Lowest-energy structures (left panels) and charge density difference plots (right panels) of 0.67 ML Cl adsorption on: (a) flat surface; (b) Au(111) covered with 0.33 ML Au adatoms; (c) 0.67 ML Au adatoms. The darker gray circles represent the top full layer of gold atoms, lighter yellow circles represent gold adatoms, and small (green) circles represent chlorine atoms. The thick dotted lines on the structural figures on the left show the planes on which the density difference is plotted. Red contours correspond to charge depletion and blue contours to charge accumulation.
Lowest-energy structures (left panels) and charge density difference plots (right panels) of: (a) 0.67 ML O adsorption on flat, Au(111) surface; (b) 0.67 ML O adsorption on Au(111) surface covered with 0.33 ML adatoms; (c) 1.00 ML O adsorption on 0.33 ML Au adatom-covered Au(111) surface. Symbols are the same as in Fig. 1, with red for O atoms.
Surface free energy as a function of the oxygen chemical potential for different oxygen and gold adatom coverages. The clean surface is represented by a horizontal line at a surface free energy of 0 eV. The transition range in the oxygen chemical potential between regions, representing the error introduced by the choice of exchange-correlation functional, is indicated by checkered-square region.
(a) Au -PDOS vs energy for the surface gold atom of the clean surface, gold adatom for the 0.33 ML adatom-covered surface, and gold adatom for the 0.33 ML adatom-covered surface with 0.67 ML Cl. (b) -PDOS vs energy for 0.67 ML of chlorine on the clean surface and 0.33 ML Au adatom-covered surface. The zero of the energy scale is the Fermi level.
Summary of total energies, , defined in Eq. (2), for two Cl coverages, [expressed in ML for the unit cell] on Au(111) with different gold adatom coverages, . Bold characters indicate the systems with the lowest energy at each chlorine and adatom coverage.
Summary of total energies, for three O coverages, , on Au(111) with different gold adatom coverages, . Notation is the same as in Table I. Energies in brackets are from the PBE functional and are used to estimate the error in Fig. 3.
Summary of calculated charges for different coverages of O and Cl on Au(111) with different gold adatom coverages . The two different methods of calculating charge are indicated, (A) sphere, or (B) Bader method.
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