Library

feed icon rss

Your email was sent successfully. Check your inbox.

An error occurred while sending the email. Please try again.

Proceed reservation?

Export
  • 1
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 90 (1989), S. 2807-2815 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Molecular beam and time of flight methods have been used to examine the angular distributions and velocity distributions of the CO2 product molecules formed in the catalytic oxidation of CO on a Rh(111) single crystal in the surface temperature range 700–1000 K. The angular distribution was sharply peaked about the surface normal, and cannot be described by a simple cosn θ expression. No temperature dependence was observed in the angular distribution over the range of temperatures studied here. Observed velocity distributions were clearly non-Maxwellian and had average translational energies in excess of those expected at the surface temperatures. Furthermore, the average velocity depended strongly on the desorption angle. Molecules desorbing along the surface normal had an average translational energy of ∼8 kcal/mol. The average energy decreased with increasing angle, reaching a value of ∼4 kcal/mol at an angle of 60°. All of the observed velocity distributions were narrower than Maxwellian distributions with the same average energies. Product velocity distributions did not appear to vary with surface temperature. The observed excess energies are believed to arise from the crossing of the activation barrier to reaction, with a fraction of the reaction energy being carried away from the surface by the product molecules.
    Type of Medium: Electronic Resource
    Library Location Call Number Volume/Issue/Year Availability
    BibTip Others were also interested in ...
  • 2
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 88 (1988), S. 7975-7994 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: In this paper we report that ultraviolet laser induced desorption from the surface of a thin nitric oxide film proceeds via two mechanisms which are present simultaneously. One mechanism is attributed to laser induced thermal desorption while the other is due to a nonthermal, single photon process. A film of 1–2000 ML (layers) of NO condensed on a Ag(111) substrate under UHV conditions at 25–50 K was irradiated by 5 ns pulses of 220–270 nm laser light (4.6–5.5 eV) with 0.5–5 mJ/cm2 (0.1–1 MW/cm2 ) power density at the surface. Translational energies of desorbed molecules were measured from time-of-flight (TOF) spectra taken with a mass spectrometer, while the internal energy distribution of molecules desorbed in the nonthermal channel was determined by a (1+1) resonance enhanced multiphoton ionization (REMPI) probe. NO monomer in the 2Π3/2,1/2 electronic ground states was the only significant product. There were two distinct characteristic TOF components, which we associate with different desorption mechanisms. Each component had a different velocity and angular distribution, and their relative yields varied with laser pulse energy and NO layer thickness. Under conditions where both mechanisms gave comparable desorption yields, we obtained TOF distributions which were bimodal. A "slow'' peak with an average translational energy up to 0.06 eV was Maxwellian with temperatures between 160 and 280 K and a broad angular distribution. Yield in this peak increased strongly with layer thickness and exponentially with laser pulse energy. A "fast'' TOF peak with average energy of 0.22 eV was non-Maxwellian, with an angular distribution peaked toward normal, and yield increasing linearly with laser pulse energy. REMPI of the fast peak showed a vibrational population ratio v=3:v=2 of 0.85. A Boltzmann plot of the rotational population distribution of v=2 molecules, if fit with a single line, gave a temperature of 2500 K. We use these angular, velocity, rotational, and vibrational distributions to suggest mechanisms for the nonthermal desorption. We also discuss factors determining the relative extent of thermal and photochemical effects, which control the morphology of ablated surfaces.
    Type of Medium: Electronic Resource
    Library Location Call Number Volume/Issue/Year Availability
    BibTip Others were also interested in ...
  • 3
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 88 (1988), S. 7893-7910 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: This is the second of three papers discussing our studies of overlayers of Ar, Kr, and Xe physisorbed on Ag(111). All of these rare gases form ordered structures, which are azimuthally aligned but translationally incommensurate with the Ag substrate. In this paper, we discuss experiments in which we utilized the angle resolved time of flight of inelastically scattered 18 MeV He atoms to examine the surface dynamics of multilayer rare gas films along the Γ¯–M¯ direction. This was done on a layer-by-layer basis for 2, 3, and ≥20 layers for each of the rare gases. Unlike the monolayers, the vibrational modes observed for the multilayers show dispersion across the surface Brillouin zone, the amount of dispersion increasing with the number of adsorbed layers. These results reveal in detail how the surface dynamical properties of a thin film evolve towards those of a thick crystal as a function of increasing dimension. Lattice dynamics calculations, which utilize realistic gas phase pair potentials, reproduce the experimentally observed phonon dispersion relations quite well. We also examine the inelastic scattering probabilities and linewidths of the transitions. One of the more notable results is that the inelastic scattering probabilities vary by at most a factor of 2–3 across the entire surface Brillouin zone. Isothermal desorption measurements for the Xe overlayers are also discussed. Like the monolayer, the bilayer and trilayer exhibit nearly zeroth order desorption until ∼90% of the top layer has desorbed, where the desorption kinetics become first order.
    Type of Medium: Electronic Resource
    Library Location Call Number Volume/Issue/Year Availability
    BibTip Others were also interested in ...
  • 4
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 88 (1988), S. 7862-7892 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: This paper is the first in a series covering our experiments examining the physical properties of ordered overlayers of Ar, Kr, and Xe physisorbed on Ag(111). In this paper, we examine the desorption kinetics of the Xe monolayer/Ag(111) system. Desorption is zeroth order until ∼90% of the monolayer has desorbed, then becomes first order. We also measured the inelastic scattering of an 18 meV He beam from unconstrained monolayers of (111) oriented Ar, Kr, and Xe. The transitions are mapped across the entire surface Brillouin zone from Γ¯ to M¯. The data are dispersionless, indicating that for the measured mode the adatoms are behaving as independent Einstein oscillators. Parametrized physisorption potentials for RG–Ag(111) [RG=Ar, Kr, Xe] are constructed using these results. Inelastic scattering probabilities and linewidths are also presented. The inelastic scattering probabilities vary by at most a factor of 3 across the entire surface Brillouin zone, and are reported as a function of incident angle, final wave vector, and surface temperature. Variations in the inelastic scattering probabilities are indicative of dynamical adatom–substrate coupling. Experimental techniques which turn these dynamical couplings on or off for the same phonon energy are discussed. Limited results for clean Ag(111) are also presented. It is hoped that these measurements, on such ideal systems as ordered rare gas monolayers, will provide further impetus for developing improved theoretical treatments of inelastic single phonon scattering.
    Type of Medium: Electronic Resource
    Library Location Call Number Volume/Issue/Year Availability
    BibTip Others were also interested in ...
  • 5
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 89 (1988), S. 1163-1169 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The catalytic oxidation of carbon monoxide on a Rh(111) surface has been investigated using modulated molecular beam techniques. Reaction proceeds via a Langmuir–Hinshelwood mechanism. Under experimental conditions which provide a high coverage of oxygen adatoms and near zero coverage of adsorbed CO, an activation energy of 24.5±0.4 kcal/mol and a preexponential factor of 2±1×10−3 cm2 s−1 were obtained. The angular distribution of the product CO2 is sharply peaked toward the surface normal, and cannot be described by a simple cosnθ expression. Present results are discussed in relation to previous work on platinum and palladium surfaces.
    Type of Medium: Electronic Resource
    Library Location Call Number Volume/Issue/Year Availability
    BibTip Others were also interested in ...
  • 6
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 88 (1988), S. 7911-7941 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We describe experiments that measured the angle resolved intensity of He (Ei=18 and 66 meV) elastically scattering from the surfaces of rare gas overlayers physisorbed on Ag(111). These studies were done on a layer-by-layer basis for 1, 2, 3, and ∼25 ordered overlayers of Ar, Kr, and Xe. Two types of experiments are described. The first is diffraction, where the scattered He intensity was measured as a function of the detector angle, with the incident polar and azimuthal angles held constant. In the second type of experiment, selective adsorption, we measured the specular intensity as a function of incident angle. The purpose of these experiments was to examine the He–surface potential, to assess the relative contributions that various He–rare gas pair potentials, nonadditive multibody terms, and He–substrate interactions make to the systems studied. The experiments are compared with the results of accurate close-coupling calculations, in order to quantitatively perform these assessments. The comparisons between the selective adsorption data and scattering calculations demonstrate the extreme sensitivity that such measurements have to the He–surface potential. In particular, observable changes in the calculated selective adsorption spectra appear when different He–rare gas potentials are tested, or when various nonadditive terms are included in the potential. The results suggest that further refinements in the He-heavy–rare gas pair potentials may be in order.
    Type of Medium: Electronic Resource
    Library Location Call Number Volume/Issue/Year Availability
    BibTip Others were also interested in ...
  • 7
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 115 (2001), S. 1916-1927 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Time-lapse scanning tunneling microscopy (STM) has been used to observe the oxygen induced reconstruction behavior of Ni(977), a stepped metallic surface. Previous studies using helium atom diffraction resolved the macroscopic kinetics for the reversible step-doubling and -singling of this vicinal surface. Sequential STM imaging recorded at elevated temperature has now elucidated atomic-level mechanistic details for the merging of steps in the presence of small amounts of adsorbed oxygen, less than 2% of a monolayer. Point contact between neighboring steps decorated with chemisorbed oxygen facilitates rapid step coalescence by means of zippering. An optimal oxygen concentration of step edge saturation was found to enable the step merging to proceed most rapidly. Excess oxygen was found to hinder the coalescence of neighboring steps through the possible growth of overlayer structures on the terraces. At sufficiently high temperatures, the surface is driven back to single steps due to oxygen dissolution. The departure of oxygen from the surface through dissolution, as well as the associated presence of oxygen in the selvedge region, may both play a role in destabilizing the double steps. Local step density influences the coalescence behavior by defining the number of available step edge sites. The microscopic details made available by time-resolved STM imaging illuminate some of the mechanistic steps related to the initial stages of metallic oxidation, and the sensitivity of surface morphological transformations to local surface structure and adsorbate coverage. © 2001 American Institute of Physics.
    Type of Medium: Electronic Resource
    Library Location Call Number Volume/Issue/Year Availability
    BibTip Others were also interested in ...
  • 8
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 114 (2001), S. 4730-4740 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Time-sequenced atomic force microscopy (AFM) studies of ultrathin films of cylinder-forming polystyrene-block-polymethylmethacrylate (PS-b-PMMA) copolymer are presented which delineate thin film mobility kinetics and the morphological changes which occur in microphase-separated films as a function of annealing temperature. Of particular interest are defect mobilities in the single layer (L thick) region, as well as the interfacial morphological changes which occur between L thick and adjacent 3L/2 thick layers, i.e., structural changes which occur during multilayer evolution. These measurements have revealed the dominant pathways by which disclinations and dislocations transform, annihilate, and topologically evolve during thermal annealing of such films. Mathematical combining equations are given to better explain such defect transformations and show the topological outcomes which result from defect–defect encounters. We also report a collective, Arrhenius-type flow of defects in localized L thick regions of the film; these are characterized by an activation energy of 377 kJ/mol. These measurements represent the first direct investigation of time-lapse interfacial morphological changes including associated defect evolution pathways for polymeric ultrathin films. Such observations will facilitate a more thorough and predictive understanding of diblock copolymer thin film dynamics, which in turn will further enable the utilization of these nanoscale phase-separated materials in a range of physical and chemical applications. © 2001 American Institute of Physics.
    Type of Medium: Electronic Resource
    Library Location Call Number Volume/Issue/Year Availability
    BibTip Others were also interested in ...
  • 9
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 112 (2000), S. 3208-3213 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The downstream composition of a skimmed supersonic binary molecular beam originally consisting of a 20% neon/80% xenon mixture before expansion has been studied as a function of nozzle stagnation pressure. We have found that the neon to xenon ratio dropped dramatically as the stagnation pressure was increased at low nozzle temperature (303 K), a drop which cannot be well described by existing theory. Time-of-flight (TOF) measurements indicate that Xe clustering occurs as the stagnation pressure is increased. This clustering coincides with the additional Ne depletion we observe. At a higher nozzle temperature where Xe clustering does not occur (573 K), this measured mass separation phenomenon is absent. Similar experiments have been done for another binary mixture, 20% O2/80% Xe. Similar anomalous mass separation is observed with this mixture, confirming the attribution of this phenomenon to clustering of the more massive component of the mixture. These findings have implications for novel methods of gas-dynamics-based mass separation potentially including isotope enrichment. © 2000 American Institute of Physics.
    Type of Medium: Electronic Resource
    Library Location Call Number Volume/Issue/Year Availability
    BibTip Others were also interested in ...
  • 10
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 112 (2000), S. 2470-2478 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: In this paper, we elaborate on our previous communication of high coverages of oxygen on Rh(111) [J. Chem. Phys. 110, 2757 (1999)]. When dosing with O2, half of a monolayer of O is adsorbed. Higher coverages can be achieved when exposing the surface to O atoms. As the quantity of adsorbed O increases from a half to a full monolayer, the overlayer structure undergoes several distinct phase changes. At a full monolayer, the (1×1)-O structure is stable at surface temperatures less than ∼400 K. Continued dosing with O atoms results in the rapid migration of O into the bulk. We also report on the chemical reactivity of this densely oxygen-covered surface with CO, H2, and propene. © 2000 American Institute of Physics.
    Type of Medium: Electronic Resource
    Library Location Call Number Volume/Issue/Year Availability
    BibTip Others were also interested in ...
Close ⊗
This website uses cookies and the analysis tool Matomo. More information can be found here...