Halide Adsorption on Single-crystal Silver Substrates: Dynamic Simulations and ab-initio Density-functional Theory

Abstract

We investigate the static and dynamic behaviors of a Br adlayer electrochemically deposited onto single-crystal Ag(100) using an off-lattice model of the adlayer. Unlike previous studies using a lattice-gas model, the off-lattice model allows adparticles to be located at any position within a two-dimensional approximation to the substrate. Interactions with the substrate are approximated by a corrugation potential. Using Density Functional Theory (DFT) to calculate surface binding energies, a sinusoidal approximation to the corrugation potential is constructed. A variety of techniques, including Monte Carlo and Langevin simulations, are used to study the behavior of the adlayer. The lateral root-mean-square (rms) deviation of the adparticles from the binding sites is presented along with equilibrium coverage isotherms, and the thermally activated Arrhenius barrier-hopping model used in previous dynamic Monte Carlo simulations is tested.

30 pages, 9 figures, 3 tables, to appear in Faraday Discussions

Cited by in corpus (11)

• Diffusion on a solid surface: Anomalous is normal
• From subdiffusion to superdiffusion of particles on solid surfaces
• First-principles calculations for the adsorption of water molecules on the Cu(100) surface
• Low-temperature nucleation in a kinetic Ising model under different stochastic dynamics with local energy barriers
• Cl electrosorption on Ag(100): Lateral interactions and electrosorption valency from comparison of Monte Carlo simulations with chronocoulometry experiments
• An Off-lattice Model for Br Electrodeposition on Au(100): from DFT to Experiment
• Determination of the basic timescale in kinetic Monte Carlo simulations by comparison with cyclic-voltammetry experiments
• Microstructure and velocity of field-driven solid-on-solid interfaces moving under stochastic dynamics with local energy barriers
• Field-driven solid-on-solid interfaces moving under a stochastic Arrhenius dynamic: effects of the barrier height
• New Cyclic Voltammetry Method for Examining Phase Transitions: Simulated Results
• Applications of Computer Simulations and Statistical Mechanics in Surface Electrochemistry