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  • 1
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 111 (1999), S. 1636-1649 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Supra-valence electron transfer from surface Cs-doped MoS2(0002) to electron acceptor adsorbates was investigated by high resolution x-ray photoelectron spectroscopy (HRXPS) in the valence band region and above the valence band maximum (VBM). Deposition of a sub-monolayer amount of Cs onto the basal plane of MoS2 introduced a new electron density of states at ca. 1.25 eV above VBM. Angle-resolved HRXPS and theoretical analysis located this electron density in the MoS2 layer. Upon the reaction with Cl2, this Cs-induced photoelectron almost completely disappeared and the Cs 3d and Cl 2p core levels indicated the formation of a surface Cs-chloride species. The Cs-covered MoS2(0002) surface also reacted with O2 to form surface peroxides and superoxides, as evidenced by two distinct binding energies of the O 1s core level peaks. However, the reaction with water proved to be more difficult: Exposure of the Cs-covered MoS2(0002) surface to H2O at 10−5 Torr did not result in electron transfer reaction, but the Cs/MoS2(0002) surface exposed to H2O at 1 Torr showed a substantial decrease in the density of states above VBM as well as formation of a surface-hydroxide, indicated by the O 1s core level position. Theoretical calculations using a full-potential linearized augmented plane wave density functional theory (FLAPW-DFT) confirm the conclusion based on experimental intensity anisotropy of the new peak: the Cs 6s electron transfers into the MoS2 substrate, forming the Cs/MoS2 electron donor–acceptor complex with Csδ+. In addition, all phenomena observed during the adsorption of electron donor–acceptor molecules are quantitatively accounted by the theory. © 1999 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 2
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 108 (1998), S. 3863-3870 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A systematic ab initio study of the dynamic multipole polarizabilities of the halogen anions F−, Cl−, Br− and I− is presented. The effects of electron correlation are included for the static as well as for the frequency-dependent polarizabilities using time-dependent second-order Møller-Plesset perturbation theory. Large one-particle basis sets, optimized for polarizabilities, are used to obtain results near the MP2 basis set limit. For the anions Br− and I− also scalar relativistic effects are accounted for by means of the spin-free no-pair Hamiltonian H(circumflex)+sf1. For the static dipole polarizabilities of the anions F− and Cl− we find good agreement with recent correlated ab initio calculations, but for the higher multipole polarizabilities and for the anions Br− and I− the discrepancies relative to previous calculations and empirical estimates are large. The effects of electron correlation on the polarizabilities of these anions are in general extremely large, while relativistic effects are in all four investigated halogen anions only of minor importance. The dynamic polarizabilities of the halogen anions are combined with previously calculated dynamic polarizabilities for rare gas atoms and the molecules CO and N2 to obtain isotropic and anisotropic dispersion coefficients for the corresponding van der Waals complexes. © 1998 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 3
    Electronic Resource
    Electronic Resource
    s.l. : American Chemical Society
    The @journal of physical chemistry 〈Washington, DC〉 99 (1995), S. 11715-11721 
    Source: ACS Legacy Archives
    Topics: Chemistry and Pharmacology , Physics
    Type of Medium: Electronic Resource
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  • 4
    Electronic Resource
    Electronic Resource
    [S.l.] : American Institute of Physics (AIP)
    Journal of Applied Physics 80 (1996), S. 5061-5066 
    ISSN: 1089-7550
    Source: AIP Digital Archive
    Topics: Physics
    Notes: A new approach to simulate electronic transport at high energies in silicon is introduced, which is based on a mixture of evolutionary optimization algorithms and the Monte Carlo technique. The optimization technique of the evolutionary algorithm is used to find electron distributions which are in agreement with a given physical quantity, for example, a measured substrate current. In this way, the evolutionary algorithm can calculate backward the electron distributions from results of measurements. A mutation operator, which is based on the Monte Carlo technique, is used to direct the optimization of the evolutionary algorithm toward physically correct distributions. A comparison of the results of this new approach with electron distributions calculated by a full band Monte Carlo program demonstrates both the backward calculation ability of the evolutionary algorithm and the correctness of the physical model in the Monte Carlo-like mutation operator. It becomes obvious that the electron distribution in silicon is mainly determined by the scattering rates. By suppressing the optimization of the evolutionary algorithm the Monte Carlo-like mutation operator alone was found to provide a powerful new type of Monte Carlo technique. While these methods are not as precise as a full band Monte Carlo approach, they are shown to be numerically efficient and give also a good fit to reliability related hot electron effects. © 1996 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 5
    Electronic Resource
    Electronic Resource
    [S.l.] : American Institute of Physics (AIP)
    Journal of Applied Physics 79 (1996), S. 2755-2761 
    ISSN: 1089-7550
    Source: AIP Digital Archive
    Topics: Physics
    Notes: We present results from numerical simulations of AlGaN/InGaN double-heterostructure light-emitting diodes. A highly convergent, fast, and memory efficient algorithm necessary for wide band-gap device simulation was developed and is described here. Charge carrier tunneling currents and a band to impurity recombination mechanism are included. The results compare favorably to experimental results. The results demonstrate that the saturation of power at high currents, the high rate of increase in currents at high voltages, and the reduced broadening of the optical emission spectrum at high biases, with only band-to-acceptor recombination occurring in the active region, are due to carriers leaving the active region by thermionic emission rather than recombining. © 1996 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 6
    Electronic Resource
    Electronic Resource
    [S.l.] : American Institute of Physics (AIP)
    Journal of Applied Physics 77 (1995), S. 3267-3276 
    ISSN: 1089-7550
    Source: AIP Digital Archive
    Topics: Physics
    Notes: The chemical potential and the capacitance of a 2D circular model quantum dot have been investigated for GaAs, InSb, and Si material parameters, covering a range from a few nanometers to micrometer dimensions. The Schrödinger equation has been solved self-consistently, with the inclusion of many-body effects, using a local density approximation as well as the optimized Krieger-Li-Iafrate exchange potential. Gate structures are included by use of the method of images. We have focused on quantum deviations from classical electrostatic capacitive behavior and found such deviations to be significant even for the material parameters of silicon for feature sizes smaller than 30 nm. The most striking features of quantum dot capacitance are signatures of the dot symmetry analogous to the orbital grouping in atoms: we find structure in the dot capacitance arising from quantum effects in correspondence with the filling of each group of energy-degenerate orbitals. We also cover the influence of a magnetic field perpendicular to the dot plane and we report some results for the chemical potential vs magnetic field and electron number, assuming an effective g-factor corresponding to the one of bulk gallium arsenide. © 1995 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 7
    Electronic Resource
    Electronic Resource
    [S.l.] : American Institute of Physics (AIP)
    Journal of Applied Physics 77 (1995), S. 1337-1373 
    ISSN: 1089-7550
    Source: AIP Digital Archive
    Topics: Physics
    Notes: The contributions of nonlocal mechanisms to nonlinear transport in semiconductors, with special emphasis on hot-electron emission at heterojunctions and its variations which are now commonly termed real-space transfer effects, are reviewed. The goal is to equitably account for and bring together the body of literature that has developed, often independently, in the U.S. and the former Soviet Union as well as in Europe and Japan. © 1995 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 8
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 109 (1998), S. 359-366 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Correlated relativistic all-electron supermolecular ab initio calculations of the ground state potential of the Ar–I2 molecule are presented. The role of differential intramonomer spin–orbit and correlation effects in the interaction energy is investigated and found to be only of minor importance. Two energetically very similar minima of the Ar–I2 complex are found, corresponding to a linear and a T-shaped geometry of the monomers. The comparatively large isomerization barrier for the two conformations indicates the existence of two stable isomers at very low temperatures. © 1998 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 9
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 107 (1997), S. 4033-4043 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Palladium single crystals have been found to be active for the C–H bond dissociation of methane in the temperature range 400–600 K, and the activities of the presently investigated Pd(111) and Pd(311) surfaces are compared with previously studied Pd(679). Structure sensitivity is reported that spans an order of magnitude in terms of the rates in the order Pd(111)〈Pd(311)〈Pd(679), while the effective activation energies range from 32–34 kJ/mol for Pd(111) and Pd(311) to 44 kJ/mol for Pd(679). These data are analyzed with a model that involves unsymmetrical barriers, first by constructing a potential-energy surface for Pd(111), in which the reaction pathway is well-simulated by the Eckart barrier. The Eckart barrier is then shown to obey exactly the Marcus rule for exothermic or endothermic processes. This property is used in comparing the H–CH3 dissociation on the different crystal faces, with the result that the Pd(679) surface provides a driving force of some 26 kJ/mol due to the role of defects compared to smooth planar Pd(111) surface and 22 kJ/mol compared to the Pd(311) surface. © 1997 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 10
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 111 (1999), S. 5461-5473 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Novel femtosecond, multiple pulse experiments including polarization control are performed to elucidate the dynamics of fragment recoil in the 400-nm photolysis of triiodide ions in liquid ethanol solution. The instantaneous resonance Raman response of the dynamic system, induced at well defined delays after impulsive bond fission of the parent ion, displays a time-dependent vibrational frequency of the diatomic fragment. This time dependence is interpreted through interactions between the fragments which decay with increasing interfragment separation. Simultaneously, the instantaneous anisotropic response of the reactive system exhibits electronically coherent contributions at very early times after bond breakage and provides direct evidence for the existence of electronic degeneracies in the vicinity of the Franck-Condon region. The decay of this coherent anisotropic component reflects a dynamic lifting of these electronic degeneracies upon recoil of the product species and decay of residual interactions between the fragments. From both experiments it can be concluded that in liquid solution it takes about 2 ps until the fragments arrive in the asymptotic limit of the reaction with negligible product interactions. © 1999 American Institute of Physics.
    Type of Medium: Electronic Resource
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