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  • 1
    Electronic Resource
    Electronic Resource
    Springer
    Il nuovo cimento della Società Italiana di Fisica 15 (1993), S. 493-499 
    ISSN: 0392-6737
    Keywords: Phonon states and bands, normal modes, and phonon dispersion
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Summary We present EELS cross-section data of surface phonons on Ag(001) along $$\bar \Gamma - \bar {\rm M}$$ . The inelastic intensity is due to the contribution of different modes which are not solved by the EEL spectrometer. However, the shape of the inelastic intensity shows a strong dependence on impact energy for all wave vectors, which allows tuning the EELS on the different modes. The dependence of the loss frequency on impact energy is at variance with the one reported previously for $$\bar {\rm M}$$ , leading to the conclusion that other modes contribute to the inelastic intensity besidesS 1 andL 1 which dominate at $$\bar {\rm M}$$ .
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  • 2
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 115 (2001), S. 3346-3355 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We investigated O2 adsorption on Ag(001) in the presence of defects induced by Ne+ sputtering at different crystal temperatures, corresponding to different surface morphologies recently identified by scanning tunneling microscopy. The gas-phase molecules were dosed with a supersonic molecular beam. The total sticking coefficient and the total uptake were measured with the retarded reflector method, while the adsorption products were characterized by high resolution electron energy loss spectroscopy. We find that, for the sputtered surfaces, both sticking probability and total O2 uptake decrease. Molecular adsorption takes place also for heavily damaged surfaces but, contrary to the flat surface case, dissociation occurs already at a crystal temperature, T, of 105 K. The internal vibrational frequency of the O2 admolecules indicates that two out of the three O2− moieties present on the flat Ag(001) surface are destabilized by the presence of defects. The dissociation probability depends on surface morphology and drops for sputtering temperatures larger than 350 K, i.e., when surface mobility prevails healing the defects. The latter, previously identified with kink sites, are saturated at large O2 doses. The vibrational frequency of the oxygen adatoms, produced by low temperature dissociation, indicates the formation of at least two different adatom moieties, which we tentatively assign to oxygen atoms at kinks and vacancies. © 2001 American Institute of Physics.
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  • 3
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 112 (2000), S. 6840-6843 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: As recently demonstrated, the morphology of a surface can be modified on the mesoscopic scale by ion sputtering. Here we show by microscopy and spectroscopy that the chemical properties of the surface are strongly affected by nanostructuring and that surface reactivity can be tuned by changing surface morphology. For the otherwise inert Ag(001) surface significant O2 dissociation takes place on the nanostructured surface, thus allowing us to control the relative coverage of admolecules and adatoms. The dissociation probability is determined by the experimentally tunable density of kinks. © 2000 American Institute of Physics.
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  • 4
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    Journal of Mathematical Physics 37 (1996), S. 4235-4242 
    ISSN: 1089-7658
    Source: AIP Digital Archive
    Topics: Mathematics , Physics
    Notes: The space of analytical test functions ξ, rapidly decreasing on the real axis (i.e., Schwartz test functions of the type S on the real axis), is used to construct the rigged Hilbert space (RHS) (ξ,H,ξ′). Gamow states (GS) can be defined in RHS starting from Dirac's formula. It is shown that the expectation value of a self-adjoint operator acting on a GS is real. We have computed exactly the probability of finding a system in a GS and found that it is finite. The validity of recently proposed approximations to calculate the expectation value of self-adjoint operators in a GS is discussed. © 1996 American Institute of Physics.
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  • 5
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    Journal of Mathematical Physics 35 (1994), S. 4429-4438 
    ISSN: 1089-7658
    Source: AIP Digital Archive
    Topics: Mathematics , Physics
    Notes: The fundamental space ζ is defined as the set of entire analytic functions [test functions cursive-phi(z)], which are rapidly decreasing on the real axis. The variable z corresponds to the complex energy plane. The conjugate or dual space ζ' is the set of continuous linear functionals (distributions) on ζ. Among those distributions are the propagators, determined by the poles implied by the equations of motion and the contour of integration implied by the boundary conditions. All propagators can be represented as linear combinations of elementary (one pole) functionals. The algebra of convolution products is also determined. The Fourier transformed space ζ˜ contains test functions cursive-phi˜(x). These functions are extra-rapidly decreasing, so that the exponentially increasing solutions of higher-order equations are distributions on ζ˜.
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  • 6
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 101 (1994), S. 713-725 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We investigated the dynamics of the adsorption of O2 on Ag(110) with the molecular beam technique combined with EEL spectroscopy and with the method of King and Wells. The initial sticking coefficient S0 is reported for molecules impinging along both high symmetry azimuthal directions 〈001〉 and 〈11¯0〉 as a function of total energy and angle of incidence of the molecules and crystal temperature. The initial sticking coefficient is anisotropic for low as well as for room temperature adsorption. The dependence of the sticking coefficient on the temperature of the sample, Ts, indicates that adsorption takes place directly into the molecular well. Dissociation is eventually induced thermally for Ts(approximately-greater-than)150 K. The physisorbed state plays no role in the chemisorption process in the investigated impact energy range.
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  • 7
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 101 (1994), S. 726-730 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We report on the dependence of the sticking coefficient S of O2 on Ag(110) on oxygen coverage, for molecular and dissociative adsorption. S is found to diminish strongly with increasing coverage. The initial dependence is linear and for dissociative adsorption the slope depends on crystal temperature. The data are indicative of a coverage dependence of the adsorption barrier height, which is caused by the change of the surface work function with coverage. The analysis of the temperature variation of the dependence of S on coverage allows to extract the variation of the ratio of the pre-exponential factors and of the height of the barriers for desorption and dissociation from the molecularly chemisorbed state.
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  • 8
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 106 (1997), S. 9297-9304 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The coverage dependence of the vibrational modes of O2 chemisorbed on Ag(001) was studied by electron energy loss spectroscopy. We observe the dipole active modes associated to the intramolecular stretch and to the molecule–surface vibrations. Moreover two further features are present in the EEL spectra, due to the anharmonicity of the molecular potential: the combination-band of the stretching and of the molecule–surface vibration, and the first overtone of the O–O stretching mode. From the EELS intensity of the O–O stretching mode versus coverage the dynamical charge transfer e*=0.61±0.02 e− is determined which corresponds to a dynamical dipole moment μ=0.16±0.01 D. The O2–Ag vibrational frequency is found to decrease with coverage, suggesting that a weakening of the molecule–surface bond takes place. This observation is confirmed by thermal desorption spectroscopy. The anharmonicity parameter xe of the O–O potential increases significantly upon chemisorption, in analogy to O2–Ag(110) and O2–Pt(111). The intensity of the overtone peak is analyzed within the Morse approximation, allowing us to discriminate the contributions arising from the mechanical anharmonicity, and from the nonlinearity of the dynamical charge flow. A correlation is observed between the magnitude of e* and the contribution of the latter term to the overtone intensity. © 1997 American Institute of Physics.
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  • 9
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 109 (1998), S. 2490-2502 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We have investigated desorption and dissociation of O2 chemisorbed on Ag(001) induced by collision with hyperthermal Xe and Ar atoms by high resolution electron energy loss spectroscopy and supersonic molecular beam technique. The cross section for both processes increases rapidly both as a function of angle of incidence and of total impact energy of the inert gas atom. While the increase with energy is expected, the increase with the angle is somewhat surprising and is sensibly larger than observed for previously investigated systems. The cross section for desorption decreases moreover with coverage. In the limit of high impact energy and high coverage its value is always larger than the one for dissociation. The branching ratio between the two processes depends thereby on energy and angle of incidence of the inert gas atom. Atomic oxygen is not removed under any impact condition, because of its larger binding energy. In order to explain the experimental results, molecular dynamics simulations have been performed using a simple model including multiple scattering. We find that the angular dependence of the cross section is determined by surface corrugation and by multiple scattering which suppresses desorption at normal incidence while the energetic threshold is determined by energy loss to the substrate. © 1998 American Institute of Physics.
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  • 10
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 106 (1997), S. 711-718 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The coverage dependence of the sticking coefficient and temperature programmed desorption kinetics for molecular adsorption of oxygen on Ag(001) are investigated both experimentally and theoretically. The nearly exponential decrease of the sticking coefficient as a function of coverage by about five orders of magnitude is explained within a kinetic lattice gas model to be the result of strong nearest- and next-nearest-neighbor repulsions. The latter also shape the desorption spectra which are calculated within the same model under the assumption that fast surface diffusion maintains the adsorbate in quasiequilibrium during desorption. Because the desorption rate is proportional to the sticking coefficient under these conditions, we find a massive decrease of the pre-exponential factor in the Arrhenius parametrization of the rate as a function of coverage which explains the peculiar shape of the desorption spectra. © 1997 American Institute of Physics.
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