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Simulation of Adsorption Processes at Metallic Interfaces: An Image Charge Augmented QM/MM Approach

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Institute of Physical Chemistry, University of Zürich, Winterthurerstrasse 190, CH-8057 Zürich, Switzerland
The Abdus Salam International Centre for Theoretical Physics, Strada Costiera 11, I-34151 Trieste, Italy
§ Empa, Swiss Federal Laboratories for Materials Science and Technology, nanotech@surfaces Laboratory, Überlandstrasse 129, CH-8600 Dübendorf, Switzerland
Cite this: J. Chem. Theory Comput. 2013, 9, 11, 5086–5097
Publication Date (Web):September 24, 2013
https://doi.org/10.1021/ct400698y
Copyright © 2013 American Chemical Society

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    Abstract

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    A novel method for including polarization effects within hybrid quantum mechanics/molecular mechanics (QM/MM) simulations of adsorbate-metal systems is presented. The interactions between adsorbate (QM) and metallic substrate (MM) are described at the MM level of theory. Induction effects are additionally accounted for by applying the image charge formulation. The charge distribution induced within the metallic substrate is modeled by a set of Gaussian charges (image charges) centered at the metal atoms. The image charges and the electrostatic response of the QM potential are determined self-consistently by imposing the constant-potential condition within the metal. The implementation is embedded in a highly efficient Gaussian and plane wave framework and is naturally suited for periodic systems. Even though the electronic properties of the metallic substrate are not taken into account explicitly, the augmented QM/MM scheme can reproduce characteristic polarization effects of the adsorbate. The method is assessed through the investigation of structural and electronic properties of benzene, nitrobenzene, thymine, and guanine on Au(111). The study of small water clusters adsorbed on Pt(111) is also reported in order to demonstrate that the approach provides a sizable correction of the MM-based interactions between adsorbate and substrate. Large-scale molecular dynamics (MD) simulations of a water film in contact with a Pt(111) surface show that the method is suitable for simulations of liquid/metal interfaces at reduced computational cost.

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    Contour plot of the electrostatic potential for nitrobenzene on Au(111), charges induced in finite Au(111) slabs by Cl and Na+, Δρelec for benzene on Au(111) as obtained by full DFT, variation of the dipole moment (x-, y-, and z-component) for guanine on Au(111), plane-averaged electrostatic potential of 151 H2O on Pt(111) for a particular snapshot of the MD simulation. This material is available free of charge via the Internet at http://pubs.acs.org/.

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