 2001 were similar. Though the 2001 testing created similar particles sizes, many new particle formation phenomena were observed. These experiment image analyses are one of the first steps toward visually characterizing these particles and it allows designers to understand what issues must be addressed in atomic propellant feed system designs for future aerospace vehicles.

  13. Solid Hydrogen Experiments for Atomic Propellants: Particle Formation, Imaging, Observations, and Analyses

    NASA Technical Reports Server (NTRS)

    Palaszewski, Bryan

    2005-01-01

    This report presents particle formation observations and detailed analyses of the images from experiments that were conducted on the formation of solid hydrogen particles in liquid helium. Hydrogen was frozen into particles in liquid helium, and observed with a video camera. The solid hydrogen particle sizes and the total mass of hydrogen particles were estimated. These newly analyzed data are from the test series held on February 28, 2001. Particle sizes from previous testing in 1999 and the testing in 2001 were similar. Though the 2001 testing created similar particles sizes, many new particle formation phenomena were observed: microparticles and delayed particle formation. These experiment image analyses are some of the first steps toward visually characterizing these particles, and they allow designers to understand what issues must be addressed in atomic propellant feed system designs for future aerospace vehicles.

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

    PubMed

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

    2015-08-12

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

  15. Single Pd atoms in activated carbon fibers and their contribution to hydrogen storage

    SciTech Connect

    Contescu, Cristian I; van Benthem, Klaus; Li, Sa; Bonifacio, Cecile S; Pennycook, Stephen J; Jena, Puru; Gallego, Nidia C

    2011-01-01

    Palladium-modified activated carbon fibers (Pd-ACF) were synthesized by meltspinning, carbonization and activation of an isotropic pitch carbon precursor premixed with an organometallic Pd compound. The hydrogen uptake at 25 oC and 20 bar on Pd- ACF exceeded the expected capacity based solely on Pd hydride formation and hydrogen physisorption on the microporous carbon support. Aberration-corrected scanning transmission electron microscopy (STEM) with sub- ngstrom spatial resolution provided unambiguous identification of isolated Pd atoms occurring in the carbon matrix that coexist with larger Pd particles. First principles calculations revealed that each single Pd atom can form Kubas-type complexes by binding up to three H2 molecules in the pressure range of adsorption measurements. Based on Pd atom concentration determined from STEM images, the contribution of various mechanisms to the excess hydrogen uptake measured experimentally was evaluated. With consideration of Kubas binding as a viable mechanism (along with hydride formation and physisorption to carbon support) the role of hydrogen spillover in this system may be smaller than previously thought.

  16. Atomic hydrogen adsorption and incipient hydrogenation of the Mg(0001) surface: a density-functional theory study.

    PubMed

    Li, Yanfang; Zhang, Ping; Sun, Bo; Yang, Yu; Wei, Yinghui

    2009-07-21

    We investigate the atomic hydrogen adsorption on Mg(0001) by using density-functional theory within the generalized gradient approximation and a supercell approach. The coverage dependence of the adsorption structures and energetics is systematically studied for a wide range of coverage Theta [from 0.11 to 2.0 monolayers (ML)] and adsorption sites. In the coverage range 0 < Theta < 1.0, the most stable among all possible adsorption sites is the on-surface fcc site followed by the hcp site, and the binding energy increases with the coverage, thus indicating the higher stability of on-surface adsorption and a tendency to the formation of H islands (clusters) when increasing the coverage within the region 0 < Theta < 1.0. The on-surface diffusion path energetics of atomic hydrogen as well as the activation barriers for hydrogen penetration from the on-surface to the subsurface sites are also presented at low coverage. At high coverage of 1.0 < Theta < or = 2.0, it is found that the coadsorption configuration with 1.0 monolayer of H residing on the surface fcc sites and the remaining (Theta-1.0) monolayer of H occupying the subsurface tetra-I sites is most energetically favorable. The resultant H-Mg-H sandwich structure for this most stable coadsorption configuration displays similar spectral features to the bulk hydride MgH(2) in the density of states. The other properties of the H/Mg(0001) system including the charge distribution, the lattice relaxation, the work function, and the electronic density of states are also studied and discussed in detail. It is pointed out that the H-Mg chemical bonding during surface hydrogenation displays a mixed ionic/covalent character.

  17. Hydrogenated graphene and hydrogenated silicene: computational insights.

    PubMed

    Nguyen, Manh-Thuong; Phong, Pham Nam; Tuyen, Nguyen Duc

    2015-06-01

    Density functional calculations are performed to study the energetic, structural, and electronic properties of graphene and silicene functionalized with hydrogen. Our calculations predict that H atoms bind much more strongly to silicene than to graphene. The adsorbed H atoms tend to cooperatively stabilize each other leading to a two-dimensional nucleation and growth mechanism. The different structural and electronic modifications induced by H in fully functionalized graphene and silicene (known as graphane and silicane) are also explained. Finally, the electronic properties of defective graphane with multiple hydrogen vacancies are investigated. Engineering the vacancies in graphane offers a way to modify the electronic properties of this material.

  18. Analytical transition-matrix treatment of electric multipole polarizabilities of hydrogen-like atoms

    SciTech Connect

    Kharchenko, V.F.

    2015-04-15

    The direct transition-matrix approach to the description of the electric polarization of the quantum bound system of particles is used to determine the electric multipole polarizabilities of the hydrogen-like atoms. It is shown that in the case of the bound system formed by the Coulomb interaction the corresponding inhomogeneous integral equation determining an off-shell scattering function, which consistently describes virtual multiple scattering, can be solved exactly analytically for all electric multipole polarizabilities. Our method allows to reproduce the known Dalgarno–Lewis formula for electric multipole polarizabilities of the hydrogen atom in the ground state and can also be applied to determine the polarizability of the atom in excited bound states. - Highlights: • A new description for electric polarization of hydrogen-like atoms. • Expression for multipole polarizabilities in terms of off-shell scattering functions. • Derivation of integral equation determining the off-shell scattering function. • Rigorous analytic solving the integral equations both for ground and excited states. • Study of contributions of virtual multiple scattering to electric polarizabilities.

  19. Nanochemistry at the atomic scale revealed in hydrogen-induced semiconductor surface metallization

    NASA Astrophysics Data System (ADS)

    Derycke, Vincent; Soukiassian, Patrick G.; Amy, Fabrice; Chabal, Yves J.; D'Angelo, Marie D.; Enriquez, Hanna B.; Silly, Mathieu G.

    2003-04-01

    Passivation of semiconductor surfaces against chemical attack can be achieved by terminating the surface-dangling bonds with a monovalent atom such as hydrogen. Such passivation invariably leads to the removal of all surface states in the bandgap, and thus to the termination of non-metallic surfaces. Here we report the first observation of semiconductor surface metallization induced by atomic hydrogen. This result, established by using photo-electron and photo-absorption spectroscopies and scanning tunnelling techniques, is achieved on a Si-terminated cubic silicon carbide (SiC) surface. It results from competition between hydrogen termination of surface-dangling bonds and hydrogen-generated steric hindrance below the surface. Understanding the ingredient for hydrogen-stabilized metallization directly impacts the ability to eliminate electronic defects at semiconductor interfaces critical for microelectronics, provides a means to develop electrical contacts on high-bandgap chemically passive materials, particularly for interfacing with biological systems, and gives control of surfaces for lubrication, for example of nanomechanical devices.

  20. Nanochemistry at the atomic scale revealed in hydrogen-induced semiconductor surface metallization.

    PubMed

    Derycke, Vincent; Soukiassian, Patrick G; Amy, Fabrice; Chabal, Yves J; D'angelo, Marie D; Enriquez, Hanna B; Silly, Mathieu G

    2003-04-01

    Passivation of semiconductor surfaces against chemical attack can be achieved by terminating the surface-dangling bonds with a monovalent atom such as hydrogen. Such passivation invariably leads to the removal of all surface states in the bandgap, and thus to the termination of non-metallic surfaces. Here we report the first observation of semiconductor surface metallization induced by atomic hydrogen. This result, established by using photo-electron and photo-absorption spectroscopies and scanning tunnelling techniques, is achieved on a Si-terminated cubic silicon carbide (SiC) surface. It results from competition between hydrogen termination of surface-dangling bonds and hydrogen-generated steric hindrance below the surface. Understanding the ingredient for hydrogen-stabilized metallization directly impacts the ability to eliminate electronic defects at semiconductor interfaces critical for microelectronics, provides a means to develop electrical contacts on high-bandgap chemically passive materials, particularly for interfacing with biological systems, and gives control of surfaces for lubrication, for example of nanomechanical devices.

  1. Rydberg hydrogen atom near a metallic surface: Stark regime and ionization dynamics

    SciTech Connect

    Inarrea, Manuel; Salas, J. Pablo; Lanchares, Victor; Pascual, Ana Isabel; Palacian, Jesus F.; Yanguas, Patricia

    2007-11-15

    We investigate the classical dynamics of a hydrogen atom near a metallic surface in the presence of a uniform electric field. To describe the atom-surface interaction we use a simple electrostatic image model. Owing to the axial symmetry of the system, the z-component of the canonical angular momentum P{sub {phi}} is an integral and the electronic dynamics is modeled by a two degrees of freedom Hamiltonian in cylindrical coordinates. The structure and evolution of the phase space as a function of the electric field strength is explored extensively by means of numerical techniques of continuation of families of periodic orbits and Poincare surfaces of section. We find that, due to the presence of the electric field, the atom is strongly polarized through two consecutive pitchfork bifurcations that strongly change the phase space structure. Finally, by means of the phase space transition state theory and the classical spectral theorem, the ionization dynamics of the atom is studied.

  2. Relativistic spectrum of hydrogen atom in the space-time non-commutativity

    SciTech Connect

    Moumni, Mustafa; BenSlama, Achour; Zaim, Slimane

    2012-06-27

    We study space-time non-commutativity applied to the hydrogen atom and its phenomenological effects. We find that it modifies the Coulomb potential in the Hamiltonian and add an r{sup -3} part. By calculating the energies from Dirac equation using perturbation theory, we study the modifications to the hydrogen spectrum. We find that it removes the degeneracy with respect to the total angular momentum quantum number and acts like a Lamb shift. Comparing the results with experimental values from spectroscopy, we get a new bound for the space-time non-commutative parameter.

  3. The contribution of dissociative processes to the production of atomic lines in hydrogen plasmas

    NASA Technical Reports Server (NTRS)

    Kunc, J. A.

    1985-01-01

    The contribution of molecular dissociative processes to the production of atomic lines is considered for a steady-state hydrogen plasma. If the contribution of dissociative processes is dominant, a substantial simplification in plasma diagnostics can be achieved. Numerical calculations have been performed for the production of Balmer alpha, beta, and gamma lines in hydrogen plasmas with medium and large degrees of ionization (x greater than about 0.0001) and for electron temperatures of 5000-45,000 K and electron densities of 10 to the 10th to 10 to the 16th/cu cm.

  4. Magnetic state selection in atomic frequency and time standards. [hydrogen masers

    NASA Technical Reports Server (NTRS)

    Peters, H. E.

    1982-01-01

    Atomic standards such as those based upon cesium and hydrogen rely upon magnetic state selection to obtain population inversion in the hyperfine transition levels. Use of new design approaches and improved magnetic materials has made it possible to fabricate improved state selectors of small size, and thus the efficiency of utilization of beam flux is greatly improved and the size and weight of the standard is reduced. The sensitivity to magnetic perturbations is also decreased, so that the accuracy and stability of the standard is improved. Several new state selector designs are illustrated and the application to standards utilizing different atomic species is analyzed.

  5. Nonadiabatic coupling in cold collisions of spin-polarized metastable hydrogen atoms

    SciTech Connect

    Forrey, Robert C.; Dalgarno, Alex; Vanne, Yulian V.; Saenz, Alejandro; Froelich, Piotr

    2007-11-15

    Previous calculations of low-temperature cross sections for collisions between spin-polarized metastable hydrogen atoms are improved to include nonadiabatic radial and angular coupling at large interatomic separations. The electrostatic dipole-quadrupole interaction produces nonadiabatic radial coupling between (2s,2p) and (2p,2p) states, while the Coriolis interaction produces nonadiabatic angular coupling. Both of these long-range contributions are handled in a space-fixed atomic gauge that is particularly convenient for a spin-polarized system. The improved theoretical results are compared with an existing experiment.

  6. Measurement of the absolute cross section for multiphoton ionization of atomic hydrogen at 248 nm

    SciTech Connect

    Kyrala, G.A.; Nichols, T.D.

    1990-01-01

    We present measurements of the absolute rates for multiphoton ionization of the ground state from atomic hydrogen by a linearly polarized, subpicosecond KrF laser pulse at a wavelength of 248 nm. A laser crossed atomic beam technique is used. The irradiance was varied from 3{times}10{sup 12} w/cm{sup 2} to 2{times}10{sup 14} w/cm{sup 2} and three above threshold ionization peaks were observed. The measured rate for total electron production is less than predicted by the numerical and perturbation calculations, but significantly higher than calculated by the Reiss and Keldysh methods. 21 refs., 7 figs.

  7. CHEMI-IONIZATION IN SOLAR PHOTOSPHERE: INFLUENCE ON THE HYDROGEN ATOM EXCITED STATES POPULATION

    SciTech Connect

    Mihajlov, Anatolij A.; Ignjatovic, Ljubinko M.; Sreckovic, Vladimir A.; Dimitrijevic, Milan S. E-mail: mihajlov@ipb.ac.rs

    2011-03-15

    In this paper, the influence of chemi-ionization processes in H*(n {>=} 2) + H(1s) collisions, as well as the influence of inverse chemi-recombination processes on hydrogen atom excited-state populations in solar photosphere, are compared with the influence of concurrent electron-atom and electron-ion ionization and recombination processes. It has been found that the considered chemi-ionization/recombination processes dominate over the relevant concurrent processes in almost the whole solar photosphere. Thus, it is shown that these processes and their importance for the non-local thermodynamic equilibrium modeling of the solar atmosphere should be investigated further.

  8. Calculation of harmonic generation during the multiphoton ionization of the hydrogen atom

    SciTech Connect

    DeVries, P.L. )

    1990-04-01

    The response of a hydrogen atom to an intense nonresonant laser field is investigated by direct numerical solution of the time-dependent Schroedinger equation. This calculation is nonperturbative and does not involve the eigenstates of the field-free atom. An ionization rate for three-photon ionization is calculated and found to be in excellent agreement with previous values. The time-dependent electric dipole moment is calculated; its Fourier transform yields the spectrum of scattered light. Odd-order harmonic peaks through at least the 25th order are present in the spectrum.

  9. Hydrogen atom abstraction from aldehydes - OH + H2CO and O + H2CO

    NASA Technical Reports Server (NTRS)

    Dupuis, M.; Lester, W. A., Jr.

    1984-01-01

    The essential features of the potential energy surfaces governing hydrogen abstraction from formaldehyde by oxygen atom and hydroxyl radical have been characterized with ab inito multiconfiguration Hartree-Fock (MCHF) and configuration interaction (CI) wave functions. The results are consistent with a very small activation energy for the OH + H2CO reaction, and an activation energy of a few kcal/mol for the O + H2CO reaction. In the transition state structure of both systems, the attacking oxygen atom is nearly collinear with the attacked CH bond.

  10. Nonadiabatic couplings in low-energy collisions of hydrogen ground-state atoms

    SciTech Connect

    Wolniewicz, L.

    2003-10-01

    The effect of nonadiabatic couplings on low-energy s-wave scattering of two hydrogen atoms is investigated. Coupling matrix elements are computed in a wide range of internuclear distances. The resulting scattering equations are numerically unstable and therefore are integrated only approximately. Computations are performed for H, D, and T atoms. The phase shifts in the zero velocity limit are inversely proportional to the nuclear reduced mass {delta}{sub 0}{approx_equal}0.392/{mu}. This leads to infinite scattering lengths.

  11. A fuzzy-atom analysis of electron delocalization on hydrogen bonds.

    PubMed

    Guillaumes, L; Salvador, P; Simon, S

    2014-02-13

    The extent of electron delocalization is quantified for set of cyclic complexes exhibiting two or more hydrogen bonds (HBs). In particular, the delocalization index (DI) between the atoms directly involved in the HB, and the ING (a normalized n-center delocalization index) have been evaluated using several fuzzy-atom schemes, namely Becke, Becke-ρ, Hirshfeld, and Hirshfeld-Iterative. The results have been compared with the widely used Quantum Theory of Atoms in Molecules (QTAIM) atomic definition. The DI values are found to correlate very well with geometrical or topological descriptors widely used in the literature to characterize HB systems. Among all fuzzy-atom methods, the ones that can better accommodate the different partial ionic character of the bonds perform particularly well. The best performing fuzzy-atom scheme for both pairwise and n-center electron delocalization is found to be the Becke-ρ method, for which similar results to QTAIM model are obtained with a much reduced computational cost. These results open up a wide range of applications of such electron delocalization descriptors based on fuzzy-atoms for noncovalent interactions in more complex and larger systems.

  12. A fuzzy-atom analysis of electron delocalization on hydrogen bonds.

    PubMed

    Guillaumes, L; Salvador, P; Simon, S

    2014-02-13

    The extent of electron delocalization is quantified for set of cyclic complexes exhibiting two or more hydrogen bonds (HBs). In particular, the delocalization index (DI) between the atoms directly involved in the HB, and the ING (a normalized n-center delocalization index) have been evaluated using several fuzzy-atom schemes, namely Becke, Becke-ρ, Hirshfeld, and Hirshfeld-Iterative. The results have been compared with the widely used Quantum Theory of Atoms in Molecules (QTAIM) atomic definition. The DI values are found to correlate very well with geometrical or topological descriptors widely used in the literature to characterize HB systems. Among all fuzzy-atom methods, the ones that can better accommodate the different partial ionic character of the bonds perform particularly well. The best performing fuzzy-atom scheme for both pairwise and n-center electron delocalization is found to be the Becke-ρ method, for which similar results to QTAIM model are obtained with a much reduced computational cost. These results open up a wide range of applications of such electron delocalization descriptors based on fuzzy-atoms for noncovalent interactions in more complex and larger systems. PMID:24444143

  13. Interstitial modification of palladium nanoparticles with boron atoms as a green catalyst for selective hydrogenation.

    PubMed

    Chan, Chun Wong Aaron; Mahadi, Abdul Hanif; Li, Molly Meng-Jung; Corbos, Elena Cristina; Tang, Chiu; Jones, Glenn; Kuo, Winson Chun Hsin; Cookson, James; Brown, Christopher Michael; Bishop, Peter Trenton; Tsang, Shik Chi Edman

    2014-01-01

    Lindlar catalysts comprising of palladium/calcium carbonate modified with lead acetate and quinoline are widely employed industrially for the partial hydrogenation of alkynes. However, their use is restricted, particularly for food, cosmetic and drug manufacture, due to the extremely toxic nature of lead, and the risk of its leaching from catalyst surface. In addition, the catalysts also exhibit poor selectivities in a number of cases. Here we report that a non-surface modification of palladium gives rise to the formation of an ultra-selective nanocatalyst. Boron atoms are found to take residence in palladium interstitial lattice sites with good chemical and thermal stability. This is favoured due to a strong host-guest electronic interaction when supported palladium nanoparticles are treated with a borane tetrahydrofuran solution. The adsorptive properties of palladium are modified by the subsurface boron atoms and display ultra-selectivity in a number of challenging alkyne hydrogenation reactions, which outclass the performance of Lindlar catalysts. PMID:25523894

  14. Oxygen atom kinetics in silane-hydrogen-nitrous oxide mixtures behind reflected shock waves

    NASA Astrophysics Data System (ADS)

    Javoy, S.; Mével, R.; Dupré, G.

    2010-11-01

    Resonance Absorption Spectroscopy has been used to study the O-atom dynamics behind reflected shock waves in highly argon diluted silane-hydrogen-nitrous oxide mixtures in the temperature range 1606-2528 K and at total pressures from 234 to 584 kPa. The absorptions at 130.5 nm of N 2O, SiH 4 and Si have been taken into account to compare simulated and experimental absorption profiles. A detailed kinetic model has been also used to interpret the results and reaction pathway and sensitivity analyses have been performed to underline important elementary reactions. A comparison with the O-atom kinetic in silane-nitrous oxide and hydrogen-nitrous oxide mixtures is also proposed.

  15. K-series X-ray yield measurement of kaonic hydrogen atoms in a gaseous target

    NASA Astrophysics Data System (ADS)

    Bazzi, M.; Beer, G.; Bellotti, G.; Berucci, C.; Bragadireanu, A. M.; Bosnar, D.; Cargnelli, M.; Curceanu, C.; Butt, A. D.; d'Uffizi, A.; Fiorini, C.; Ghio, F.; Guaraldo, C.; Hayano, R. S.; Iliescu, M.; Ishiwatari, T.; Iwasaki, M.; Levi Sandri, P.; Marton, J.; Okada, S.; Pietreanu, D.; Piscicchia, K.; Romero Vidal, A.; Sbardella, E.; Scordo, A.; Shi, H.; Sirghi, D. L.; Sirghi, F.; Tatsuno, H.; Vazquez Doce, O.; Widmann, E.; Zmeskal, J.

    2016-10-01

    We measured the K-series X-rays of the K- p exotic atom in the SIDDHARTA experiment with a gaseous hydrogen target of 1.3 g /l, which is about 15 times the ρSTP of hydrogen gas. At this density, the absolute yields of kaonic X-rays, when a negatively charged kaon stopped inside the target, were determined to be 0.012-0.003+0.004 for Kα and 0.043-0.011+0.012 for all the K-series transitions Ktot. These results, together with the KEK E228 experiment results, confirm for the first time a target density dependence of the yield predicted by the cascade models, and provide valuable information to refine the parameters used in the cascade models for the kaonic atoms.

  16. Catechols as Sources of Hydrogen Atoms in Radical Deiodination and Related Reactions.

    PubMed

    Povie, Guillaume; Ford, Leigh; Pozzi, Davide; Soulard, Valentin; Villa, Giorgio; Renaud, Philippe

    2016-09-01

    When used with trialkylboranes, catechol derivatives, which are low-cost and low toxicity, are valuable hydrogen atom donors for radical chain reactions involving alkyl iodides and related radical precursors. The system 4-tert-butylcatechol/triethylborane has been used to reduce a series of secondary and tertiary iodides, a xanthate, and a thiohydroxamate ester. Catechol derivatives are right in the optimal kinetic window for synthetic applications, as demonstrated by highly efficient radical cyclizations. Cyclizations leading to the formation of quaternary centers can be performed in an all-at-once process (no slow addition of the hydrogen atom donor) at standard concentrations. The H-donor properties of catechol derivatives can be fine-tuned by changing their substitution pattern. In slow radical cyclization processes, an enhanced ratio of cyclized/uncyclized products was obtained by using 3-methoxycatechol instead of 4-tert-butylcatechol.

  17. Interstitial modification of palladium nanoparticles with boron atoms as a green catalyst for selective hydrogenation

    NASA Astrophysics Data System (ADS)

    Chan, Chun Wong Aaron; Mahadi, Abdul Hanif; Li, Molly Meng-Jung; Corbos, Elena Cristina; Tang, Chiu; Jones, Glenn; Kuo, Winson Chun Hsin; Cookson, James; Brown, Christopher Michael; Bishop, Peter Trenton; Tsang, Shik Chi Edman

    2014-12-01

    Lindlar catalysts comprising of palladium/calcium carbonate modified with lead acetate and quinoline are widely employed industrially for the partial hydrogenation of alkynes. However, their use is restricted, particularly for food, cosmetic and drug manufacture, due to the extremely toxic nature of lead, and the risk of its leaching from catalyst surface. In addition, the catalysts also exhibit poor selectivities in a number of cases. Here we report that a non-surface modification of palladium gives rise to the formation of an ultra-selective nanocatalyst. Boron atoms are found to take residence in palladium interstitial lattice sites with good chemical and thermal stability. This is favoured due to a strong host-guest electronic interaction when supported palladium nanoparticles are treated with a borane tetrahydrofuran solution. The adsorptive properties of palladium are modified by the subsurface boron atoms and display ultra-selectivity in a number of challenging alkyne hydrogenation reactions, which outclass the performance of Lindlar catalysts.

  18. Proton scattering by a hydrogen atom in an effectively two-body model

    SciTech Connect

    Pupyshev, V. V.

    2013-02-15

    It is assumed that the total potential of proton interaction with a hydrogen atom is the sum of the short-range nuclear soft-core Reid potential and the long-range Thomas-Fermi potential. A quantum mechanical analysis of low-energy features of the phase shift and cross section for elastic proton scattering on a hydrogen atom is given for the case of zero total angular momentum. The calculations performed in the present study within a nonlinear version of the variable-phase approach ultimately revealed that, because of a long-range character of the asymptotic behavior of the Thomas-Fermi potential, the respective cross section at low energies oscillates but has a finite number of zeros.

  19. Spectrum of the hydrogen atom in Snyder space in a semiclassical approximation

    NASA Astrophysics Data System (ADS)

    Ivetić, B.; Mignemi, S.; Samsarov, A.

    2016-03-01

    We study the spectrum of the hydrogen atom in Snyder space in a semiclassical approximation based on a generalization of the Born-Sommerfeld quantization rule. While the corrections to the standard quantum mechanical spectrum arise at first order in the Snyder parameter for the l =0 states, they are of second order for l ≠0 . This can be understood as due to the different topology of the regions of integration in phase space.

  20. Hydrogen atom donor compounds as contrast enhancers for black-and-white photothermographic and thermographic elements

    DOEpatents

    Harring, Lori S.; Simpson, Sharon M.; Sansbury, Francis H.

    1997-01-01

    Hydrogen atom donor compounds are useful as contrast enhancers when used in combination with (i) hindered phenol developers, and (ii) trityl hydrazide and/or formyl-phenyl hydrazine co-developers, to produce ultra-high contrast black-and-white photothermographic and thermographic elements. The photothermographic and thermographic elements may be used as a photomask in a process where there is a subsequent exposure of an ultraviolet or short wavelength visible radiation-sensitive imageable medium.

  1. Lamb shift in the hydrogen atom: Lifetime of the 2p{1/2}level

    SciTech Connect

    Karshenboim, S.G.

    1995-05-01

    Corrections of order {alpha}(Z{alpha}){sup 2} to the width of the 2p{1/2} level in the hydrogen atom are considered in the logarithmic approximation. The ratio of this width to the splitting of n=2 states can be measured to high accuracy. With the aid of the experimental data available for this ratio, the new value for the Lamb splitting is found to be 1057.8576(21) MHz. 17 refs.

  2. Distortion effects in electron excitation of hydrogen atoms by impact of heavy ions

    SciTech Connect

    Ramirez, C.A.; Rivarola, R.D.

    1995-12-01

    Electron excitation from the fundamental state of hydrogen atoms by impact of bare ions is studied at intermediate and high collision velocities. Total cross sections for final {ital np} states by impact of protons, alpha particles, and He{sup +} ions are calculated using the symmetric eikonal approximation and compared with experimental data. This comparison supports the existence of distortion effects recently predicted by Bugacov and co-workers [Phys. Rev. A {bold 47}, 1052 (1993)]. The validity of scaling laws is analyzed.

  3. Absolute rate of the reaction of hydrogen atoms with ozone from 219-360 K

    NASA Technical Reports Server (NTRS)

    Lee, J. H.; Michael, J. V.; Payne, W. A.; Stief, L. J.

    1978-01-01

    Absolute rate constants for the reaction of atomic hydrogen with ozone were obtained over the temperature range 219-360 K by the flash photolysis-resonance fluorescence technique. The results can be expressed in Arrhenius form by K = (1.33 plus or minus 0.32)x10 to the minus 10 power exp (-449 plus or minus 58/T) cu cm/molecule/s (two standard deviations). The present work is compared to two previous determinations and is discussed theoretically.

  4. Lower bounds to energies for cusped-gaussian wavefunctions. [hydrogen atom ground state

    NASA Technical Reports Server (NTRS)

    Eaves, J. O.; Walsh, B. C.; Steiner, E.

    1974-01-01

    Calculations for the ground states of H, He, and Be, conducted by Steiner and Sykes (1972), show that the inclusion of a very small number of cusp functions can lead to a substantial enhancement of the quality of the Gaussian basis used in molecular wavefunction computations. The properties of the cusped-Gaussian basis are investigated by a calculation of lower bounds concerning the ground state energy of the hydrogen atom.

  5. Effects of disorder on the correlation energy of rings of hydrogen atoms

    NASA Astrophysics Data System (ADS)

    Liegener, C.-M.; Ladik, J.

    1985-01-01

    The correlation energy of disordered systems has been calculated by means of second-order Rayleigh-Schrödinger perturbation theory in the M∅ller-Plesset partitioning. Rings of hydrogen atoms have been chosen as model systems and the degree of disorder has been varied from complete delocalization to complete localization of the one-particle states. The correlation energy was found to have an extremum at an intermediate degree of disorder, corresponding to incomplete localization.

  6. Tables of branching ratios for electric dipole transitions between arbitrary levels of hydrogen-like atoms

    NASA Technical Reports Server (NTRS)

    Omidvar, K.

    1977-01-01

    The branching ratios in hydrogen-like atoms due to the electric-dipole transitions are tabulated for the initial principal and azimuthal quantum numbers n prime l prime, and final principal and azimuthal quantum numbers n l. Average values with respect to l prime are given. The branching ratios not tabulated, including the initial states n prime yields infinity l prime corresponding to the threshold of the continuum, could be obtained by extrapolation.

  7. Uranium Adsorbent Fibers Prepared by Atom-Transfer Radical Polymerization (ATRP) from Poly(vinyl chloride)- co -chlorinated Poly(vinyl chloride) (PVC- co -CPVC) Fiber

    DOE PAGES

    Brown, Suree; Yue, Yanfeng; Kuo, Li-Jung; Mehio, Nada; Li, Meijun; Gill, Gary; Tsouris, Costas; Mayes, Richard T.; Saito, Tomonori; Dai, Sheng

    2016-03-11

    The need to secure future supplies of energy attracts researchers in several countries to a vast resource of nuclear energy fuel: uranium in seawater (estimated at 4.5 billion tons in seawater). In this study, we developed effective adsorbent fibers for the recovery of uranium from seawater via atom-transfer radical polymerization (ATRP) from a poly-(vinyl chloride)-co-chlorinated poly(vinyl chloride) (PVC-co-CPVC) fiber. ATRP was employed in the surface graft polymerization of acrylonitrile (AN) and tert-butyl acrylate (tBA), precursors for uranium-interacting functional groups, from PVC-co-CPVC fiber. The [tBA]/[AN] was systematically varied to identify the optimal ratio between hydrophilic groups (from tBA) and uranyl-binding ligandsmore » (from AN). The best performing adsorbent fiber, the one with the optimal [tBA]/[AN] ratio and a high degree of grafting (1390%), demonstrated uranium adsorption capacities that are significantly greater than those of the Japan Atomic Energy Agency (JAEA) reference fiber in natural seawater tests (2.42 3.24 g/kg in 42 days of seawater exposure and 5.22 g/kg in 49 days of seawater exposure, versus 1.66 g/kg in 42 days of seawater exposure and 1.71 g/kg in 49 days of seawater exposure for JAEA). Lastly, adsorption of other metal ions from seawater and their corresponding kinetics were also studied. The grafting of alternative monomers for the recovery of uranium from seawater is now under development by this versatile technique of ATRP.« less

  8. THE INFRARED SPECTRA OF POLYCYCLIC AROMATIC HYDROCARBONS WITH SOME OR ALL HYDROGEN ATOMS REMOVED

    SciTech Connect

    Bauschlicher, Charles W. Jr.; Ricca, Alessandra E-mail: Alessandra.Ricca-1@nasa.gov

    2013-10-20

    The loss of one hydrogen from C{sub 96}H{sub 24} does not significantly affect the infrared spectra of the neutral, cation, or anion. Excluding a very weak C-C stretching band at 5.1 μm, the loss of two adjacent duo hydrogens does not significantly affect the spectra compared with the parent. Removing all of the hydrogen atoms significantly increases the intensity of the new C-C stretching band, and, for the cation, shifts it to a longer (5.2 μm) wavelength. Observations show a feature near 5.25 μm, which has been attributed to overtone and combination bands from polycyclic aromatic hydrocarbons (PAHs). This current work suggests that dehydrogenated PAHs might also contribute to this band, but its weakness implies that fully dehydrogenated cationic or dicationic species are very rare.

  9. Absolute rate calculations: atom and proton transfers in hydrogen-bonded systems.

    PubMed

    Barroso, Mónica; Arnaut, Luis G; Formosinho, Sebastião J

    2005-02-01

    We calculate energy barriers of atom- and proton-transfer reactions in hydrogen-bonded complexes in the gas phase. Our calculations do not involve adjustable parameters and are based on bond-dissociation energies, ionization potentials, electron affinities, bond lengths, and vibration frequencies of the reactive bonds. The calculated barriers are in agreement with experimental data and high-level ab initio calculations. We relate the height of the barrier with the molecular properties of the reactants and complexes. The structure of complexes with strong hydrogen bonds approaches that of the transition state, and substantially reduces the barrier height. We calculate the hydrogen-abstraction rates in H-bonded systems using the transition-state theory with the semiclassical correction for tunneling, and show that they are in excellent agreement with the experimental data. H-bonding leads to an increase in tunneling corrections at room temperature. PMID:15751360

  10. Europa - Ultraviolet emissions and the possibility of atomic oxygen and hydrogen clouds

    NASA Technical Reports Server (NTRS)

    Wu, F.-M.; Judge, D. L.; Carlson, R. W.

    1978-01-01

    Emission signals from Europa with wavelength below 800 A were detected by the Pioneer 10 ultraviolet photometer. In the present paper, improved procedures for data reduction are used to determine the spatial region as well as the intensity of the suggested emission sources. The observations indicate a cloud with a radius of about 1.5 Jupiter radii and an apparent brightness of approximately 10 rayleighs for a wavelength of 500 A. It is argued that neutral oxygen atoms, along with neutral hydrogen, are produced through dissociation of water ice on the surface of Europa by particle impact. Electron impact ionization excitation of oxygen atoms in the resulting cloud then gives rise to the observed emission. The present source brightness and cloud radius results are used to estimate an oxygen column density of the order of 10 trillion per sq cm, while the density of atomic hydrogen is at most 100 billion per sq cm and 1 trillion per sq cm for molecular hydrogen.

  11. Polarized Atomic Hydrogen Beam Tests in the Michigan Ultra-Cold Jet Target

    NASA Astrophysics Data System (ADS)

    Kageya, T.; Blinov, B. B.; Denbow, J. M.; Kandes, M. C.; Krisch, A. D.; Kulkarni, D. A.; Lehman, M. A.; Luppov, V. G.; Morozov, V. S.; Murray, J. R.; Peters, C. C.; Raymond, R. S.; Ross, M. R.; Yonehara, K.; Borisov, N. S.; Fimushkin, V. V.; Kleppner, D.; Grishin, V. N.; Mysnik, A. L.

    2001-04-01

    To study spin effects in high energy collisions, we are developing an ultra-cold high-density jet target of proton-spin-polarized hydrogen atoms (Michigan Jet Target). The target uses a 12 Tesla magnetic field and a 0.3 K separation cell coated with superfluid helium-4 to produce a slow monochromatic electron-spin-polarized atomic hydrogen beam; an rf transition unit then converts this into a proton-spin-polarized beam, which is focused by a superconducting sextupole into the interaction region. The Jet produced, at the detector, a spin-polarized atomic hydrogen beam with a measured intensity of about 1.7 10^15 H s-1 and a FWHM area of less than 0.13 cm^2. This intensity corresponds to a free jet density of about 1.3 10^12 H cm-3 with a proton polarization of about 50%. When the transition RF unit is installed, we expect a proton polarization higher than 90%.

  12. Polarized Atomic Hydrogen Beam Tests in the Mark-II Ultra-Cold Jet Target.

    NASA Astrophysics Data System (ADS)

    Luppov, V. G.; Blinov, B. B.; Gladycheva, S. E.; Kageya, T.; Kantsyrev, D. Yu.; Krisch, A. D.; Murray, J. R.; Neumann, J. J.; Raymond, R. S.; Borisov, N. S.; Kleppner, D.; Davidenko, A. M.; Grishin, V. N.

    2000-04-01

    To study spin effects in high energy collisions, we are developing an ultra-cold high-density jet target of proton-spin-polarized hydrogen atoms (Mark-II). The target uses a 12 Tesla magnetic field and a 0.3 K separation cell coated with superfluid helium-4 to produce a slow monochromatic electron-spin-polarized atomic hydrogen beam; an rf transition unit then converts this into a proton-spin-polarized beam, which is focused by a superconducting sextupole into the interaction region. Recently, the Jet produced a measured electron-spin-polarized atomic hydrogen beam of about 10^15 H s-1 into a 0.3 cm^2 area at the detector. This intensity corresponds to the free jet density of about 10^11 H cm-3 with a proton polarization of about 50%. So far, the intensity is limited by the high insulation vacuum pressure due to the evaporation of the separation cell's helium film. The beam's angular and radial distributions were measured. A test of a new superfluid-^4He-coated parabolic mirror, attached to the separation cell, appeared to increase the beam intensity by a factor of about 3, as expected.

  13. Confinement effects of magnetic field on two-dimensional hydrogen atom in plasmas

    SciTech Connect

    Bahar, M. K.; Soylu, A.

    2015-05-15

    In this study, for the first time, the Schrödinger equation with more general exponential cosine screened Coulomb (MGECSC) potential is solved numerically in the presence and in the absence of an external magnetic field within two-dimensional formalism using the asymptotic iteration method. The MGECSC potential includes four different potential forms when considering different sets of the parameters in the potential. The plasma screening effects in the weak and strong magnetic field regimes as well as the confinement effects of magnetic field on the two-dimensional hydrogen atom in Debye and quantum plasmas are investigated by solving the corresponding equations. It is found that applying a uniform magnetic field on the hydrogen atom embedded in a plasma leads to change in the profile of the total interaction potential. Thus, confinement effects of magnetic field on hydrogen atom embedded in Debye and quantum plasmas modeled by a MGECSC potential lead to shift bound state energies. This effect would be important to isolate the plasma from the external environment in the experimental applications of plasma physics.

  14. Transport of atomic hydrogen through graphite and its reaction with azoaromatic compounds.

    PubMed

    Ye, Jianchang; Chiu, Pei C

    2006-06-15

    Graphite is a major non-iron component in commercial iron granules that are typically used for groundwater remediation. Recent studies suggest graphite inclusions in commercial iron may serve as both adsorption and reaction sites for nitrogenous pollutants such as nitroaromatics, nitrate esters, and heterocyclic nitramines. In this study, we investigated graphite-mediated reduction of azoaromatic compounds with elemental iron in dialysis cells, where azo compounds and iron were physically separated by graphite foil. Both the nonpolar azobenzene and the water-soluble orange G were reduced to aniline, suggesting that exposed graphite in granular iron may mediate reduction of both polar and nonpolar compounds. Orange G reduction was zero-order and commenced after a long initial lag. Both the lag time and the zero-order rate constant varied with graphite thickness, consistent with the explanation that orange G reduction was limited by atomic hydrogen, which was formed via anaerobic iron corrosion and spilled over to graphite. Involvement of atomic hydrogen was confirmed by detection of deuterated aniline when iron was placed in a D2O-based buffer. Our results indicate that atomic hydrogen is mobile in graphite at room temperature, is reactive toward azoaromatic compounds, and may be consumed during transport in graphite.

  15. RAPID COMMUNICATION: High silicon etch rates by hot filament generated atomic hydrogen

    NASA Astrophysics Data System (ADS)

    Wanka, H. N.; Schubert, M. B.

    1997-04-01

    The etching of hydrogenated amorphous silicon (a-Si:H) and microcrystalline silicon by hot tungsten filament generated atomic hydrogen has been investigated. Room-temperature etch rates of 27 Å 0022-3727/30/8/002/img1 for amorphous and 20 Å 0022-3727/30/8/002/img1 for microcrystalline silicon have been achieved. Boron doping decreases the etch rate, whereas phosphorus doping does not affect it. No surface roughening occurs, even for the highest a-Si:H etch rates. In the initial phase of the etch process, however, a bond structure modification arises close to the surface. An increase of microcrystalline silicon etch rates towards the substrate/film interface reflects the coalescence of the microcrystalline nuclei. Hot filament atomic hydrogen etching provides high etch rates of amorphous and polycrystalline silicon with a high selectivity against metals and thermal oxide. Due to its simple setup and control, this kind of hydrogen etching is very interesting for applications in semiconductor technology where F- or Cl-etchants are to be avoided.

  16. Isotope Dependence and Quantum Effects on Atomic Hydrogen Diffusion in Liquid Water.

    PubMed

    Walker, J A; Mezyk, S P; Roduner, E; Bartels, D M

    2016-03-01

    Relative diffusion coefficients were determined in water for the D, H, and Mu isotopes of atomic hydrogen by measuring their diffusion-limited spin-exchange rate constants with Ni(2+) as a function of temperature. H and D atoms were generated by pulse radiolysis of water and measured by time-resolved pulsed EPR. Mu atoms are detected by muonium spin resonance. To isolate the atomic mass effect from solvent isotope effect, we measured all three spin-exchange rates in 90% D2O. The diffusion depends on the atomic mass, demonstrating breakdown of Stokes-Einstein behavior. The diffusion can be understood using a combination of water "cavity diffusion" and "hopping" mechanisms, as has been proposed in the literature. The H/D isotope effect agrees with previous modeling using ring polymer molecular dynamics. The "quantum swelling" effect on muonium due to its larger de Broglie wavelength does not seem to slow its "hopping" diffusion as much as predicted in previous work. Quantum effects of both the atom mass and the water librations have been modeled using RPMD and a qTIP4P/f quantized flexible water model. These results suggest that the muonium diffusion is very sensitive to the Mu versus water potential used.

  17. Nonperturbative treatments of nonresonant multiphoton ionization of the hydrogen atom: weak field limit

    SciTech Connect

    Trombetta, F.; Basile, S.; Ferrante, G.

    1989-04-01

    A nonperturbative treatment of the multiphoton ionization of the hydrogen atom based on the S matrix and devised for nonresonant strong-field situations is analyzed in the weak-field limit. Comparisons are presented with other S matrices as well as other nonperturbative approaches. Our treatment is found to perform generally better than similar S-matrix treatments. The usual perturbative results are recovered provided that the photon wavelengths are sufficiently short and are off resonance with the atomic transitions. Important indications are obtained as to the role of the atomic structure, the relevance of the gauge consistency, and the reliability and improvement of the present nonperturbative treatment. The results represent a significant step toward an assessment of the S-matrix-based treatments of multiphoton ionization.

  18. Excited-state hydrogen-atom transfer along solvent wires: water molecules stop the transfer.

    PubMed

    Tanner, Christian; Thut, Markus; Steinlin, Andreas; Manca, Carine; Leutwyler, Samuel

    2006-02-01

    Excited-state hydrogen-atom transfer (ESHAT) along a hydrogen-bonded solvent wire occurs for the supersonically cooled n = 3 ammonia-wire cluster attached to the scaffold molecule 7-hydroxyquinoline (7HQ) [Tanner, C.; et al. Science 2003, 302, 1736]. Here, we study the analogous three-membered solvent-wire clusters 7HQ.(NH3)n.(H2O)m, n + m = 3, using resonant two-photon ionization (R2PI) and UV-UV hole-burning spectroscopies. Substitution of H2O for NH3 has a dramatic effect on the excited-state H-atom transfer: The threshold for the ESHAT reaction is approximately 200 cm(-1) for 7HQ.(NH3)3, approximately 350 cm(-1) for both isomers of the 7HQ.(NH3)2.H2O cluster, and approximately 600 cm(-1) for 7HQ.NH3.(H2O)2 but increases to approximately 2000 cm(-1) for the pure 7HQ.(H2O)3 water-wire cluster. To understand the effect of the chemical composition of the solvent wire on the H-atom transfer, the reaction profiles of the low-lying electronic excited states of the n = 3 pure and mixed solvent-wire clusters are calculated with the configuration interaction singles (CIS) method. For those solvent wires with an NH3 molecule at the first position, injection of the H atom into the wire can occur by tunneling. However, further H-atom transfer is blocked by a high barrier at the first (and second) H2O molecule along the solvent wire. H-atom transfer along the entire length of the solvent wire, leading to formation of the 7-ketoquinoline (7KQ) tautomer, cannot occur for any of the H2O-containing clusters, in agreement with experimentally observed absence of 7KQ fluorescence.

  19. Synthetic use of the primary kinetic isotope effect in hydrogen atom transfer: generation of α-aminoalkyl radicals.

    PubMed

    Wood, Mark E; Bissiriou, Sabine; Lowe, Christopher; Norrish, Andrew M; Sénéchal, Katell; Windeatt, Kim M; Coles, Simon J; Hursthouse, Michael B

    2010-10-21

    The extent to which deuterium can act as a protecting group to prevent unwanted 1,5-hydrogen atom transfer to aryl and vinyl radical intermediates was examined in the context of the generation of α-aminoalkyl radicals in a pyrrolidine ring. Intra- and intermolecular radical trapping following hydrogen atom transfer provides an illustration of the use of the primary kinetic isotope effect in directing the outcome of synthetic C-C bond-forming processes.

  20. Two-step adsorption on jungle-gym-type porous coordination polymers: dependence on hydrogen-bonding capability of adsorbates, ligand-substituent effect, and temperature.

    PubMed

    Uemura, Kazuhiro; Yamasaki, Yukari; Onishi, Fumiaki; Kita, Hidetoshi; Ebihara, Masahiro

    2010-11-01

    A preliminary study of isopropanol (IPA) adsorption/desorption isotherms on a jungle-gym-type porous coordination polymer, [Zn(2)(bdc)(2)(dabco)](n) (1, H(2)bdc = 1,4-benzenedicarboxylic acid, dabco =1,4-diazabicyclo[2.2.2]octane), showed unambiguous two-step profiles via a highly shrunk intermediate framework. The results of adsorption measurements on 1, using probing gas molecules of alcohol (MeOH and EtOH) for the size effect and Me(2)CO for the influence of hydrogen bonding, show that alcohol adsorption isotherms are gradual two-step profiles, whereas the Me(2)CO isotherm is a typical type-I isotherm, indicating that a two-step adsorption/desorption is involved with hydrogen bonds. To further clarify these characteristic adsorption/desorption behaviors, selecting nitroterephthalate (bdc-NO(2)), bromoterephthalate (bdc-Br), and 2,5-dichloroterephthalate (bdc-Cl(2)) as substituted dicarboxylate ligands, isomorphous jungle-gym-type porous coordination polymers, {[Zn(2)(bdc-NO(2))(2)(dabco)]·solvents}(n) (2 ⊃ solvents), {[Zn(2)(bdc-Br)(2)(dabco)]·solvents}(n) (3 ⊃ solvents), and {[Zn(2)(bdc-Cl(2))(2)(dabco)]·solvents}(n) (4 ⊃ solvents), were synthesized and characterized by single-crystal X-ray analyses. Thermal gravimetry, X-ray powder diffraction, and N(2) adsorption at 77 K measurements reveal that [Zn(2)(bdc-NO(2))(2)(dabco)](n) (2), [Zn(2)(bdc-Br)(2)(dabco)](n) (3), and [Zn(2)(bdc-Cl(2))(2)(dabco)](n) (4) maintain their frameworks without guest molecules with Brunauer-Emmett-Teller (BET) surface areas of 1568 (2), 1292 (3), and 1216 (4) m(2) g(-1). As found in results of MeOH, EtOH, IPA, and Me(2)CO adsorption/desorption on 2-4, only MeOH adsorption on 2 shows an obvious two-step profile. Considering the substituent effects and adsorbate sizes, the hydrogen bonds, which are triggers for two-step adsorption, are formed between adsorbates and carboxylate groups at the corners in the pores, inducing wide pores to become narrow pores. Interestingly, such

  1. FORMATION OF FORMALDEHYDE AND CARBON DIOXIDE ON AN ICY GRAIN ANALOG USING FAST HYDROGEN ATOMS

    SciTech Connect

    Madzunkov, S. M.; MacAskill, J. A.; Chutjian, A.; Darrach, M. R.; Vidali, G.; Shortt, B. J.

    2009-05-20

    Formaldehyde (H{sub 2}CO) and carbon dioxide (CO{sub 2}) were produced in collisions of a superthermal, 3 eV beam of H({sup 2}S) atoms with CO molecules adsorbed on a gold surface at 4.8 K. The reaction-generated products were detected and analyzed using the techniques of temperature programmed desorption (TPD), quadrupole mass spectrometry, and a novel application of the Metropolis algorithm, random-walk procedure to identify the unique fractionation patterns of H{sub 2}CO and CO{sub 2} from the patterns of other species such as N{sub 2}, CO, and H{sub 2}O embedded in the CO blanket and devolved in the TPD/mass spectrometry process. Reaction sequences are given to account for the formation of H{sub 2}CO and CO{sub 2}.

  2. Selective hydrogenation of 1,3-butadiene on platinum–copper alloys at the single-atom limit

    PubMed Central

    Lucci, Felicia R.; Liu, Jilei; Marcinkowski, Matthew D.; Yang, Ming; Allard, Lawrence F.; Flytzani-Stephanopoulos, Maria; Sykes, E. Charles H.

    2015-01-01

    Platinum is ubiquitous in the production sectors of chemicals and fuels; however, its scarcity in nature and high price will limit future proliferation of platinum-catalysed reactions. One promising approach to conserve platinum involves understanding the smallest number of platinum atoms needed to catalyse a reaction, then designing catalysts with the minimal platinum ensembles. Here we design and test a new generation of platinum–copper nanoparticle catalysts for the selective hydrogenation of 1,3-butadiene,, an industrially important reaction. Isolated platinum atom geometries enable hydrogen activation and spillover but are incapable of C–C bond scission that leads to loss of selectivity and catalyst deactivation. γ-Alumina-supported single-atom alloy nanoparticle catalysts with <1 platinum atom per 100 copper atoms are found to exhibit high activity and selectivity for butadiene hydrogenation to butenes under mild conditions, demonstrating transferability from the model study to the catalytic reaction under practical conditions. PMID:26449766

  3. Selective hydrogenation of 1,3-butadiene on platinum–copper alloys at the single-atom limit

    SciTech Connect

    Lucci, Felicia R.; Liu, Jilei; Marcinkowski, Matthew D.; Yang, Ming; Allard, Lawrence F.; Flytzani-Stephanopoulos, Maria; Sykes, E. Charles H.

    2015-10-09

    Platinum is ubiquitous in the production sectors of chemicals and fuels; however, its scarcity in nature and high price will limit future proliferation of platinum-catalysed reactions. One definite approach to conserve platinum involves understanding the smallest number of platinum atoms needed to catalyse a reaction, then designing catalysts with the minimal platinum ensembles. Here we design and test a new generation of platinum–copper nanoparticle catalysts for the selective hydrogenation of 1,3-butadiene,, an industrially important reaction. Isolated platinum atom geometries enable hydrogen activation and spillover but are incapable of C–C bond scission that leads to loss of selectivity and catalyst deactivation. γ-Alumina-supported single-atom alloy nanoparticle catalysts with <1 platinum atom per 100 copper atoms are found to exhibit high activity and selectivity for butadiene hydrogenation to butenes under mild conditions, demonstrating transferability from the model study to the catalytic reaction under practical conditions.

  4. Selective hydrogenation of 1,3-butadiene on platinum-copper alloys at the single-atom limit

    NASA Astrophysics Data System (ADS)

    Lucci, Felicia R.; Liu, Jilei; Marcinkowski, Matthew D.; Yang, Ming; Allard, Lawrence F.; Flytzani-Stephanopoulos, Maria; Sykes, E. Charles H.

    2015-10-01

    Platinum is ubiquitous in the production sectors of chemicals and fuels; however, its scarcity in nature and high price will limit future proliferation of platinum-catalysed reactions. One promising approach to conserve platinum involves understanding the smallest number of platinum atoms needed to catalyse a reaction, then designing catalysts with the minimal platinum ensembles. Here we design and test a new generation of platinum-copper nanoparticle catalysts for the selective hydrogenation of 1,3-butadiene,, an industrially important reaction. Isolated platinum atom geometries enable hydrogen activation and spillover but are incapable of C-C bond scission that leads to loss of selectivity and catalyst deactivation. γ-Alumina-supported single-atom alloy nanoparticle catalysts with <1 platinum atom per 100 copper atoms are found to exhibit high activity and selectivity for butadiene hydrogenation to butenes under mild conditions, demonstrating transferability from the model study to the catalytic reaction under practical conditions.

  5. Selective hydrogenation of 1,3-butadiene on platinum-copper alloys at the single-atom limit.

    PubMed

    Lucci, Felicia R; Liu, Jilei; Marcinkowski, Matthew D; Yang, Ming; Allard, Lawrence F; Flytzani-Stephanopoulos, Maria; Sykes, E Charles H

    2015-01-01

    Platinum is ubiquitous in the production sectors of chemicals and fuels; however, its scarcity in nature and high price will limit future proliferation of platinum-catalysed reactions. One promising approach to conserve platinum involves understanding the smallest number of platinum atoms needed to catalyse a reaction, then designing catalysts with the minimal platinum ensembles. Here we design and test a new generation of platinum-copper nanoparticle catalysts for the selective hydrogenation of 1,3-butadiene,, an industrially important reaction. Isolated platinum atom geometries enable hydrogen activation and spillover but are incapable of C-C bond scission that leads to loss of selectivity and catalyst deactivation. γ-Alumina-supported single-atom alloy nanoparticle catalysts with <1 platinum atom per 100 copper atoms are found to exhibit high activity and selectivity for butadiene hydrogenation to butenes under mild conditions, demonstrating transferability from the model study to the catalytic reaction under practical conditions. PMID:26449766

  6. Formation of metastable atomic hydrogen in the 2s state from symmetry-resolved doubly excited states of molecular hydrogen

    SciTech Connect

    Odagiri, Takeshi; Kumagai, Yoshiaki; Nakano, Motoyoshi; Tanabe, Takehiko; Kitajima, Masashi; Kouchi, Noriyuki; Suzuki, Isao H.

    2011-11-15

    The cross sections for the formation of the metastable atomic hydrogen in the 2s state in photoexcitation of H{sub 2} and D{sub 2} were measured as a function of the incident photon energy in the range of the doubly excited states with their symmetries of the electronic states, {sup 1}{Sigma}{sub u}{sup +} or {sup 1}{Pi}{sub u}, being resolved. It has turned out from the comparison with the cross-section curves for other dissociation processes and the theoretical calculation [J. D. Bozek et al., J. Phys. B 39, 4871 (2006)] that the Q{sub 2}{sup 1}{Pi}{sub u}(1) doubly excited state of H{sub 2} dissociates into both H(2s) + H(2p) and H(2p) + H(2p). The dissociation dynamics of this state has been discussed in terms of the nonadiabatic transition during neutral dissociations.

  7. A Guided-Inquiry Lab for the Analysis of the Balmer Series of the Hydrogen Atomic Spectrum

    ERIC Educational Resources Information Center

    Bopegedera, A. M. R. P.

    2011-01-01

    A guided-inquiry lab was developed to analyze the Balmer series of the hydrogen atomic spectrum. The emission spectrum of hydrogen was recorded with a homemade benchtop spectrophotometer. By drawing graphs and a trial-and-error approach, students discover the linear relationship presented in the Rydberg formula and connect it with the Bohr model…

  8. Unoccupied electronic states in adsorbate systems

    NASA Astrophysics Data System (ADS)

    Bertel, E.

    1991-11-01

    Experimental work on unoccupied electronic states in adsorbate systems on metallic substrates is reviewed with emphasis on recent developments. The first part is devoted to molecular adsorbates. Weakly chemisorbed hydrocarbons are briefly discussed. An exhaustive inverse photoemission (IPE) study of the CO bond to the transition metals Ni, Pb, and Pt is presented. Adsorbed NO is taken as an example to demonstrate the persisting discrepancies in the interpretation of IPE spectra. Atomic adsorbates are discussed in the second part. The quantum well state model is applied to interpret the surface states in reconstructing and non-reconstructing adsorption systems of alkali metals and hydrogen. A recent controversy on the unoccupied electronic states of the Cu(110)/O p(2×1) surface is critically reviewed. The quantum well state model is then compared to tight binding and local-density-functional calculations of the unoccupied bands and the deficiencies of the various approaches are pointed out. Finally, the relation between the surface state model and more chemically oriented models of surface bonding is briefly discussed.

  9. Stable isolated metal atoms as active sites for photocatalytic hydrogen evolution.

    PubMed

    Xing, Jun; Chen, Jian Fu; Li, Yu Hang; Yuan, Wen Tao; Zhou, Ying; Zheng, Li Rong; Wang, Hai Feng; Hu, P; Wang, Yun; Zhao, Hui Jun; Wang, Yong; Yang, Hua Gui

    2014-02-17

    The process of using solar energy to split water to produce hydrogen assisted by an inorganic semiconductor is crucial for solving our energy crisis and environmental problems in the future. However, most semiconductor photocatalysts would not exhibit excellent photocatalytic activity without loading suitable co-catalysts. Generally, the noble metals have been widely applied as co-catalysts, but always agglomerate during the loading process or photocatalytic reaction. Therefore, the utilization efficiency of the noble co-catalysts is still very low on a per metal atom basis if no obvious size effect exists, because heterogeneous catalytic reactions occur on the surface active atoms. Here, for the first time, we have synthesized isolated metal atoms (Pt, Pd, Rh, or Ru) stably by anchoring on TiO2 , a model photocatalystic system, by a facile one-step method. The isolated metal atom based photocatalysts show excellent stability for H2 evolution and can lead to a 6-13-fold increase in photocatalytic activity over the metal clusters loaded on TiO2 by the traditional method. Furthermore, the configurations of isolated atoms as well as the originality of their unusual stability were analyzed by a collaborative work from both experiments and theoretical calculations.

  10. Density functional study of manganese atom adsorption on hydrogen-terminated armchair boron nitride nanoribbons

    NASA Astrophysics Data System (ADS)

    Abdullahi, Yusuf Zuntu; Rahman, Md. Mahmudur; Shuaibu, Alhassan; Abubakar, Shamsu; Zainuddin, Hishamuddin; Muhida, Rifki; Setiyanto, Henry

    2014-08-01

    In this paper, we have investigated stable structural, electric and magnetic properties of manganese (Mn) atom adsorption on armchair hydrogen edge-terminated boron nitride nanoribbon (A-BNNRs) using first principles method based on density-functional theory with the generalized gradient approximation. Calculation shows that Mn atom situated on the ribbons of A-BNNRs is the most stable configuration, where the bonding is more pronounced. The projected density of states (PDOS) of the favored configuration has also been computed. It has been found that the covalent bonding of boron (B), nitrogen (N) and Mn is mainly contributed by s, d like-orbitals of Mn and partially occupied by the 2p like-orbital of N. The difference in energy between the inner and the edge adsorption sites of A-BNNRs shows that Mn atoms prefer to concentrate at the edge sites. The electronic structures of the various configurations are wide, narrow-gap semiconducting and half-metallic, and the magnetic moment of Mn atoms are well preserved in all considered configurations. This has shown that the boron nitride (BN) sheet covered with Mn atoms demonstrates additional information on its usefulness in future spintronics, molecular magnet and nanoelectronics devices.

  11. The Absolute Rates of the Solution Phase Addition of Atomic Hydrogen to a Vinyl Ether and a Vinyl Ester. The Effect of Oxygen Substitution on Hydrogen Atom Reactivity with Olefins

    SciTech Connect

    Tanner, D. D.; Kandanarachchi, P.; Das, N. C.; Franz, James A.

    2003-04-08

    The reactions of vinyl butyl ether and vinyl butyrate with atomic hydrogen and deuterium lead to addition of atomic hydrogen to the terminal position of the olefins. This observation is consistent with the reactions carried out earlier with other olefins. Both the absolute rates of addition to vinylbutyl ether and vinyl butyrate in acetone and hexane were carried out at several temperatures. The relative rates are consistent with only modest stabilization of the transition state of the radical adduct by the ??-o substituent compared with hydrogen atom addition to 1-octene. The relative rates measured in acetone and hexane indicate no significant differential solvation of ground state relative to the transition structures of the hydrogen atom addition. The kinetics reveal that the early transition states of hydrogen atom addition exhibit little selectivity (vinyl ether versus simple olefin) in either abstraction of hydrogen ??- to the oxygen or by terminal addition to the olefinic ether, reflecting the modest influence of the increased enthalpy of reaction associated with resonance stabilization by the oxygen substituent at the developing radical site.

  12. Exposure of GaAs to atomic hydrogen for cleaning prior to NEA photocathode activation

    SciTech Connect

    Sinclair, C.K.; Poelker, B.M.; Price, J.S.

    1998-12-31

    Creating an atomically clean semiconductor surface is an essential step in preparing negative electron affinity (NEA) photoemission cathodes. While bulk GaAs can be satisfactorily cleaned by chemical etching and in situ heat cleaning, many high polarization electron source materials are either much too thin, or have oxides and carbides which are too tightly bound, to be cleaned by these methods. Some polarized source candidate materials may be degraded during the heat cleaning step. It is well established that the exposure of many III-V, II-VI, and elemental semiconductors to atomic hydrogen, typically at elevated temperatures, produces semiconductor surfaces free of contamination. Furthermore, this cleaning, possibly followed by thermal annealing, leaves surfaces which show sharp LEED patterns, indicating good stoichiometry and surface order. Atomic hydrogen cleaning should eliminate the chemical etching step, and might reduce the temperature and/or temperature-time product presently used in forming NEA cathodes. The process is readily adaptable to in situ use in ultrahigh vaccum.

  13. Antiradical power of carotenoids and vitamin E: testing the hydrogen atom transfer mechanism.

    PubMed

    Martínez, Ana; Barbosa, Andrés

    2008-12-25

    The antiradical capacities of 13 carotenoids (CAR) and vitamin E are explored, by assessing CAR-H bond dissociation energy. Density functional theory (DFT) calculations were performed, in order to evaluate the hydrogen atom transfer (HAT) antiradical mechanism. Results indicate that C4 or C4' is not always the reactive position when it is unsubstituted and also that CAR without H atoms in the 4 position may be as effective against free radicals as other CAR with H atoms in C4 and C4'. Lutein is the most effective antiradical for the purpose of hydrogen abstraction, whereas the least effective antiradical for this process is canthaxanthin, which is one of the reddest CAR. Vitamin E is not as effective as most of the yellow CAR but may be a better antiradical than canthaxanthin. In addition to the CAR-H bond dissociation energy, the number of reactive positions as we report in this paper represents another important aspect for consideration, when analyzing capacity for scavenging free radicals. Many additional aspects exist, which we do not consider here; thus we cannot attempt to reflect all the factors seen in vivo. However, our results provide comparative information on the relative ability of CAR to protect against free radicals, using the CAR-H bond dissociation energy, as one useful parameter. We hope that our theoretical results will contribute to the advancement of this complex research field.

  14. Comparison of Adsorbed Mercury Screening Method With Cold-Vapor Atomic Absorption Spectrophotometry for Determination of Mercury in Soil

    NASA Technical Reports Server (NTRS)

    Easterling, Donald F.; Hovanitz, Edward S.; Street, Kenneth W.

    2000-01-01

    A field screening method for the determination of elemental mercury in environmental soil samples involves the thermal desorption of the mercury from the sample onto gold and then the thermal desorption from the gold to a gold-film mercury vapor analyzer. This field screening method contains a large number of conditions that could be optimized for the various types of soils encountered. In this study, the conditions were optimized for the determination of mercury in silty clay materials, and the results were comparable to the cold-vapor atomic absorption spectrophotometric method of determination. This paper discusses the benefits and disadvantages of employing the field screening method and provides the sequence of conditions that must be optimized to employ this method of determination on other soil types.

  15. Hydrogen atom transfer reactions in thiophenol: photogeneration of two new thione isomers.

    PubMed

    Reva, Igor; Nowak, Maciej J; Lapinski, Leszek; Fausto, Rui

    2015-02-21

    Photoisomerization reactions of monomeric thiophenol have been investigated for the compound isolated in low-temperature argon matrices. The initial thiophenol population consists exclusively of the thermodynamically most stable thiol form. Phototransformations were induced by irradiation of the matrices with narrowband tunable UV light. Irradiation at λ > 290 nm did not induce any changes in isolated thiophenol molecules. Upon irradiation at 290-285 nm, the initial thiol form of thiophenol converted into its thione isomer, cyclohexa-2,4-diene-1-thione. This conversion occurs by transfer of an H atom from the SH group to a carbon atom at the ortho position of the ring. Subsequent irradiation at longer wavelengths (300-427 nm) demonstrated that this UV-induced hydrogen-atom transfer is photoreversible. Moreover, upon irradiation at 400-425 nm, the cyclohexa-2,4-diene-1-thione product converts, by transfer of a hydrogen atom from the ortho to para position, into another thione isomer, cyclohexa-2,5-diene-1-thione. The latter thione isomer is also photoreactive and is consumed if irradiated at λ < 332 nm. The obtained results clearly show that H-atom-transfer isomerization reactions dominate the unimolecular photochemistry of thiophenol confined in a solid argon matrix. A set of low-intensity infrared bands, observed in the spectra of UV irradiated thiophenol, indicates the presence of a phenylthiyl radical with an H- atom detached from the SH group. Alongside the H-atom-transfer and H-atom-detachment processes, the ring-opening photoreaction occurred in cyclohexa-2,4-diene-1-thione by the cleavage of the C-C bond at the alpha position with respect to the thiocarbonyl C[double bond, length as m-dash]S group. The resulting open-ring conjugated thioketene adopts several isomeric forms, differing by orientations around single and double bonds. The species photogenerated upon UV irradiation of thiophenol were identified by comparison of their experimental infrared

  16. Use of predissociation to enhance the atomic hydrogen ion fraction in ion sources

    DOEpatents

    Kim, Jinchoon

    1979-01-01

    A duopigatron ion source is modified by replacing the normal oxide-coated wire filament cathode of the ion source with a hot tungsten oven through which hydrogen gas is fed into the arc chamber. The hydrogen gas is predissociated in the hot oven prior to the arc discharge, and the recombination rate is minimized by hot walls inside of the arc chamber. With the use of the above modifications, the atomic H.sub.1.sup.+ ion fraction output can be increased from the normal 50% to greater than 70% with a corresponding decrease in the H.sub.2.sup.+ and H.sub.3.sup.+ molecular ion fraction outputs from the ion source.

  17. Multiply Confined Nickel Nanocatalysts Produced by Atomic Layer Deposition for Hydrogenation Reactions.

    PubMed

    Gao, Zhe; Dong, Mei; Wang, Guizhen; Sheng, Pei; Wu, Zhiwei; Yang, Huimin; Zhang, Bin; Wang, Guofu; Wang, Jianguo; Qin, Yong

    2015-07-27

    To design highly efficient catalysts, new concepts for optimizing the metal-support interactions are desirable. Here we introduce a facile and general template approach assisted by atomic layer deposition (ALD), to fabricate a multiply confined Ni-based nanocatalyst. The Ni nanoparticles are not only confined in Al2 O3 nanotubes, but also embedded in the cavities of Al2 O3 interior wall. The cavities create more Ni-Al2 O3 interfacial sites, which facilitate hydrogenation reactions. The nanotubes inhibit the leaching and detachment of Ni nanoparticles. Compared with the Ni-based catalyst supported on the outer surface of Al2 O3 nanotubes, the multiply confined catalyst shows a striking improvement of catalytic activity and stability in hydrogenation reactions. Our ALD-assisted template method is general and can be extended for other multiply confined nanoreactors, which may have potential applications in many heterogeneous reactions.

  18. Compact solid-state laser source for 1S-2S spectroscopy in atomic hydrogen

    SciTech Connect

    Kolachevsky, N.; Alnis, J.; Bergeson, S. D.; Haensch, T. W.

    2006-02-15

    We demonstrate a compact solid-state laser source for high-resolution two-photon spectroscopy of the 1S-2S transition in atomic hydrogen. The source emits up to 20 mW at 243 nm and consists of a 972 nm diode laser, a tapered amplifier, and two doubling stages. The diode laser is actively stabilized to a high-finesse cavity. We compare the new source to the stable 486 nm dye laser used in previous experiments and record 1S-2S spectra using both systems. With the solid-state laser system, we demonstrate a resolution of the hydrogen spectrometer of 6x10{sup 11}, which is promising for a number of high-precision measurements in hydrogenlike systems.

  19. Atom-economical synthesis of γ-valerolactone with self-supplied hydrogen from methanol.

    PubMed

    Li, Zheng; Tang, Xing; Jiang, Yetao; Wang, Yanjun; Zuo, Miao; Chen, Wei; Zeng, Xianhai; Sun, Yong; Lin, Lu

    2015-11-25

    γ-Valerolactone (GVL), a versatile biomass derived platform molecule, was synthesized with a highest yield of 89.8% from methyl levulinate (ML) using self-supplied H2 coming from the decomposition of MeOH derived partially from ML. Cu-Cr acted as a bi-functional catalyst for both H2 production from MeOH and carbonyl hydrogenation. An extremely low amount of MeOH (29 mol% relative to ML) was initially necessary to start up the hydrocyclization of ML to GVL and MeOH, which is in turn employed as an in situ H2 source for ML hydrogenation, providing an atom-economical pathway for GVL production. PMID:26403664

  20. Exact nonrelativistic polarizabilities of the hydrogen atom with the Lagrange-mesh method

    NASA Astrophysics Data System (ADS)

    Baye, Daniel

    2012-12-01

    Exact analytical expressions of the dipole polarizabilities of the nonrelativistic hydrogen atom in spherical coordinates are derived with the help of the Lagrange-mesh numerical method. This method can provide exact energies and wave functions for well-chosen conditions of calculation. Exact dipole polarizabilities are obtained after an unambiguous rounding up to at least principal quantum numbers around n=30. The scalar polarizability of any nl level is given by n4[4n2+14+7l(l+1)]/4 and its tensor polarizability is given by -n4[3n2-9+11l(l+1)]l/4(2l+3), which allows the calculation of the polarizability of any hydrogen state nlm.

  1. Activation of extended red emission photoluminescence in carbon solids by exposure to atomic hydrogen and UV radiation

    NASA Technical Reports Server (NTRS)

    Furton, Douglas G.; Witt, Adolf N.

    1993-01-01

    We report on new laboratory results which relate directly to the observation of strongly enhanced extended red emission (ERE) by interstellar dust in H2 photodissociation zones. The ERE has been attributed to photoluminescence by hydrogenated amorphous carbon (HAC). We are demonstrating that exposure to thermally dissociated atomic hydrogen will restore the photoluminescence efficiency of previously annealed HAC. Also, pure amorphous carbon (AC), not previously photoluminescent, can be induced to photoluminesce by exposure to atomic hydrogen. This conversion of AC into HAC is greatly enhanced by the presence of UV irradiation. The presence of dense, warm atomic hydrogen and a strong UV radiation field are characteristic environmental properties of H2 dissociation zones. Our results lend strong support to the HAC photoluminescence explanation for ERE.

  2. Imaging of a soft, weakly adsorbing, living cell with a colloid probe tapping atomic force microscope technique.

    PubMed

    McNamee, Cathy E; Pyo, Nayoung; Tanaka, Saaya; Kanda, Yoichi; Higashitani, Ko

    2006-01-15

    Here, we propose a new method to improve the atomic force microscopy (AFM) image resolution of soft samples, such as cells, in liquid. Attaching a colloid probe to a cantilever was seen improve the image resolution of a living cell in a physiological buffer solution, obtained by the normal tapping mode, when compared to an image obtained using a regular cantilever tip. This may be due to the averaging out of the cantilever tip swinging caused by the visco-elasticity of the cell. The resolution was best, when silica spheres with a 3.3 microm diameter were attached. Although larger spheres gave a resolution better than a bare cantilever tip, their resolution was less than that obtained for the 3.3 microm diameter silica colloid. This dependency of the image resolution on the colloid probe size may be a result of the increased macroscopic van der Waals attraction between the cell and probe, the decreased repulsive force dependence on the cantilever probe radius, and the decrease in resolution due to the increased probe size. The size of the colloid probe, which should be attached to the cantilever to give the best image resolution, would be the one that optimises the combined result of these facts. PMID:16406494

  3. Interaction of atomic hydrogen with anthracene and polyacene from density functional theory

    NASA Astrophysics Data System (ADS)

    Ferullo, Ricardo M.; Castellani, Norberto J.; Belelli, Patricia G.

    2016-03-01

    The interaction of atomic hydrogen with two linear polycyclic aromatic hydrocarbons (PAHs), anthracene and polyacene (the polymer of benzene), was studied within the density functional theory (DFT). Using a proper dispersion-corrected method (DFT-D) the preferential physisorption sites were explored. The activation barrier for the bond formation between a peripheral C and the incoming H was calculated to be 58.5 and 34.1 meV with pure DFT on anthracene and polyacene at its antiferromagnetic ground state, respectively. DFT-D, although improves the description of the physisorbed state, tends to underestimate the chemisorption barriers due an artifact arising from the dispersion correction.

  4. Reaction of O/sup +/, CO/sup +/, and CH/sup +/ ions with atomic hydrogen

    SciTech Connect

    Federer, W.; Villinger, H.; Howorka, F.; Lindinger, W.; Tosis, P.; Bassi, D.; Ferguson, E.

    1984-06-04

    Rate coefficients for reactions of the ions O/sup +/, CO/sup +/, and CH/sup +/ with atomic hydrogen have been measured for the first time at 300 K. This provides basic data for the ion chemistry of planetary atmospheres, cometary atmospheres, and interstellar molecular clouds. The O/sup +/+H measurement supports quantal calculations of this reaction. The CO/sup +/+H reaction provides an example of partial spin nonconservation in a charge-transfer reaction occurring in a deep potential well. Reactions of the same ions with H/sub 2/ that have been measured elsewhere are also reported.

  5. Traces of Lorentz symmetry breaking in a hydrogen atom at ground state

    NASA Astrophysics Data System (ADS)

    Borges, L. H. C.; Barone, F. A.

    2016-02-01

    Some traces of a specific Lorentz symmetry breaking scenario in the ground state of the hydrogen atom are investigated. We use standard Rayleigh-Schrödinger perturbation theory in order to obtain the corrections to the ground state energy and the wave function. It is shown that an induced four-pole moment arises, due to the Lorentz symmetry breaking. The model considered is the one studied in Borges et al. (Eur Phys J C 74:2937, 2014), where the Lorentz symmetry is broken in the electromagnetic sector.

  6. Hydrogen Gas Sensors Fabricated on Atomically Flat 4H-SiC Webbed Cantilevers

    NASA Technical Reports Server (NTRS)

    Neudeck, Philip G.; Spry, David J.; Trunek, Andrew J.; Evans, Laura J.; Chen, Liang-Yu; Hunter, Gary W.; Androjna, Drago

    2007-01-01

    This paper reports on initial results from the first device tested of a "second generation" Pt-SiC Schottky diode hydrogen gas sensor that: 1) resides on the top of atomically flat 4H-SiC webbed cantilevers, 2) has integrated heater resistor, and 3) is bonded and packaged. With proper selection of heater resistor and sensor diode biases, rapid detection of H2 down to concentrations of 20 ppm was achieved. A stable sensor current gain of 125 +/- 11 standard deviation was demonstrated during 250 hours of cyclic test exposures to 0.5% H2 and N2/air.

  7. Relativistic corrections for screening effects on the energies of hydrogen-like atoms embedded in plasmas

    SciTech Connect

    Poszwa, A.; Bahar, M. K.

    2015-01-15

    The influence of relativistic and plasma screening effects on energies of hydrogen-like atoms embedded in plasmas has been studied. The Dirac equation with a more general exponential cosine screened potential has been solved numerically and perturbatively, by employing the direct perturbation theory. Properties of spectra corresponding to bound states and to different sets of the potential parameters have been studied both in nonrelativistic and relativistic approximations. Binding energies, fine-structure splittings, and relativistic energy shifts have been determined as functions of parameters of the potential. The results have been compared with the ones known from the literature.

  8. The Anomalous Zeeman Effect for the Hydrogen Atom in Noncommutative Space

    NASA Astrophysics Data System (ADS)

    Santos, Willien O.; Souza, Andre M. C.

    2012-12-01

    The Hamiltonian describing an anomalous Zeeman effect for the hydrogen atom on noncommutative space is studied using a Bopp's shift. Using first order perturbation theory, the correction to the energy is calculated for the case of a weak external magnetic field. We also obtained the orbital and spin g-factors in noncommutative space. We show that the experimental values for the orbital and spin g-factors put an upper bound on the magnitude of the parameter of noncommutativity of the order of, respectively, Θ≤(8 GeV)-2 and Θ≤(0.01 GeV)-2.

  9. Phase transition into the metallic state in hypothetical (without molecules) dense atomic hydrogen

    SciTech Connect

    Khomkin, A. L. Shumikhin, A. S.

    2013-10-15

    A simple physical model of the metal-dielectric (vapor-liquid) phase transition in hypothetical (without molecules) atomic hydrogen is proposed. The reason for such a transition is the quantum collective cohesive energy occurring due to quantum electron-electron exchange similar to the cohesive energy in the liquid-metal phase of alkali metals. It is found that the critical parameters of the transition are P{sub c} ∼ 41000 atm, ρ{sub c} ∼ 0.1 g/cm{sup 3}, and T{sub c} ∼ 9750 K.

  10. Exposure of epitaxial graphene on SiC(0001) to atomic hydrogen.

    PubMed

    Guisinger, Nathan P; Rutter, Gregory M; Crain, Jason N; First, Phillip N; Stroscio, Joseph A

    2009-04-01

    Graphene films on SiC exhibit coherent transport properties that suggest the potential for novel carbon-based nanoelectronics applications. Recent studies suggest that the role of the interface between single layer graphene and silicon-terminated SiC can strongly influence the electronic properties of the graphene overlayer. In this study, we have exposed the graphitized SiC to atomic hydrogen in an effort to passivate dangling bonds at the interface, while investigating the results utilizing room temperature scanning tunneling microscopy.

  11. Atomic and ionic spectrum lines below 2000A: hydrogen through argon

    SciTech Connect

    Kelly, R.L.

    1982-10-01

    A critical tabulation of observed spectral lines below 2000 angstroms has been prepared from the published literature up to July 1978. It is intended principally as an aid to those physicists and astronomers who deal with the spectra of highly stripped atoms. This report includes the first 18 elements, from hydrogen (including deuterium) through argon. The tabulation is divided into two main sections: the spectrum lines by spectrum, and a finding list. The entries for each element give the ionization species, ground state term, and ionization potential, as well as the best values of vacuum wavelength, intensity, and classification. A list of the pertinent references is appended at the end.

  12. Dichotomy of the hydrogen atom in superintense, high-frequency laser fields

    SciTech Connect

    Pont, M.; Walet, N.R.; Gavrila, M.; McCurdy, C.W.

    1988-08-22

    We study the behavior of atomic hydrogen in a monochromatic radiation field of high frequency ..omega.. and high-intensity I, when its structure depends only on the parameter ..cap alpha../sub 0/ = I/sup 1/2/..omega../sup -2/ a.u., and multiphoton ionization is quenched. At large ..cap alpha../sub 0/ the ground-state binding energy undergoes a drastic reduction. This is coupled to an unprecedented stretching of the (oscillating) electron wave function, culminating in its separation into two parts (dichotomy) for ..cap alpha../sub 0/>50 a.u.

  13. Absorption of infrared radiation by electrons in the field of a neutral hydrogen atom

    NASA Technical Reports Server (NTRS)

    Stallcop, J. R.

    1974-01-01

    An analytical expression for the absorption coefficient is developed from a relationship between the cross-section for inverse bremsstrahlung absorption and the cross-section for electron-atom momentum transfer; it is accurate for those photon frequencies v and temperatures such that hv/kT is small. The determination of the absorption of infrared radiation by free-free transitions of the negative hydrogen ion has been extended to higher temperatures. A simple analytical expression for the absorption coefficient has been derived.

  14. Absolute differential cross sections for electron capture and loss by kilo-electron-volt hydrogen atoms

    NASA Technical Reports Server (NTRS)

    Smith, G. J.; Johnson, L. K.; Gao, R. S.; Smith, K. A.; Stebbings, R. F.

    1991-01-01

    This paper reports measurements of absolute differential cross sections for electron capture and loss for fast hydrogen atoms incident on H2, N2, O2, Ar, and He. Cross sections have been determined in the 2.0- to 5.0-keV energy range over the laboratory angular range 0.02-2 deg, with an angular, resolution of 0.02 deg. The high angular resolution allows observation of the structure at small angles in some of the cross sections. Comparison of the present results with those of other authors generally shows very good agreement.

  15. Experimentally attainable example of chaotic tunneling: The hydrogen atom in parallel static electric and magnetic fields

    SciTech Connect

    Delande, Dominique; Zakrzewski, Jakub

    2003-12-01

    Statistics of tunneling rates in the presence of chaotic classical dynamics is discussed on a realistic example: a hydrogen atom placed in parallel, uniform, static electric, and magnetic fields, where tunneling is followed by ionization along the fields direction. Depending on the magnetic quantum number, one may observe either a standard Porter-Thomas distribution of tunneling rates or, for strong scarring by a periodic orbit parallel to the external fields, strong deviations from it. For the latter case, a simple model based on random matrix theory gives the correct distribution.

  16. A correlational analysis of the effects of changing environmental conditions on the NR atomic hydrogen maser

    NASA Technical Reports Server (NTRS)

    Dragonette, Richard A.; Suter, Joseph J.

    1992-01-01

    An extensive statistical analysis has been undertaken to determine if a correlation exists between changes in an NR atomic hydrogen maser's frequency offset and changes in environmental conditions. Correlation analyses have been performed comparing barometric pressure, humidity, and temperature with maser frequency offset as a function of time for periods ranging from 5.5 to 17 days. Semipartial correlation coefficients as large as -0.9 have been found between barometric pressure and maser frequency offset. Correlation between maser frequency offset and humidity was small compared to barometric pressure and unpredictable. Analysis of temperature data indicates that in the most current design, temperature does not significantly affect maser frequency offset.

  17. Low Energy Charge Transfer between C5+ and Atomic Hydrogen

    SciTech Connect

    Draganic, Ilija N; Seely, D. G.; Havener, Charles C

    2011-01-01

    Charge transfer (CT) with carbon ions has been identified for a long time as important in both magnetic fusion plasma devices and more recently in solar wind interactions with comets, planets, or neutrals in the heliosphere. A merged-beams technique is used to measure the absolute total charge transfer cross section for C5+ and atomic H over four orders of magnitude in collision energy, from 12,000 eV/u to 0.64 eV/u. The present measurements are compared with previous measurements using an atomic hydrogen target and benchmark available classical trajectory Monte-Carlo and molecular-orbital close-coupling calculations. An increasing cross section below 10 eV/u is attributed to trajectory effects due to the ion-induced dipole attraction between reactants.

  18. Low-energy charge transfer between C5+ and atomic hydrogen

    SciTech Connect

    Draganic, Ilija N; Havener, Charles C; Seely, D. G.

    2011-01-01

    Charge transfer with carbon ions has been identified as important in both magnetic fusion plasma devices and, more recently, in solar wind interactions with comets, planets, or neutrals in the heliosphere. A merged-beams technique is used to measure the absolute total charge-transfer cross section for C{sup 5+} and atomic H over four orders of magnitude in collision energy, from 12,000 to 0.64 eV/u. The present measurements are compared with previous measurements using an atomic hydrogen target and benchmark available classical trajectory Monte Carlo and molecular-orbital close-coupling calculations. An observed increasing cross section below 10 eV/u is attributed to trajectory effects due to the ion-induced dipole attraction between reactants.

  19. Hidden momentum in a hydrogen atom and the Lorentz-force law

    NASA Astrophysics Data System (ADS)

    Filho, J. S. Oliveira; Saldanha, Pablo L.

    2015-11-01

    By using perturbation theory, we show that a hydrogen atom with magnetic moment due to the orbital angular momentum of the electron has so-called hidden momentum in the presence of an external electric field. This means that the atomic electronic cloud has a nonzero linear momentum in its center-of-mass rest frame due to a relativistic effect. This is completely analogous to the hidden momentum that a classical current loop has in the presence of an external electric field. We discuss how this effect is essential for the validity of the Lorentz-force law in quantum systems. We also connect our results to the long-standing Abraham-Minkowski debate about the momentum of light in material media.

  20. Low-energy charge transfer between C{sup 5+} and atomic hydrogen

    SciTech Connect

    Draganic, I. N.; Havener, C. C.; Seely, D. G.

    2011-05-15

    Charge transfer with carbon ions has been identified as important in both magnetic fusion plasma devices and, more recently, in solar wind interactions with comets, planets, or neutrals in the heliosphere. A merged-beams technique is used to measure the absolute total charge-transfer cross section for C{sup 5+} and atomic H over four orders of magnitude in collision energy, from 12 000 to 0.64 eV/u. The present measurements are compared with previous measurements using an atomic hydrogen target and benchmark available classical trajectory Monte Carlo and molecular-orbital close-coupling calculations. An observed increasing cross section below 10 eV/u is attributed to trajectory effects due to the ion-induced dipole attraction between reactants.

  1. State of the art and future directions for the atomic hydrogen maser

    NASA Technical Reports Server (NTRS)

    Vessot, Robert F. C.

    1990-01-01

    The present status of technology development for atomic hydrogen masers (H-masers) is reviewed. The limitations to frequency stability and accuracy are discussed with emphasis on the problems associated with cavity resonator instability and the lack of reproducibility and stability of the storage volume wall coating frequency shift. New types of coating developed in the Soviet Union and better, cavity resonator materials, are expected to make possible frequency at the 10(exp -16) level at 10(exp 4) sec. Better control of systematic effects should extend the long-term stability to levels better than 10(exp -15) for intervals beyond one day. Present use of H-masers as flywheel oscillators in timekeeping systems is discussed as is the outlook for the future cryogenic and room temperature H-masers as flywheel oscillators to operate very high resolution frequency discriminators based on the newly evolving technology of trapped and cooled ions and atoms.

  2. Resonant charge transfer of hydrogen Rydberg atoms incident at a metallic sphere

    NASA Astrophysics Data System (ADS)

    Gibbard, J. A.; Softley, T. P.

    2016-06-01

    A wavepacket propagation study is reported for the charge transfer of low principal quantum number (n = 2) hydrogen Rydberg atoms incident at an isolated metallic sphere. Such a sphere acts as a model for a nanoparticle. The three-dimensional confinement of the sphere yields discrete surface-localized ‘well-image’ states, the energies of which vary with sphere radius. When the Rydberg atom energy is degenerate with one of the quantized nanoparticle states, charge transfer is enhanced, whereas for off-resonant cases little to no charge transfer is observed. Greater variation in charge-transfer probability is seen between the resonant and off-resonant examples in this system than for any other Rydberg-surface system theoretically investigated thus far. The results presented here indicate that it may be possible to use Rydberg-surface ionization as a probe of the surface electronic structure of a nanoparticle, and nanostructures in general.

  3. Spontaneous light emission by atomic hydrogen: Fermi's golden rule without cheating

    NASA Astrophysics Data System (ADS)

    Debierre, V.; Durt, T.; Nicolet, A.; Zolla, F.

    2015-10-01

    Focusing on the 2 p- 1 s transition in atomic hydrogen, we investigate through first order perturbation theory the time evolution of the survival probability of an electron initially taken to be in the excited (2 p) state. We examine both the results yielded by the standard dipole approximation for the coupling between the atom and the electromagnetic field - for which we propose a cutoff-independent regularisation - and those yielded by the exact coupling function. In both cases, Fermi's golden rule is shown to be an excellent approximation for the system at hand: we found its maximal deviation from the exact behaviour of the system to be of order 10-8 /10-7. Our treatment also yields a rigorous prescription for the choice of the optimal cutoff frequency in the dipole approximation. With our cutoff, the predictions of the dipole approximation are almost indistinguishable at all times from the exact dynamics of the system.

  4. On the role of atomic metastability in the production of Balmer line radiation from ‘cold’ atomic hydrogen, deuterium and hydrogenic ion impurities in fusion edge plasmas

    NASA Astrophysics Data System (ADS)

    Hey, J. D.

    2012-03-01

    Published arguments, which assign an important role to atomic metastability in the production of ‘narrow’ Zeeman component radiation from the boundary region of fusion plasmas, are examined critically in relation to l-redistribution by proton and electron collisions, and mixing of unperturbed atomic states by the ion microfield and microfield gradient. It is concluded that these important processes indeed severely constrain the contribution from ‘metastable’ states to the generation of the hydrogen Balmer spectra, for electron concentrations above 1012 cm-3, as pointed out before by the present author (Hey et al 1999 J. Phys. B: At. Mol. Opt. Phys. 32 3555). The analysis of collision-induced l-redistribution represents an extension of that used previously (Hey et al 1996 Contrib. Plasma Phys. 36 583), applicable up to higher electron densities. For comparison purposes, we also consider the question of metastability of ionized helium in a low-temperature plasma, and that of some common hydrogenic impurities (C5+ and Ne9+) in a hydrogen (deuterium) fusion plasma. While for low nuclear charge Z the metastability of 2s1/2 levels is quenched by the plasma environment, it is much reduced in high-Z ions owing to the rapid increase with Z of the two-photon electric dipole (2E1) and magnetic dipole (M1) spontaneous transition rates to the ground state, whereas the role of the plasma in these cases is less important. The main new principle elaborated in this work is the sensitivity of atomic line strengths, and hence collision strengths, to perturbation by the plasma environment for transitions between fine-structure sublevels of the same principal quantum number. As the plasma microfield strength grows, ‘allowed’ transitions diminish in strength, while ‘forbidden’ transitions grow. However, owing to violation of the parity selection rule, there is an overall loss of collision strength available to transitions, resulting from the appearance of significant

  5. Adsorbent phosphates

    NASA Technical Reports Server (NTRS)

    Watanabe, S.

    1983-01-01

    An adsorbent which uses as its primary ingredient phosphoric acid salts of zirconium or titanium is presented. Production methods are discussed and several examples are detailed. Measurements of separating characteristics of some gases using the salts are given.

  6. Ab initio study of Ga-GaN system: Transition from adsorbed metal atoms to a metal–semiconductor junction

    SciTech Connect

    Witczak, Przemysław; Kempisty, Pawel; Strak, Pawel

    2015-11-15

    Ab initio studies of a GaN(0001)-Ga system with various thicknesses of a metallic Ga layer were undertaken. The studied systems extend from a GaN(0001) surface with a fractional coverage of gallium atoms to a Ga-GaN metal–semiconductor (m–s) contact. Electronic properties of the system are simulated using density functional theory calculations for different doping of the bulk semiconductor. It is shown that during transition from a bare GaN(0001) surface to a m–s heterostructure, the Fermi level stays pinned at a Ga-broken bond highly dispersive surface state to Ga–Ga states at the m–s interface. Adsorption of gallium leads to an energy gain of about 4 eV for a clean GaN(0001) surface and the energy decreases to 3.2 eV for a thickly Ga-covered surface. The transition to the m–s interface is observed. For a thick Ga overlayer such interface corresponds to a Schottky contact with a barrier equal to 0.9 and 0.6 eV for n- and p-type, respectively. Bond polarization-related dipole layer occurring due to an electron transfer to the metal leads to a potential energy jump of 1.5 eV, independent on the semiconductor doping. Additionally high electron density in the Ga–Ga bond region leads to an energy barrier about 1.2 eV high and 4 Å wide. This feature may adversely affect the conductivity of the n-type m–s system.

  7. Reduction of FeO/Pt(1 1 1) Thin Films by Exposure to Atomic Hydrogen

    SciTech Connect

    Knudsen, Jan; Merte, L. R.; Grabow, Lars C.; Eichhorn, Falk M.; Porsgaard, Soeren; Zeuthen, Helene; Vang, Ronnie T.; Laegsgaard, E.; Mavrikakis, Manos; Besenbacher, Fleming

    2010-01-01

    Using scanning tunneling microscopy (STM), X-ray photoemission spectroscopy (XPS) and density functional theory (DFT) calculations we have studied the reduction of ultra-thin films of FeO(1 1 1) grown on Pt(1 1 1) after exposure to atomic hydrogen at room temperature. A number of new ordered, partlyreduced FeOx structures are identified and as a general trend we reveal that all the reduced FeOx structures incorporate 2-fold coordinated Fe atoms as opposed to the original 3-fold coordinated Fe atoms in the FeO film. We find that when all the Fe atoms are 2-fold O-coordinated the FeOx surface structure is resistant to further reduction at room temperature. We observe that water easily dissociates on the most heavily reduced FeOx, structure in contrast to the initially inert FeO film, and reveal that it is possible to partially re-oxidize the FeOx film by heating the surface slightly in the presence of water.

  8. Time-resolved Absorption Spectra of the Laser-dressed Hydrogen Atom

    NASA Astrophysics Data System (ADS)

    Murakami, Mitsuko; Chu, Shih-I.

    2013-05-01

    A theoretical study of the transient absorption spectra for the laser-dressed hydrogen atom based on the accurate numerical solution of the time-dependent Schrödinger equation is presented. The timing of absorption is controlled by the time delay between an isolated extreme ultraviolet (XUV) pulse and a dressing infrared (IR) field. We identify two different kinds of physical processes in the spectra. One is the formation of dressed states, signified by the appearance of sidebands between the XUV absorption lines separated by one IR-photon energy. We show that their population is maximized when the XUV pulse coincides with the zero-crossing of the IR field, and that their energy can be manipulated by using a chirped IR field. The other process is the dynamical AC Stark shift induced by the IR field and probed by the XUV pulse. Our calculations indicate that the accidental degeneracy of the hydrogen atom leads to the multiple splittings of each XUV absorption line whose separations change in response to a slowly-varying IR envelope. Furthermore, we observe the Autler-Townes doublets for the n=2 and 3 states using the 656 nm dressing field, but their separation does not agree with the prediction by the conventional 3-level model that neglects the dynamical AC Stark effects.

  9. First-principles calculations of the interaction between hydrogen and 3d alloying atom in nickel

    NASA Astrophysics Data System (ADS)

    Liu, Wenguan; Qian, Yuan; Zhang, Dongxun; Liu, Wei; Han, Han

    2015-10-01

    Knowledge of the behavior of hydrogen (H) in Ni-based alloy is essential for the prediction of Tritium behavior in Molten Salt Reactor. First-principles calculations were performed to investigate the interaction between H and 3d transition metal (TM) alloying atom in Ni-based alloy. H prefers the octahedral interstitial site to the tetrahedral interstitial site energetically. Most of the 3d TM elements (except Zn) attract H. The attraction to H in the Ni-TM-H system can be mainly attributed to the differences in electronegativity. With the large electronegativity, H and Ni gain electrons from the other TM elements, resulting in the enhanced Ni-H bonds which are the source of the attraction to H in the Ni-TM-H system. The obviously covalent-like Cr-H and Co-H bindings are also beneficial to the attraction to H. On the other hand, the repulsion to H in the Ni-Zn-H system is due to the stable electronic configuration of Zn. We mainly utilize the results calculated in 32-atom supercell which corresponds to the case of a relatively high concentration of hydrogen. Our results are in good agreement with the experimental ones.

  10. Three-dimensional atomic mapping of hydrogenated polymorphous silicon solar cells

    NASA Astrophysics Data System (ADS)

    Chen, Wanghua; Pareige, Philippe; Roca i Cabarrocas, Pere

    2016-06-01

    Hydrogenated polymorphous silicon (pm-Si:H) is a nanostructured material consisting of silicon nanocrystals embedded in an amorphous silicon matrix. Its use as the intrinsic layer in thin film p-i-n solar cells has led to good cell properties in terms of stability and efficiency. Here, we have been able to assess directly the concentration and distribution of nanocrystals and impurities (dopants) in p-i-n solar cells, by using femtosecond laser-assisted atom probe tomography (APT). An effective sample preparation method for APT characterization is developed. Based on the difference in atomic density between hydrogenated amorphous and crystalline silicon, we are able to distinguish the nanocrystals from the amorphous matrix by using APT. Moreover, thanks to the three-dimensional reconstruction, we demonstrate that Si nanocrystals are homogeneously distributed in the entire intrinsic layer of the solar cell. The influence of the process pressure on the incorporation of nanocrystals and their distribution is also investigated. Thanks to APT we could determine crystalline fractions as low as 4.2% in the pm-Si:H films, which is very difficult to determine by standard techniques, such as X-ray diffraction, Raman spectroscopy, and spectroscopic ellipsometry. Moreover, we also demonstrate a sharp p/i interface in our solar cells.

  11. Observation and Interpretation of Energetic Neutral Hydrogen Atoms from the December 5, 2006 Solar Flare

    NASA Technical Reports Server (NTRS)

    Barghouty, A. F.; Mewaldt, R. A.; Leske, R. A.; Shih, A. Y.; Stone, E. C.; Cohen, C. M. S.; Cummings, A. C.; Labrador, A. W.; vonRosenvinge, T. T.; Wiedenbeck, M. E.

    2009-01-01

    We discuss observations of energetic neutral hydrogen atoms (ENAs) from a solar flare/coronal mass ejection event reported by Mewaldt et al. (2009). The observations were made during the 5 December 2006 X9 solar flare, located at E79, by the Low Energy Telescopes (LETs) on STEREO A and B. Prior to the arrival of the main solar energetic particle (SEP) event at Earth, both LETs observed a sudden burst of 1.6 to 15 MeV particles arriving from the Sun. The derived solar emission profile, arrival directions, and energy spectrum all show that the <5 MeV particles were due to energetic neutral hydrogen atoms produced by either flare or shock-accelerated protons. RHESSI measurements of the 2.2-MeV gamma-ray line provide an estimate of the number of interacting flare-accelerated protons in this event, which leads to an improved estimate of ENA production by flare-accelerated protons. CME-driven shock acceleration is also considered. Taking into account ENA losses, we conclude that the observed ENAs must have been produced in the high corona at heliocentric distances .2 solar radii.

  12. Observations and Interpretations of Energetic Neutral Hydrogen Atoms from the December 5, 2006 Solar Event

    NASA Technical Reports Server (NTRS)

    Mewaldt, R. A.; Leske, R. A.; Shih, A. Y.; Stone, E. C.; Barghouty, A. f.; Cohen, C. M. S.; Cummings, A. c.; Labrador, A. W.; vonRosenvinge, T. T.

    2009-01-01

    We discuss recently reported observations of energetic neutral hydrogen atoms (ENAs) from an X9 solar flare/coronal mass ejection event on 5 December 2006, located at E79. The observations were made by the Low Energy Telescopes (LETs) on STEREO A and B. Prior to the arrival of the main solar energetic particle (SEP) event at Earth, both LETs observed a sudden burst of 1.6 to 15 MeV energetic neutral hydrogen atoms produced by either flare or shock-accelerated protons. RHESSI measurements of the 2.2-MeV gamma-ray line provide an estimate of the number of interacting flare-accelerated protons in this event, which leads to an improved estimate of ENA production by flare-accelerated protons. Taking into account ENA losses, we find that the observed ENAs must have been produced in the high corona at heliocentric distances > or equal to 2 solar radii. Although there are no CME images from this event, it is shown that CME-shock-accelerated protons can, in principle, produce a time-history consistent with the observations.

  13. STEREO Observations of Energetic Neutral Hydrogen Atoms during the 5 December 2006 Solar Flare

    NASA Technical Reports Server (NTRS)

    Mewaldt, R. A.; Leske, R. A.; Stone, E. C.; Barghouty, A. F.; Labrador, A. W.; Cohen, C. M. S.; Cummings, A. C.; Davis, A. J.; vonRosenvinge, T. T.; Wiedenbeck, M. E.

    2009-01-01

    We report the discovery of energetic neutral hydrogen atoms emitted during the X9 solar event of December 5, 2006. Beginning 1 hour following the onset of this E79 flare, the Low Energy Telescopes (LETs) on both the STEREO A and B spacecraft observed a sudden burst of 1.6 to 15 MeV protons beginning hours before the onset of the main solar energetic particle (SEP) event at Earth. More than 70% of these particles arrived from a longitude within 10 of the Sun, consistent with the measurement resolution. The derived emission profile at the Sun had onset and peak times remarkably similar to the GOES soft X-ray profile and continued for more than an hour. The observed arrival directions and energy spectrum argue strongly that the particle events less than 5 MeV were due to energetic neutral hydrogen atoms (ENAs). To our knowledge, this is the first reported observation of ENA emission from a solar flare/coronal mass ejection. Possible origins for the production of ENAs in a large solar event are considered. We conclude that the observed ENAs were most likely produced in the high corona and that charge-transfer reactions between accelerated protons and partially-stripped coronal ions are an important source of ENAs in solar events.

  14. Neutron diffraction determination of hydrogen atom locations in the α(TiCrSiO) 1/1 crystal approximant

    NASA Astrophysics Data System (ADS)

    Kim, J. Y.; Kim, W. J.; Gibbons, P. C.; Kelton, K. F.; Yelon, W. B.

    1999-08-01

    Titanium/zirconium-based quasicrystals and their related crystal approximants have been identified as potential new materials for hydrogen storage applications. To better understand the local chemistry and atomic ordering in these phases, preferential interstitial sites for hydrogen/deuterium were determined for α(TiCrSiO). This is a bcc 1/1 crystal approximant to the icosahedral quasicrystal phase that contains a two-shell, Mackay-icosahedral cluster of atoms at each bcc site. It absorbs hydrogen or deuterium, without formation of other hydride phases, to a maximum hydrogen to metal atom ratio (H/M) of 0.26. For fully deuterated samples, both tetrahedral and octahedral interstitial sites are occupied with fractions of 0.14 and 0.12, respectively. Here, the hydrogen/deuterium sites are determined from a Rietveld analysis of x-ray and neutron powder diffraction data taken from samples of α(TiCrSiO) loaded with deuterium. Only the octahedral sites are occupied in the partially deuterated samples (D/M=0.11). A decrease in the oxygen concentration below the stoichiometric value for α(TiCrSiO) leads to an increase in the total amount of hydrogen that can be absorbed, suggesting that these interstitial atoms are competing for the same octahedral interstitial sites.

  15. Emission of hydrogen energetic neutral atoms from the Martian subsolar magnetosheath

    NASA Astrophysics Data System (ADS)

    Wang, X.-D.; Alho, M.; Jarvinen, R.; Kallio, E.; Barabash, S.; Futaana, Y.

    2016-01-01

    We have simulated the hydrogen energetic neutral atom (ENA) emissions from the subsolar magnetosheath of Mars using a hybrid model of the proton plasma charge exchanging with the Martian exosphere to study statistical features revealed from the observations of the Neutral Particle Detectors on Mars Express. The simulations reproduce well the observed enhancement of the hydrogen ENA emissions from the dayside magnetosheath in directions perpendicular to the Sun-Mars line. Our results show that the neutralized protons from the shocked solar wind are the dominant ENA population rather than those originating from the pickup planetary ions. The simulation also suggests that the observed stronger ENA emissions in the direction opposite to the solar wind convective electric field result from a stronger proton flux in the same direction at the lower magnetosheath; i.e., the proton fluxes in the magnetosheath are not cylindrically symmetric. We also confirm the observed increasing of the ENA fluxes with the solar wind dynamical pressure in the simulations. This feature is associated with a low altitude of the induced magnetic boundary when the dynamic pressure is high and the magnetosheath protons can reach to a denser exosphere, and thus, the charge exchange rate becomes higher. Overall, the analysis suggests that kinetic effects play an important and pronounced role in the morphology of the hydrogen ENA distribution and the plasma environment at Mars, in general.

  16. Sensitized anti-Stokes luminescence centers in microcrystals of Zn0.6Cd0.4S solid solutions with adsorbed dye molecules and few-atomic silver clusters

    NASA Astrophysics Data System (ADS)

    Ovchinnikov, O. V.; Kosyakova, E. A.; Leonova, L. Yu.; Smirnov, M. S.; Evlev, A. B.; Latyshev, A. N.; Utekhin, A. N.

    2008-03-01

    The sensitized anti-Stokes luminescence excited by radiation with wavelengths from 610 to 750 nm and flux densities of 1014 1015 quanta/(cm2·s) is detected for microcrystals of Zn 0.6 Cd 0.4 S solid solutions with adsorbed organic malachite green and methylene blue dye molecules. The position of its excitation spectra coincides with that of the absorption spectra of adsorbed dye molecules, which suggests the cooperative mechanism of its occurrence. The possibility of amplification of the anti-Stokes luminescence by means of adsorption of silver atoms and few-atomic silver clusters, in addition to the dye molecules, on the Zn 0.6 Cd 0.4 S surface is investigated. It is assumed that in the latter case, the anti-Stokes luminescence is excited as a result of two-quantum optical transitions with electron or electron excitation energy transfer from the dye molecules adsorbed on the Zn 0.6 Cd 0.4 S surface to silver atoms and few-atomic silver clusters creating deep local states with photoionization energies of 1.8 2.0 eV in the gap.

  17. Absolute Rates of the Solution-Phase Addition of Atomic Hydrogen to a Vinyl Ether and a Vinyl Ester: Effect of Oxygen Substitution on Hydrogen Atom Reactivity with Olefins

    SciTech Connect

    Tanner, D D.; Kandanarachchi, P; Das, N. C.; Franz, James A.

    2003-04-08

    The reactions of vinyl butyl ether and vinyl butyrate with atomic hydrogen and deuterium lead to addition at the terminal position of the olefins. This observation is consistent with the reactions carried out earlier with other olefins. Both of the absolute rates of addition to vinylbutyl ether and vinyl butyrate, in acetone and hexane, were measured at several temperatures. The relative rates are consistent with only modest stabilization of the transition state of the radical adduct by the R-O substituent compared with that of hydrogen atom addition to 1-octene. The relative rates measured in acetone and hexane indicate no significant differential solvation of the ground state relative to the transition structures of the hydrogen atom addition. The kinetics reveal that the early transition states for hydrogen atom addition exhibit little selectivity (vinyl ether versus simple olefin) in either the abstraction of hydrogen R to the oxygen or by terminal addition to the olefinic ether and reflects the modest influence of the increased enthalpy of reaction associated with resonance stabilization by the oxygen substituent at the developing radical site.

  18. Radiative cascade of highly excited hydrogen atoms in strong magnetic fields

    SciTech Connect

    Topcu, Tuerker; Robicheaux, Francis

    2006-04-15

    We have studied the radiative decay of atomic hydrogen in strong magnetic fields of up to 4 T. We have followed the radiative cascade from completely l,m mixed distributions of highly excited states as well as from distributions that involve highly excited states with |m|{approx}n. We have found that the time it takes to populate the ground state is not affected by the magnetic field for the initial states with n < or approx. 20. For higher n manifolds, the electrons in the most negative m states are substantially slowed down by the magnetic field resulting in a much longer lifetime. We show that less than 10% of the antihydrogen atoms with n{approx}35 generated in antihydrogen experiments at 4 K will decay to their ground states before they hit the wall of the vacuum container unless they are trapped. We have also found that the decay time is mainly determined by the fraction of atoms that were initially in highest negative m states due to the fact that only {delta}m+{delta}{pi}=1 transitions are allowed in the magnetic field. We give a semiclassical method for calculating the decay rates for circular states and show that when the initial states have high-m, semiclassical rates agree with the full quantum mechanical rates within a couple of percent for states with effective n > or approx. 20.

  19. Concerted Hydrogen Atom and Electron Transfer Mechanism for Catalysis by Lysine-Specific Demethylase

    PubMed Central

    Yu, Tao; Higashi, Masahiro; Cembran, Alessandro; Gao, Jiali; Truhlar, Donald G.

    2015-01-01

    We calculate the free energy profile for the postulated hydride transfer reaction mechanism for the catalysis of lysine demethylation by lysine-specific demethylase LSD1. The potential energy surface is obtained by using combined electrostatically embedded multi-configuration molecular mechanics (EE-MCMM) and single-configuration molecular mechanics (MM). We employ a constant valence bond coupling term to obtain analytical energies and gradients of the EE-MCMM subsystem, which contains 45 QM atoms and which is parametrized with a density functional calculations employing specific reaction parameters obtained by matching high-level wave function calculations. In the MM region, we employ the Amber ff03 and TIP3P force fields. The free energy of activation at 300 K is calculated by molecular dynamics (MD) umbrella sampling on a system with 102090 atoms as the maximum of the free energy profile along the reaction coordinate as obtained by the weighted histogram analysis method with 17 umbrella sampling windows. This yields a free energy of activation of only 10 kcal/mol, showing that the previously postulated direct hydride transfer reaction mechanism is plausible, although we find that it is better interpreted as a concerted transfer of a hydrogen atom and an electron. PMID:23725223

  20. Imaging the South Pole-Aitken basin in backscattered neutral hydrogen atoms

    NASA Astrophysics Data System (ADS)

    Vorburger, A.; Wurz, P.; Barabash, S.; Wieser, M.; Futaana, Y.; Bhardwaj, A.; Asamura, K.

    2015-09-01

    The lunar surface is very efficient in reflecting impinging solar wind ions as energetic neutral atoms (ENAs). A global analysis of lunar hydrogen ENAs showed that on average 16% of the solar wind protons are reflected, and that the reflected fraction can range from less than 8% to more than 24%, depending on location. It is established that magnetic anomalies reduce the flux of backscattered hydrogen ENAs by screening-off a fraction of the impinging solar wind. The effects of the surface properties, such as porosity, roughness, chemical composition, and extent of weathering, were not known. In this paper, we conduct an in-depth analysis of ENA observations of the South Pole-Aitken basin to determine which of the surface properties might be responsible for the observed variation in the integral ENA flux. The South Pole-Aitken basin with its highly variable surface properties is an ideal object for such studies. It is very deep, possesses strikingly elevated concentrations in iron and thorium, has a low albedo and coincides with a cluster of strong magnetic anomalies located on the northern rim of the basin. Our analysis shows that whereas, as expected, the magnetic anomalies can account well for the observed ENA depletion at the South Pole-Aitken basin, none of the other surface properties seem to influence the ENA reflection efficiency. Therefore, the integral flux of backscattered hydrogen ENAs is mainly determined by the impinging plasma flux and ENA imaging of backscattered hydrogen captures the electrodynamics of the plasma at the surface. We cannot exclude minor effects by surface features. We create two maps of surface reflected ENAs at the South Pole-Aitken basin. We compare these ENA maps to elevation, albedo, composition and magnetic field maps. The ENA maps only significantly correlate with the magnetic field map. ENA imaging captures solely the electrodynamics of the plasma at the surface.

  1. Production of high brightness H- beam by charge exchange of hydrogen atom beam in sodium jet

    SciTech Connect

    Davydenko, V.; Zelenski, A.; Ivanov, A.; Kolmogorov, A.

    2010-11-16

    Production of H{sup -} beam for accelerators applications by charge exchange of high brightness hydrogen neutral beam in a sodium jet cell is experimentally studied in joint BNL-BINP experiment. In the experiment, a hydrogen-neutral beam with 3-6 keV energy, equivalent current up to 5 A and 200 microsecond pulse duration is used. The atomic beam is produced by charge exchange of a proton beam in a pulsed hydrogen target. Formation of the proton beam is performed in an ion source by four-electrode multiaperture ion-optical system. To achieve small beam emittance, the apertures in the ion-optical system have small enough size, and the extraction of ions is carried out from the surface of plasma emitter with a low transverse ion temperature of {approx}0.2 eV formed as a result of plasma jet expansion from the arc plasma generator. Developed for the BNL optically pumped polarized ion source, the sodium jet target with recirculation and aperture diameter of 2 cm is used in the experiment. At the first stage of the experiment H{sup -} beam with 36 mA current, 5 keV energy and {approx}0.15 cm {center_dot} mrad normalized emittance was obtained. To increase H{sup -} beam current ballistically focused hydrogen neutral beam will be applied. The effects of H{sup -} beam space-charge and sodium-jet stability will be studied to determine the basic limitations of this approach.

  2. Electron-stimulated reactions in layered CO/H2O films: Hydrogen atom diffusion and the sequential hydrogenation of CO to methanol

    SciTech Connect

    Petrik, Nikolay G.; Monckton, Rhiannon J.; Koehler, Sven; Kimmel, Gregory A.

    2014-05-28

    Low-energy (100 eV) electron-stimulated reactions in layered H2O/CO/H2O ices are investigated. For CO trapped within approximately 50 ML of the vacuum interface in the amorphous solid water (ASW) films, both oxidation and reduction reactions are observed. However for CO buried more deeply in the film, only the reduction of CO to methanol is observed. Experiments with layered films of H2O and D2O show that the hydrogen atoms participating in the reduction of the buried CO originate in region from ~10 – 40 ML below the surface of the ASW films and subsequently diffuse through the film. For deeply buried CO layers, the CO reduction reactions quickly increase with temperature above ~60 K. We present a simple chemical kinetic model that treats the diffusion of hydrogen atoms in the ASW and sequential hydrogenation of the CO to methanol that accounts for the observations.

  3. Doppler spectroscopy of hydrogen atoms from the photodissociation of saturated hydrocarbons and methyl halides at 157 nm

    SciTech Connect

    Tonokura, K.; Matsumi, Y.; Kawasaki, M. ); Kasatani, K. )

    1991-10-01

    Hydrocarbons (C{sub {ital n}}H{sub 2{ital n}+2}, {ital n}=3, 4, and 6) and methyl halides (CH{sub 3}{ital X}, {ital X}=Cl, Br, I) are photodissociated at 157 nm. The hydrogen atom photofragments are detected by a resonance-enhanced multiphoton ionization technique. The Doppler profiles of the hydrogen atoms from hydrocarbons are well represented by a Gaussian profile, while those from methyl halides by a mixture of a Gaussian and a non-Gaussian profiles. These Doppler profiles are interpreted assuming that (a) hot ethyl photofragments from hydrocarbons result in the formation of hydrogen atoms and (b) methyl halides undergo both direct and indirect photolytic scissions of the C---H bonds at 157 nm.

  4. The distribution of atomic hydrogen and oxygen in the magnetosphere of Saturn

    NASA Astrophysics Data System (ADS)

    Melin, Henrik; Shemansky, Don E.; Liu, Xianming

    2009-12-01

    The intensity of H Ly α1216A˚ ( 2P- 1S) and OI 1304A˚ ( 2p33s3S-2p4P) is mapped in the magnetosphere of Saturn using the ultraviolet imaging spectrograph (UVIS) [Esposito, L.W., Barth, C.A., Colwell, J.E., Lawrence, G.M., McClintock, W.E., Stewart, A.I.F., Keller, H.U., Korth, A., Lauche, H., Festou, M.C., Lane, A.L., Hansen, C.J., Maki, J.N., West, R.A., Jahn, H., Reulke, R., Warlich, K., Shemansky, D.E., Yung, Y.L., 2004. The Cassini ultraviolet imaging spectrograph investigation. Space Science Reviews 115, 299-361] onboard Cassini. Spatial coverage is built up by stepping the slit sequentially across the system (system scan). Data are obtained at a large range of space-craft-Saturn distances. The observed atomic hydrogen distribution is very broad, extending beyond 40RS in the equatorial plane, with the intensity increasing with decreasing distances to Saturn. The distribution displays persistent local-time asymmetries, and is seen connecting continuously to the upper atmosphere of the planet at sub-solar latitudes located well outside of the equatorial (ring) plane. This is consistent with the source of the atomic hydrogen being located at the top of the atmosphere on the sun-lit side of the planet on the southern hemisphere. In addition there are a number of temporally persistent features in the intensity distribution, indicating a complex hydrogen energy distribution. The emission from OI 1304A˚ is generally distributed as a broad torus centered around ˜4RS although the position of the peak intensity can vary by as much as ±1RS. There is significant intensity present out to ±10RS. HST observations of hydroxyl (OH) are re-analyzed and display a distribution half as broad as that of oxygen, also centered at 4RS. The observed atomic oxygen distribution requires a sourcing of 1.3×1028atomss-1 against loss due to charge capture with the plasma. Using the ion partitioning of Schippers et al. [2008. Multi-instrument analysis of electron populations in Saturn

  5. Effect of hydrogen atoms on the structures of trinuclear metal carbonyl clusters: trinuclear manganese carbonyl hydrides.

    PubMed

    Liu, Xian-mei; Wang, Chao-yang; Li, Qian-shu; Xie, Yaoming; King, R Bruce; Schaefer, Henry F

    2009-05-18

    The structures of the trinuclear manganese carbonyl hydrides H(3)Mn(3)(CO)(n) (n = 12, 11, 10, 9) have been investigated by density functional theory (DFT). Optimization of H(3)Mn(3)(CO)(12) gives the experimentally known structure in which all carbonyl groups are terminal and each edge of a central Mn(3) equilateral triangle is bridged by a single hydrogen atom. This structure establishes the canonical distance 3.11 A for the Mn-Mn single bond satisfying the 18-electron rule. The central triangular (mu-H)(3)Mn(3) unit is retained in the lowest energy structure of H(3)Mn(3)(CO)(11), which may thus be derived from the H(3)Mn(3)(CO)(12) structure by removal of a carbonyl group with concurrent conversion of one of the remaining carbonyl groups into a semibridging carbonyl group to fill the resulting hole. The potential energy surface of H(3)Mn(3)(CO)(10) is relatively complicated with six singlet and five triplet structures. One of the lower energy H(3)Mn(3)(CO)(10) structures has one of the hydrogen atoms bridging the entire Mn(3) triangle and the other two hydrogen atoms bridging Mn-Mn edges. This H(3)Mn(3)(CO)(10) structure achieves the favored 18-electron configuration with a very short MnMn triple bond of 2.36 A. The other low energy H(3)Mn(3)(CO)(10) structure retains the (mu-H)(3)Mn(3) core of H(3)Mn(3)(CO)(12) but has a unique six-electron donor eta(2)-mu(3) carbonyl group bridging the entire Mn(3) triangle similar to the unique carbonyl group in the known compound Cp(3)Nb(3)(CO)(6)(eta(2)-mu(3)-CO). For H(3)Mn(3)(CO)(9) a structure with a central (mu(3)-H)(2)Mn(3) trigonal bipyramid lies >20 kcal/mol below any of the other structures. Triplet structures were found for the unsaturated H(3)Mn(3)(CO)(n) (n = 11, 10, 9) systems but at significantly higher energies than the lowest lying singlet structures.

  6. The distribution of atomic hydrogen in EAGLE galaxies: morphologies, profiles, and H I holes

    NASA Astrophysics Data System (ADS)

    Bahé, Yannick M.; Crain, Robert A.; Kauffmann, Guinevere; Bower, Richard G.; Schaye, Joop; Furlong, Michelle; Lagos, Claudia; Schaller, Matthieu; Trayford, James W.; Dalla Vecchia, Claudio; Theuns, Tom

    2016-02-01

    We compare the mass and internal distribution of atomic hydrogen (H I) in 2200 present-day central galaxies with Mstar > 1010 M⊙ from the 100 Mpc EAGLE `Reference' simulation to observational data. Atomic hydrogen fractions are corrected for self-shielding using a fitting formula from radiative transfer simulations and for the presence of molecular hydrogen using an empirical or a theoretical prescription from the literature. The resulting neutral hydrogen fractions, M_{H_I+H_2} / M_star, agree with observations to better than 0.1 dex for galaxies with Mstar between 1010 and 1011 M⊙. Our fiducial, empirical H2 model based on gas pressure results in galactic H I mass fractions, M_{H I/ M_star, that agree with observations from the GASS survey to better than 0.3 dex, but the alternative theoretical H2 formula from high-resolution simulations leads to a negative offset in M_{H I}/ M_star of up to 0.5 dex. Visual inspection of mock H I images reveals that most H I discs in simulated H I-rich galaxies are vertically disturbed, plausibly due to recent accretion events. Many galaxies (up to 80 per cent) contain spuriously large H I holes, which are likely formed as a consequence of the feedback implementation in EAGLE. The H I mass-size relation of all simulated galaxies is close to (but 16 per cent steeper than) observed, and when only galaxies without large holes in the H I disc are considered, the agreement becomes excellent (better than 0.1 dex). The presence of large H I holes also makes the radial H I surface density profiles somewhat too low in the centre, at Σ _{H I} > 1 M_{⊙} pc^{-2} (by a factor of ≲ 2 compared to data from the Bluedisk survey). In the outer region (Σ _{H I} < 1 M_{⊙} pc^{-2}), the simulated profiles agree quantitatively with observations. Scaled by H I size, the simulated profiles of H I-rich (M_{H I}> 10^{9.8} M_{⊙}) and control galaxies (10^{9.1} M_{⊙}> M_{H I} > 10^{9.8} M_{⊙}) follow each other closely, as observed.

  7. Surface loss probability of atomic hydrogen for different electrode cover materials investigated in H₂-Ar low-pressure plasmas

    SciTech Connect

    Sode, M. Schwarz-Selinger, T.; Jacob, W.; Kersten, H.

    2014-07-07

    In an inductively coupled H₂-Ar plasma at a total pressure of 1.5 Pa, the influence of the electrode cover material on selected line intensities of H, H₂, and Ar are determined by optical emission spectroscopy and actinometry for the electrode cover materials stainless steel, copper, tungsten, Macor{sup ®}, and aluminum. Hydrogen dissociation degrees for the considered conditions are determined experimentally from the measured emission intensity ratios. The surface loss probability β{sub H} of atomic hydrogen is correlated with the measured line intensities, and β{sub H} values are determined for the considered materials. Without the knowledge of the atomic hydrogen temperature, β{sub H} cannot be determined exactly. However, ratios of β{sub H} values for different surface materials are in first order approximation independent of the atomic hydrogen temperature. Our results show that β{sub H} of copper is equal to the value of stainless steel, β{sub H} of Macor{sup ®} and tungsten is about 2 times smaller and β{sub H} of aluminum about 5 times smaller compared with stainless steel. The latter ratio is in reasonable agreement with literature. The influence of the atomic hydrogen temperature T{sub H} on the absolute value is thoroughly discussed. For our assumption of T{sub H}=600 K, we determine a β{sub H} for stainless steel of 0.39±0.13.

  8. Excitation and charge transfer in low-energy hydrogen-atom collisions with neutral atoms: Theory, comparisons, and application to Ca

    NASA Astrophysics Data System (ADS)

    Barklem, Paul S.

    2016-04-01

    A theoretical method is presented for the estimation of cross sections and rates for excitation and charge-transfer processes in low-energy hydrogen-atom collisions with neutral atoms, based on an asymptotic two-electron model of ionic-covalent interactions in the neutral atom-hydrogen-atom system. The calculation of potentials and nonadiabatic radial couplings using the method is demonstrated. The potentials are used together with the multichannel Landau-Zener model to calculate cross sections and rate coefficients. The main feature of the method is that it employs asymptotically exact atomic wave functions, which can be determined from known atomic parameters. The method is applied to Li+H , Na+H , and Mg+H collisions, and the results compare well with existing detailed full-quantum calculations. The method is applied to the astrophysically important problem of Ca+H collisions, and rate coefficients are calculated for temperatures in the range 1000-20 000 K.

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

    PubMed

    Cao, Xinrui; Fu, Qiang; Luo, Yi

    2014-05-14

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

  10. A comprehensive study on atomic layer deposition of molybdenum sulfide for electrochemical hydrogen evolution

    NASA Astrophysics Data System (ADS)

    Kwon, Do Hyun; Jin, Zhenyu; Shin, Seokhee; Lee, Wook-Seong; Min, Yo-Sep

    2016-03-01

    Atomic layer deposition (ALD) has emerged as an efficient method to design and prepare catalysts with atomic precision. Here, we report a comprehensive study on ALD of molybdenum sulfide (MoSx) for an electrocatalytic hydrogen evolution reaction. By using molybdenum hexacarbonyl and dimethyldisulfide as the precursors of Mo and S, respectively, the MoSx catalysts are grown at 100 °C on porous carbon fiber papers (CFPs). The ALD process results in the growth of particle-like MoSx on the CFP due to the lack of adsorption sites, and its crystallographic structure is a mixture of amorphous and nano-crystalline phases. In order to unveil the intrinsic activity of the ALD-MoSx, the exchange current densities, Tafel slopes, and turnover frequencies of the catalysts grown under various ALD conditions have been investigated by considering the fractional surface coverage of MoSx on the CFP and catalytically-active surface area. In addition, the ALD-MoSx/CFP catalysts exhibit excellent catalytic stability due to the strong adhesion of MoSx on the CFP and the mixed phase.Atomic layer deposition (ALD) has emerged as an efficient method to design and prepare catalysts with atomic precision. Here, we report a comprehensive study on ALD of molybdenum sulfide (MoSx) for an electrocatalytic hydrogen evolution reaction. By using molybdenum hexacarbonyl and dimethyldisulfide as the precursors of Mo and S, respectively, the MoSx catalysts are grown at 100 °C on porous carbon fiber papers (CFPs). The ALD process results in the growth of particle-like MoSx on the CFP due to the lack of adsorption sites, and its crystallographic structure is a mixture of amorphous and nano-crystalline phases. In order to unveil the intrinsic activity of the ALD-MoSx, the exchange current densities, Tafel slopes, and turnover frequencies of the catalysts grown under various ALD conditions have been investigated by considering the fractional surface coverage of MoSx on the CFP and catalytically

  11. Relativistic electronic dressing in laser-assisted ionization of atomic hydrogen by electron impact

    SciTech Connect

    Attaourti, Y.; Taj, S.

    2004-06-01

    Within the framework of the coplanar binary geometry where it is justified to use plane wave solutions for the study of the (e,2e) reaction and in the presence of a circularly polarized laser field, we introduce as a first step the Dirac-Volkov plane wave Born approximation 1 where we take into account only the relativistic dressing of the incident and scattered electrons. Then, we introduce the Dirac-Volkov plane wave Born approximation 2 where we take totally into account the relativistic dressing of the incident, scattered, and ejected electrons. We then compare the corresponding triple differential cross sections for laser-assisted ionization of atomic hydrogen by electron impact both for the nonrelativistic and the relativistic regime.

  12. Atomic layer deposition of aluminum sulfide thin films using trimethylaluminum and hydrogen sulfide

    SciTech Connect

    Sinha, Soumyadeep; Sarkar, Shaibal K.; Mahuli, Neha

    2015-01-15

    Sequential exposures of trimethylaluminum and hydrogen sulfide are used to deposit aluminum sulfide thin films by atomic layer deposition (ALD) in the temperature ranging from 100 to 200 °C. Growth rate of 1.3 Å per ALD cycle is achieved by in-situ quartz crystal microbalance measurements. It is found that the growth rate per ALD cycle is highly dependent on the purging time between the two precursors. Increased purge time results in higher growth rate. Surface limited chemistry during each ALD half cycle is studied by in-situ Fourier transformed infrared vibration spectroscopy. Time of flight secondary ion-mass spectroscopy measurement is used to confirm elemental composition of the deposited films.

  13. Bose-Einstein condensation and heat capacity of two-dimensional spin-polarized atomic hydrogen

    SciTech Connect

    Al-Sugheir, M. K.; Ghassib, H. B.; Awawdeh, M.

    2011-07-15

    The static fluctuation approximation (SFA) is used to study the condensate fraction and the specific heat capacity of finite two-dimensional spin-polarized atomic hydrogen. It is found that Bose-Einstein condensation occurs in this system. The transition temperature at different densities decreases as the number of particles of the system increases. At low density, a sharp peak in the specific heat capacity is observed at the transition temperature. On the other hand, as the density of the system increases, the transition temperature becomes no longer well-defined, and a hump is observed in the specific heat capacity around the transition temperature. A qualitative comparison of our results to published results for finite Bose systems shows good agreement.

  14. Method of producing a storage bulb for an atomic hydrogen maser

    NASA Technical Reports Server (NTRS)

    Erpenbach, H. (Inventor)

    1975-01-01

    A storage bulb for an atomic hydrogen maser is produced by coating its internal surface with an emulsion containing both TFE and FEP particles. The emulsion is produced by mixing a first quantity of TFE in an aqueous dispersion with a second quantity of FEP in an aqueous dispersion, with a third quantity of distilled water. The emulsion is poured into the bulb to coat it uniformly so as to form a thin film of emulsion on the bulb's internal surface. After excess emulsion is drained out of the bulb the emulsion in the bulb is dried to remove the water and most of the aqueous matter therefrom. The remaining emulsion is then cured by heating the bulb to a temperature of at least 380 C.

  15. Circular Rydberg States of the Hydrogen Atom in a Magnetic Field

    SciTech Connect

    Germann, T.C.; Herschbach, D.R. ); Dunn, M.; Watson, D.K. )

    1995-01-30

    Dimensional perturbation theory is used to study circular Rydberg states ([vert bar][ital m][vert bar]=[ital n][minus]1[much gt]1) and other large [vert bar][ital m][vert bar] states of the hydrogen atom in a uniform magnetic field. Because of a degeneracy between states of increased angular momentum and states of increased Cartesian dimensionality, the accuracy of the zeroth-order [ital D][r arrow][infinity] limit and a dimensional perturbation expansion improves significantly for states with larger [vert bar][ital m][vert bar]. In contrast to other approaches, this method is applicable to the entire range of magnetic field strengths. Energies and expectation values are presented as functions of the field strength.

  16. Reaction of an Iron(IV) Nitrido Complex with Cyclohexadienes: Cycloaddition and Hydrogen-Atom Abstraction

    PubMed Central

    2015-01-01

    The iron(IV) nitrido complex PhB(MesIm)3Fe≡N reacts with 1,3-cyclohexadiene to yield the iron(II) pyrrolide complex PhB(MesIm)3Fe(η5-C4H4N) in high yield. The mechanism of product formation is proposed to involve sequential [4 + 1] cycloaddition and retro Diels–Alder reactions. Surprisingly, reaction with 1,4-cyclohexadiene yields the same iron-containing product, albeit in substantially lower yield. The proposed reaction mechanism, supported by electronic structure calculations, involves hydrogen-atom abstraction from 1,4-cyclohexadiene to provide the cyclohexadienyl radical. This radical is an intermediate in substrate isomerization to 1,3-cyclohexadiene, leading to formation of the pyrrolide product. PMID:25068927

  17. Positronium formation in the n = 2 level in positron scattering from hydrogen and helium atoms

    SciTech Connect

    Khan, P.; Mazumdar, P.S.; Ghosh, A.S.

    1985-03-01

    A distorted-wave model (Phys. Rev. A 27, 1904 (1983); 28, 2180 (1983)) is applied to calculate the formation of positronium in the n = 2 states in e/sup +/ scattering from hydrogen and helium atoms. The incident wave is represented by a polarized-orbital method. The first-Born-approximation results of the 2p-excited-state capture cross section in the case of helium is reported for the first time. The first Born approximation is found to be unsuitable for prediction of the rearrangement processes. The present total (ground- and excited-state) positronium-formation cross sections have been compared with the corresponding observed values of Fornari et al. (Phys. Rev. Lett. 51, 2276 (1983)) and of Charlton et al. (J. Phys. B 16, L465 (1983)).

  18. Long term variations and solar variability of atomic oxygen and hydrogen in the mesosphere / lower thermosphere

    NASA Astrophysics Data System (ADS)

    Ern, Manfred; Kaufmann, Martin; Lehmann, Catrin; Riese, Martin; Smith, Anne; Marsh, Daniel

    Global measurements of the hydroxyl mesospheric airglow as observed by the SCIAMACHY satellite instrument are presented. SCIAMACHY is mounted on ESA's Envisat launched in March 2002 into a polar, sun-synchronous orbit with an inclination of 98.7deg and an ascending node at 22:00 local solar time. Limb observations on the night side cover about 70 degrees in terms of latitude during each orbit, covering 30S-70N, depending on season. Based on these measurements altitude profiles of atomic oxygen and hydrogen are retrieved by means of an OH non-LTE model. These data are analyzed with respect to solar illumination conditions and global wave activity. A windowed space-time Fourier analysis is carried out to investigate seasonal changes in mesopause wave activity. First comparisons with simulations of the NCAR ROSE model are shown.

  19. Chemical reactivity of hydrogen, nitrogen, and oxygen atoms at temperatures below 100 k

    NASA Technical Reports Server (NTRS)

    Mcgee, H. A., Jr.

    1973-01-01

    The synthesis of unusual compounds by techniques employing cryogenic cooling to retard their very extreme reactivity was investigated. Examples of such species that were studied are diimide (N2H2), cyclobutadiene (C4H4), cyclopropanone (C3H4O), oxirene (C2H2O), and many others. Special purpose cryogenically cooled inlet arrangements were designed such that the analyses incurred no warm-up of the cold, and frequently explosively unstable, compounds. Controlled energy electron impact techniques were used to measure critical potentials and to develop the molecular energetics and thermodynamics of these molecules and to gain some insight into their kinetic characteristics as well. Three and four carbon strained ring molecules were studied. Several reactions of oxygen and hydrogen atoms with simple molecules of H, N, C, and O in hard quench configurations were studied. And the quench stabilization of BH3 was explored as a model system in cryochemistry.

  20. Calculation of the total and total ionization cross sections for positron scattering on atomic hydrogen

    SciTech Connect

    Bray, I. ); Stelbovics, A.T. )

    1994-04-01

    The total and total ionization cross sections for positron scattering on atomic hydrogen are calculated by applying the convergent-close-coupling method to the model where positronium-formation channels are omitted. This model accurately describes the physics of the scattering whenever the positronium formation cross section is negligible, in particular, above 100 eV for this system. The total ionization cross section results in this energy region are in excellent agreement with the recent measurements of Jones [ital et] [ital al]. [J. Phys. B 26, L483 (1993)], and so lie below the earlier measurements of Spicher [Phys. Rev. Lett. 64, 1019 (1990)], and the recent calculations of Acacia [ital et] [ital al]. [Phys. Rev. Lett. (to be published)]. The total cross section is in very good agreement with the recent measurements of Zhou [ital et] [ital al]. (unpublished) down to 30 eV.

  1. Experiments on continuum electron capture in atomic hydrogen and collisional interaction of trapped ions. Progress report

    SciTech Connect

    Sellin, I.A.; Elston, S.B.

    1981-01-01

    This section describes the background and scope of as well as progress made on experiments designed to test the present theory of charge exchange to continuum for the case of bare nuclei on atomic hydrogen. The charge transfer process is well known to be an essential ingredient of any attempt to understand the ionization of gaseous media traversed by highly-charged energetic ions. Surprisingly, a sometimes dominant contribution to such ionization remained undiscovered until the past decade. This process, known as charge transfer to the continuum, involves the ionization of electrons from the target species into unbound states closely matched in exit direction and speed to the charged particles which generate them. Subsequent measurements of the resultant forward electron production, performed by University of Tennessee searchers at Oak Ridge and Brookhaven National Laboratories, were unique in employing more highly charged projectiles than previously.

  2. Design of an atomic layer deposition reactor for hydrogen sulfide compatibility

    NASA Astrophysics Data System (ADS)

    Dasgupta, Neil P.; Mack, James F.; Langston, Michael C.; Bousetta, Al; Prinz, Fritz B.

    2010-04-01

    A customized atomic layer deposition (ALD) reactor was designed with components compatible with hydrogen sulfide (H2S) chemistry. H2S is used as a reactant for the ALD of metal sulfides. The use of H2S in an ALD reactor requires special attention to safety issues due to its highly toxic, flammable, and corrosive nature. The reactor was designed with respect to materials compatibility of all wetted components with H2S. A customized safety interlock system was developed to shut down the system in the event of toxic gas leakage, power outage, loss of building ventilation or compressed air pressure. ALD of lead sulfide (PbS) and zinc sulfide (ZnS) were demonstrated with no chemical contamination or detectable release of H2S.

  3. Rate of reaction of the hydrogen atom with nitrous oxide in ambient water

    NASA Astrophysics Data System (ADS)

    Kazmierczak, Lukasz; Swiatla-Wojcik, Dorota; Szala-Bilnik, Joanna; Wolszczak, Marian

    2016-08-01

    The reaction of the hydrogen atom with nitrous oxide has been investigated by pulse radiolysis of N2O-saturated 0.1 M HCl solution at room temperature (24±1 °C). The value of (9±2)×104 M-1 s-1 obtained for the reaction rate constant is between the early estimates 1×104 M-1 s-1 by Czapski and Jortner (1960) and 4.3×105 M-1 s-1 by Thomas (1969), and is much lower than 2×106 M-1 s-1 used recently (Janik et al., 2007; Ismail et al., 2013; Liu et al., 2015; Meesungnoen et al., 2015).

  4. Atomic Hydrogen as High-Precision Field Standard for High-Field EPR

    PubMed Central

    Stoll, Stefan; Ozarowski, Andrew; Britt, R. David; Angerhofer, Alexander

    2010-01-01

    We introduce atomic hydrogen trapped in an octaisobutylsilsesquioxane nanocage (H@iBuT8) as a new molecular high-precision magnetic field standard for high-field EPR spectroscopy of organic radicals and other systems with signals around g = 2. Its solid-state EPR spectrum consists of two narrow lines separated by about 51 mT and centered at g ≈ 2. The isotropic g factor is 2.00294(3) and essentially temperature independent. The isotopic 1H hyperfine coupling constant is 1416.8(2) MHz below 70 K and decreases slightly with increasing temperature to 1413.7(1) MHz at room temperature. The spectrum of the standard does not overlap with those of most organic radicals, and it can be easily prepared and is stable at room temperature. PMID:20813570

  5. Absolute rate constants for the reaction of atomic hydrogen with ketene from 298 to 500 K

    NASA Technical Reports Server (NTRS)

    Michael, J. V.; Nava, D. F.; Payne, W. A.; Stief, L. J.

    1979-01-01

    Rate constants for the reaction of atomic hydrogen with ketene have been measured at room temperature by two techniques, flash photolysis-resonance fluorescence and discharge flow-resonance fluorescence. The measured values are (6.19 + or - 1.68) x 10 to the -14th and (7.3 + or - 1.3) x 10 to the -14th cu cm/molecule/s, respectively. In addition, rate constants as a function of temperature have been measured over the range 298-500 K using the FP-RF technique. The results are best represented by the Arrhenius expression k = (1.88 + or - 1.12) x 10 to the -11th exp(-1725 + or - 190/T) cu cm/molecule/s, where the indicated errors are at the two standard deviation level.

  6. Absolute rate constant of the reaction between chlorine /2P/ atoms and hydrogen peroxide from 298 to 424 K

    NASA Technical Reports Server (NTRS)

    Keyser, L. F.

    1980-01-01

    The absolute rate constant of the reaction between chlorine (2P) atoms and hydrogen peroxide was determined from 298 to 424 K, using the discharge flow resonance fluorescence technique. Pseudo-first-order conditions were used with hydrogen peroxide in large excess. A fast flow-sampling procedure limited hydrogen peroxide decomposition to less than 5% over the temperature range studied. At 298 K, the rate constant is (4.1 plus or minus 0.2) x 10 to the minus 13th cu cm/molecule-sec.

  7. Effectiveness of the statistical potential in the description of fermions in a worm-algorithm path-integral Monte Carlo simulation of 3He atoms placed on a 4He layer adsorbed on graphite.

    PubMed

    Ghassib, Humam B; Sakhel, Asaad R; Obeidat, Omar; Al-Oqali, Amer; Sakhel, Roger R

    2012-01-01

    We demonstrate the effectiveness of a statistical potential (SP) in the description of fermions in a worm-algorithm path-integral Monte Carlo simulation of a few 3He atoms floating on a 4He layer adsorbed on graphite. The SP in this work yields successful results, as manifested by the clusterization of 3He, and by the observation that the 3He atoms float on the surface of 4He. We display the positions of the particles in 3D coordinate space, which reveal clusterization of the 3He component. The correlation functions are also presented, which give further evidence for the clusterization.

  8. Low temperature removal of surface oxides and hydrocarbons from Ge(100) using atomic hydrogen

    NASA Astrophysics Data System (ADS)

    Walker, M.; Tedder, M. S.; Palmer, J. D.; Mudd, J. J.; McConville, C. F.

    2016-08-01

    Germanium is a group IV semiconductor with many current and potential applications in the modern semiconductor industry. Key to expanding the use of Ge is a reliable method for the removal of surface contamination, including oxides which are naturally formed during the exposure of Ge thin films to atmospheric conditions. A process for achieving this task at lower temperatures would be highly advantageous, where the underlying device architecture will not diffuse through the Ge film while also avoiding electronic damage induced by ion irradiation. Atomic hydrogen cleaning (AHC) offers a low-temperature, damage-free alternative to the common ion bombardment and annealing (IBA) technique which is widely employed. In this work, we demonstrate with X-ray photoelectron spectroscopy (XPS) that the AHC method is effective in removing surface oxides and hydrocarbons, yielding an almost completely clean surface when the AHC is conducted at a temperature of 250 °C. We compare the post-AHC cleanliness and (2 × 1) low energy electron diffraction (LEED) pattern to that obtained via IBA, where the sample is annealed at 600 °C. We also demonstrate that the combination of a sample temperature of 250 °C and atomic H dosing is required to clean the surface. Lower temperatures prove less effective in removal of the oxide layer and hydrocarbons, whilst annealing in ultra-high vacuum conditions only removes weakly bound hydrocarbons. Finally, we examine the subsequent H-termination of an IBA-cleaned sample using XPS, LEED and ultraviolet photoelectron spectroscopy (UPS) in order to examine changes in the work function of Ge(100) upon hydrogenation.

  9. Atomic hydrogen in the mesopause region derived from SABER: Algorithm theoretical basis, measurement uncertainty, and results

    NASA Astrophysics Data System (ADS)

    Mlynczak, Martin G.; Hunt, Linda A.; Marshall, B. Thomas; Mertens, Christopher J.; Marsh, Daniel R.; Smith, Anne K.; Russell, James M.; Siskind, David E.; Gordley, Larry L.

    2014-03-01

    Atomic hydrogen (H) is a fundamental component in the photochemistry and energy balance of the terrestrial mesopause region (80-100 km). H is generated primarily by photolysis of water vapor and participates in a highly exothermic reaction with ozone. This reaction is a significant source of heat in the mesopause region and also creates highly vibrationally excited hydroxyl (OH) from which the Meinel band radiative emission features originate. Concentrations (cm-3) and volume mixing ratios of H are derived from observations of infrared emission from the OH (υ = 9 + 8, Δυ = 2) vibration-rotation bands near 2.0 µm made by the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) instrument on the NASA Thermosphere Ionosphere Mesosphere Energetics and Dynamics satellite. The algorithms for deriving day and night H are described herein. Day and night concentrations exhibit excellent agreement between 87 and 95 km. SABER H results also exhibit good agreement with observations from the Solar Mesosphere Explorer made nearly 30 years ago. An apparent inverse dependence on the solar cycle is observed in the SABER H concentrations, with the H increasing as solar activity decreases. This increase is shown to be primarily due to the temperature dependence of various reaction rate coefficients for H photochemistry. The SABER H data, coupled with SABER atomic oxygen, ozone, and temperature, enable tests of mesospheric photochemistry and energetics in atmospheric models, studies of formation of polar mesospheric clouds, and studies of atmospheric evolution via escape of hydrogen. These data and studies are made possible by the wide range of parameters measured simultaneously by the SABER instrument.

  10. Predicting organic hydrogen atom transfer rate constants using the Marcus cross relation

    PubMed Central

    Warren, Jeffrey J.; Mayer, James M.

    2010-01-01

    Chemical reactions that involve net hydrogen atom transfer (HAT) are ubiquitous in chemistry and biology, from the action of antioxidants to industrial and metalloenzyme catalysis. This report develops and validates a procedure to predict rate constants for HAT reactions of oxyl radicals (RO•) in various media. Our procedure uses the Marcus cross relation (CR) and includes adjustments for solvent hydrogen-bonding effects on both the kinetics and thermodynamics of the reactions. Kinetic solvent effects (KSEs) are included by using Ingold’s model, and thermodynamic solvent effects are accounted for by using an empirical model developed by Abraham. These adjustments are shown to be critical to the success of our combined model, referred to as the CR/KSE model. As an initial test of the CR/KSE model we measured self-exchange and cross rate constants in different solvents for reactions of the 2,4,6-tri-tert-butylphenoxyl radical and the hydroxylamine 2,2′-6,6′-tetramethyl-piperidin-1-ol. Excellent agreement is observed between the calculated and directly determined cross rate constants. We then extend the model to over 30 known HAT reactions of oxyl radicals with OH or CH bonds, including biologically relevant reactions of ascorbate, peroxyl radicals, and α-tocopherol. The CR/KSE model shows remarkable predictive power, predicting rate constants to within a factor of 5 for almost all of the surveyed HAT reactions. PMID:20215463

  11. Hybrid Modeling of Hydrogen Energetic Neutral Atoms from Mars: Emission from Subsolar Magnetosheath

    NASA Astrophysics Data System (ADS)

    Wang, Xiao-Dong; Kallio, Esa; Barabash, Stas; Futaana, Yoshifumi

    2015-04-01

    We simulated the hydrogen energetic neutral atom (ENA) emission from the subsolar magnetosheath of Mars using a hybrid scheme in order to reproduce multiple features of the statistical features obtained from statistical observations of the Neutral Particle Detectors on the Mars Express spacecraft. We track the charge exchange reaction between the ions produced by the hybrid plasma model under a Martian neutral exosphere model. The simulation exhibits a directional emission of hydrogen ENAs from dayside magnetosheath. Particularly, the stronger ENA emission in the opposite direction of the solar wind convection electric field is reproduced, being consistent with the observations, by a corresponding asymmetry in the proton flux at the lower magnetosheath. This proton flux asymmetry is caused by the mass loading of ionospheric heavy ions in the direction of the convection electric field. We also investigate the influences of the upstream solar wind dynamic pressure. We demonstrate that higher dynamic pressure causes stronger and more anisotropic ENA emission, besides the influence of the proton flux. This dependence suggests that the induced magnetic boundary is lower during higher dynamic pressure, where the sheath protons can access to a denser exosphere and thus the charge exchange rate is higher.

  12. Intermolecular and intramolecular hydrogen bonds involving fluorine atoms: implications for recognition, selectivity, and chemical properties.

    PubMed

    Dalvit, Claudio; Vulpetti, Anna

    2012-02-01

    A correlation between 19F NMR isotropic chemical shift and close intermolecular F⋅⋅⋅H-X contacts (with X=N or O) has been identified upon analysis of the X-ray crystal structures of fluorinated molecules listed in the Cambridge Structural Database (CSD). An optimal F⋅⋅⋅X distance involving primary and shielded secondary fluorine atoms in hydrogen-bond formation along with a correlation between F⋅⋅⋅H distance and F⋅⋅⋅H-X angle were also derived from the analysis. The hydrogen bonds involving fluorine are relevant, not only for the recognition mechanism and stabilization of a preferred conformation, but also for improvement in the permeability of the molecules, as shown with examples taken from a proprietary database. Results of an analysis of the small number of fluorine-containing natural products listed in the Protein Data Bank (PDB) appear to strengthen the derived correlation between 19F NMR isotropic chemical shift and interactions involving fluorine (also known as the "rule of shielding") and provides a hypothesis for the recognition mechanism and catalytic activity of specific enzymes. Novel chemical scaffolds, based on the rule of shielding, have been designed for recognizing distinct structural motifs present in proteins. It is envisaged that this approach could find useful applications in drug design for the efficient optimization of chemical fragments or promising compounds by increasing potency and selectivity against the desired biomolecular target.

  13. Formation of hydrogen atom in 2s state in proton-sodium inelastic scattering

    NASA Astrophysics Data System (ADS)

    Sabbah, A. Elkilany

    2015-03-01

    The inelastic collision of protons with sodium atoms are treated for the first time within the framework of the coupled-static and frozen core approximations. The method is used for calculating partial and total cross-sections with the assumption that only two channels (elastic and hydrogen formation in 2s state) are open. In each case, the calculations are carried out for seven values of the total angular momentum ℓ(0 ≤ ℓ ≤ 6). The target is described using the Clementi Roetti wave functions within the framework of the one valence electron model. We use Lipmann-Swinger equation to solve the derived equations of the problem, then apply an iterative numerical method to obtain the code of computer to calculate iterative partial cross-sections. This can be done through calculating the reactance matrix at different values of considered energies to obtain the transition matrix that gives partial and total cross sections. The present results for total hydrogen (2s state) formation cross sections are in agreement with results of other available ones in wide range of incident energy.

  14. The elimination of a hydrogen atom in Na(H2O)n

    NASA Astrophysics Data System (ADS)

    Chan, Ka Wai; Siu, Chi-Kit; Wong, S. Y.; Liu, Zhi-Feng

    2005-09-01

    By a systematic examination on Na(H2O)n, with n =4-7, 9, 10, and 15, we demonstrate that a hydrogen loss reaction can be initiated by a single sodium atom with water molecules. This reaction is similar to the well-known size-dependent intracluster hydrogen loss in Mg+(H2O)n, which is isoelectronic to Na(H2O)n. However, with one less charge on Na(H2O)n than that on Mg+(H2O)n, the hydrogen loss for Na(H2O)n is characterized by a higher barrier and a more flexible solvation shell around the metal ion, although the reaction should be accessible, as the lowest barrier is around 8kcal/mol. Interestingly, the hydroxide ion OH- produced in the process is stabilized by the solvation of H2O molecules and the formation of an ion pair Na+(H2O)4(H2O)n-l-4[OH-(H2O)l]. The activation barrier is reduced as the unpaired electron in Na(H2O)n moves to higher solvation shells with increasing cluster size, and the reaction is not switched off for larger clusters. This is in sharp contrast to the reaction for Mg+(H2O)n, in which the OH- ion is stabilized by direct coordination with Mg2+ and the reaction is switched off for n >17, as the unpaired electron moved to higher solvation shells. Such a contrast illustrates the important link between microsolvation environment and chemical reactivity in solvation clusters.

  15. Partial redistribution in multilevel atoms. I. Method and application to the solar hydrogen line formation

    SciTech Connect

    Hubeny, I.

    1995-12-01

    We present a robust method for solution of multilevel non-LTE line transfer problems including the effects of partial frequency redistribution (PRD). This method allows the self-consistent solution for redistribution of scattered line photons simultaneously in multiple transitions of a model atom, including the effects of resonant Raman scattering ({open_quote}{open_quote}cross-redistribution{close_quote}{close_quote}) among lines sharing common upper levels. The method is incorporated into the framework of the widely used non-LTE complete redistribution code MULTI. We have applied this method to the problem of transfer in hydrogen lines in a plane-parallel solar model atmosphere, including cross-redistribution between the H{alpha} and L{beta}, using general redistribution functions for the L{alpha} and L{beta} lines which are not restricted by the impact approximation. The convergence properties of this method are demonstrated to be comparable to that of the equivalent complete redistribution problem. In this solar model, PRD in the L{alpha} line produces the dominant influence on the level populations. It changes considerably the populations of the excited states of hydrogen, as well as the proton number density, in the middle and upper chromosphere, owing to modification of the L{alpha} wing radiation. The population of the hydrogen ground state undergoes only modest changes, however. The influence of cross-redistribution and PRD in L{beta} has a much smaller influence on the level populations but a considerable influence on the wing intensity of the L{beta} line. {copyright} {ital 1995 The American Astronomical Society.}

  16. Stable path to ferromagnetic hydrogenated graphene growth

    NASA Astrophysics Data System (ADS)

    Hemmatiyan, Shayan; Polini, Marco; Abanov, Artem; MacDonald, Allan H.; Sinova, Jairo

    2014-07-01

    In this paper, we propose a practical way to stabilize half-hydrogenated graphene (graphone). We show that the dipole moments induced by a hexagonal-boron nitride (h-BN) substrate on graphene stabilize the hydrogen atoms on one sublattice of the graphene layer and suppress the migration of the adsorbed hydrogen atoms. Based upon first principle spin polarized density of states calculations, we show that the graphone obtained in different graphene/h-BN heterostructures exhibits a half metallic state. We propose to use this exotic material for spin valve systems and other spintronics devices.

  17. A comprehensive study on atomic layer deposition of molybdenum sulfide for electrochemical hydrogen evolution.

    PubMed

    Kwon, Do Hyun; Jin, Zhenyu; Shin, Seokhee; Lee, Wook-Seong; Min, Yo-Sep

    2016-04-01

    Atomic layer deposition (ALD) has emerged as an efficient method to design and prepare catalysts with atomic precision. Here, we report a comprehensive study on ALD of molybdenum sulfide (MoSx) for an electrocatalytic hydrogen evolution reaction. By using molybdenum hexacarbonyl and dimethyldisulfide as the precursors of Mo and S, respectively, the MoSx catalysts are grown at 100 °C on porous carbon fiber papers (CFPs). The ALD process results in the growth of particle-like MoSx on the CFP due to the lack of adsorption sites, and its crystallographic structure is a mixture of amorphous and nano-crystalline phases. In order to unveil the intrinsic activity of the ALD-MoSx, the exchange current densities, Tafel slopes, and turnover frequencies of the catalysts grown under various ALD conditions have been investigated by considering the fractional surface coverage of MoSx on the CFP and catalytically-active surface area. In addition, the ALD-MoSx/CFP catalysts exhibit excellent catalytic stability due to the strong adhesion of MoSx on the CFP and the mixed phase. PMID:26973254

  18. Atomic layer deposition of magnesium fluoride via bis(ethylcyclopentadienyl)magnesium and anhydrous hydrogen fluoride

    SciTech Connect

    Hennessy, John Jewell, April D.; Greer, Frank; Lee, Michael C.; Nikzad, Shouleh

    2015-01-15

    A new process has been developed to deposit magnesium fluoride (MgF{sub 2}) thin films via atomic layer deposition (ALD) for use as optical coatings in the ultraviolet. MgF{sub 2} was deposited in a showerhead style ALD reactor using bis(ethylcyclopentadienyl)magnesium and anhydrous hydrogen fluoride (HF) as precursors at substrate temperatures from 100 to 250 °C. The use of HF was observed to result in improved morphology and reduced impurity content compared to other reported MgF{sub 2} ALD approaches that use metal fluoride precursors as the fluorine-containing chemistry. Characterization of these films has been performed using spectroscopic ellipsometry, atomic force microscopy, and x-ray photoelectron spectroscopy for material deposited on silicon substrates. Films at all substrate temperatures were transparent at wavelengths down to 190 nm and the low deposition temperature combined with low surface roughness makes these coatings good candidates for a variety of optical applications in the far ultraviolet.

  19. Nonresonant corrections for the optical resonance frequency measurements in the hydrogen atom

    SciTech Connect

    Labzowsky, Leonti; Schedrin, Gavriil; Solovyev, Dmitrii; Chernovskaya, Evgenia; Plunien, Guenter; Karshenboim, Savely

    2009-05-15

    The deviation of the natural spectral line profile from the Lorentz shape for the optical resonant frequency measurements is considered. This deviation leads to an asymmetry, which is mainly due to nonresonant correction to the resonant Lorentz profile. The nonresonant corrections are studied for the different types of the atomic resonant experiments. The most accurate recent optical resonance experiments are analyzed, i.e., the two-photon 1s-2s resonance excitation of the hydrogen atom with the delayed decay in the external electric field. The description of the nonresonant correction in the latter case requires the employment of QED with different in and out Hamiltonians. The nonresonant corrections for this experiment are investigated and found to be about 10{sup -5} Hz, while the recent experimental uncertainty is 34 Hz and in the near feature is expected to be a few hertz. The projected 1s-2s resonance excitation experiment with the three-photon ionization detection (which is now in progress) is also considered.

  20. Photoionization microscopy of Rydberg hydrogen atom in a non-uniform electrical field

    NASA Astrophysics Data System (ADS)

    Shao-Hao, Cheng; De-Hua, Wang; Zhao-Hang, Chen; Qiang, Chen

    2016-06-01

    In this paper, we investigate the photoionization microscopy of the Rydberg hydrogen atom in a gradient electric field for the first time. The observed oscillatory patterns in the photoionization microscopy are explained within the framework of the semiclassical theory, which can be considered as a manifestation of interference between various electron trajectories arriving at a given point on the detector plane. In contrast with the photoionization microscopy in the uniform electric field, the trajectories of the ionized electron in the gradient electric field will become chaotic. An infinite set of different electron trajectories can arrive at a given point on the detector plane, which makes the interference pattern of the electron probability density distribution extremely complicated. Our calculation results suggest that the oscillatory pattern in the electron probability density distribution depends sensitively on the electric field gradient, the scaled energy and the position of the detector plane. Through our research, we predict that the interference pattern in the electron probability density distribution can be observed in an actual photoionization microscopy experiment once the external electric field strength and the position of the electron detector plane are reasonable. This study provides some references for the future experimental research on the photoionization microscopy of the Rydberg atom in the non-uniform external fields. Project supported by the National Natural Science Foundation of China (Grant No. 11374133) and the Project of Shandong Provincial Higher Educational Science and Technology Program, China (Grant No. J13LJ04).