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  • 2000-2004  (12)
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Year
  • 1
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 115 (2001), S. 4314-4321 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The dynamics of the image potential states n=3 and n=4 at the Cu(100) surface are studied. We solve the Liouville–von Neumann equation for an open system and treat the dissipation within the Lindblad formalism. We compute the two-photon photoemission spectrum (2PPE) using first order perturbation theory and study the populations of the image potential states and the two-photon photoemission spectrum as functions of the lifetimes and dephasings of the image potential states. The computed two-photon photoemission spectrum is compared with the measured spectrum obtained by Höfer et al. [Appl. Phys. B 68, 383 (1999); Science 277, 1480 (1997)]. © 2001 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 115 (2001), S. 2721-2729 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: The self-assembly of ink molecules deposited using dip-pen nanolithography (DPN) is modeled as a two-dimensional diffusion with a source (tip). A random walk simulation and simple analytic theory are used to study how the diffusion dynamics affects patterns generated in DPN. For a tip generating a constant flux of ink molecules, circles, lines, and letters are studied by varying the deposition rate of ink molecules and the tip scan speed. Even under the most favorable condition studied here, peripheries of patterns fluctuate from perfect circles or lines, due to the random, diffusional nature of self-assembly. The degree of fluctuation is quantified for circles and lines. Circles generated by fixing the tip position do not depend on the deposition rate if the same amount of ink is deposited. For a moving tip, patterns change drastically depending on tip speed and deposition rate. Overall, fast scan or slow deposition relative to the diffusion time scale makes lines narrower. When the tip deposits ink too slowly or scans too fast, patterns become incoherent, making molecules in patterns separated from each other. Therefore, there seems to be an optimal choice of the deposition rate and tip speed that gives both narrow and coherent patterns. We also explore the consequences of varying the relative rates of diffusion of ink molecules on bare surface and on previously deposited molecules. © 2001 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 3
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 115 (2001), S. 718-725 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Stationary direct perturbation theory is used to calculate a scalar relativistic correction to the species in the G3/99 test set. We observe that the relativistic energy almost always reduces atomization energies, electron affinities, and ionization potentials. Exceptions occur when s orbitals play a predominant role in the energy differences between reactants and products. The scalar relativistic energy, when added to G3 theory and the empirical parameters are reoptimized, gives slightly worse agreement with experiment. © 2001 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 4
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 114 (2001), S. 3790-3799 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Methods for calculating potential energy surfaces of image potential states are presented. The methods cover metal–vacuum interfaces, metal–dielectric medium interfaces, and metal–dielectric medium–vacuum interfaces. The metal is approximated as a perfect conductor or as a Fermi–Thomas metal. Potential energy surfaces and the induced charge densities are presented as functions of the properties of the dielectric medium, the metal and the thickness of the absorbed material. © 2001 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 5
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 114 (2001), S. 9048-9058 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A mixture of large and small Lennard-Jones particles is studied; in the study we focus on the relations among temperature, packing, structure, and transport in the supercooled state. As the temperature decreases, one sees increasing component separation, and local ordering. Clusters consisting of only small particles grow in size with time and cooling; the dominant local structure in those clusters is hexagonal. The rest of the system, including almost all large and some small particles, remains amorphous, with local order dictated by the geometry of dense packing of mixed large and small particles. To study these effects independently, we modified the conventional model by managing the relaxation of large particles. At low temperatures, the diffusion of small particles dramatically decreases when the large particles are frozen. An interpretation of these findings based on the local rearrangement kinetics is proposed. © 2001 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 6
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 115 (2001), S. 8185-8192 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We present a method for determining quadratic response molecular properties of heterogeneously solvated molecules. The method enables the calculation of frequency-dependent hyperpolarizabilities and two-photon transition matrix elements of molecules that are (i) located at the surface of a metal or (ii) solvated alongside the surface of a metal. The metal is represented as a perfect conductor and the solvent is described by a dielectric medium. The method is able to describe the electronic structure of the molecular systems both at the uncorrelated and correlated electronic structure levels. The latter is given by the multiconfigurational self-consistent field method. We have completed sample calculations of the frequency-dependent first-order hyperpolarizability tensor and two-photon matrix elements for heterogeneously solvated CO. We find that the molecular properties depend strongly on the heterogeneous solvent configuration. © 2001 American Institute of Physics.
    Type of Medium: Electronic Resource
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  • 7
    Electronic Resource
    Electronic Resource
    College Park, Md. : American Institute of Physics (AIP)
    The Journal of Chemical Physics 114 (2001), S. 3800-3808 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: Methods for calculating wavefunctions and eigenvalues of image potential states are presented. We consider cases corresponding to metal–vacuum interfaces, metal–dielectric medium interfaces and metal–dielectric medium–vacuum interfaces. We represent the metal as a perfect conductor or as a Fermi–Thomas metal. We present the dependence of the wavefunctions and eigenvalues of the image potential states on dielectric constants, electron affinity, work function of the metal, and inverse Fermi screening parameter. © 2001 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 114 (2001), S. 2062-2066 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We develop a simple semiempirical Pariser–Parr–Pople-type model of a metal. It can be used for studies of adsorption and of the interactions between the metal surface and external charges, and is compatible with ab initio description of the molecules outside the metal. We investigate the dependence of the image-type field on the few parameters that control the model behavior, and develop a simple direct minimization self-consistent field technique that is useful for convergence in nearly degenerate cases. © 2001 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 112 (2000), S. 4014-4019 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: We study the correlation energy in the H2 molecule as a function of bond distance and the electron coupling parameter that modifies the strength of electron–electron repulsion. For the unscaled electron repulsion we find an unusual complexity of the correlation energy dependence on the bond distance. This complexity remains if the electron repulsion is scaled down. We pay particular attention to the range of bond distances near the H2 equilibrium geometry. We confirm that good performance of the modern exchange–correlation functionals in molecular geometry optimization is due to the cancellation of errors between the exchange and correlation components. These components have different functional dependence on the electron coupling parameter, so the cancellation of errors no longer occurs when the electron repulsion is scaled down. This observation is important if the adiabatic connection theorem is used to construct the exchange–correlation functionals. It is also relevant for the performance of exchange–correlation functionals to study ionic interactions. The performance of the correlation operator in the molecular environment is also investigated and discussed. © 2000 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 115 (2001), S. 3792-3803 
    ISSN: 1089-7690
    Source: AIP Digital Archive
    Topics: Physics , Chemistry and Pharmacology
    Notes: A multiconfigurational self-consistent reaction field (MCSCRF) method is presented for solvation of a molecule on a metal surface. We assume that the molecular system is enclosed in a half-spherical cavity and adsorbed on the surface of a perfect conductor. The half-spherical cavity is embedded in a linear, homogeneous, isotropic dielectric medium. A multiconfigurational self-consistent reaction field linear response method is presented for calculating frequency dependent polarizabilities as well as electronic excitation energies and transition moments of a solvated molecule on a metal surface. © 2001 American Institute of Physics.
    Type of Medium: Electronic Resource
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