An Off-lattice Model for Br Electrodeposition on Au(100): from DFT to Experiment

TL;DR

This paper develops an off-lattice model for bromine electrodeposition on gold, derived from density functional theory calculations, accurately capturing experimental observations of the incommensurate ordered phase.

Contribution

It introduces a parameter-free off-lattice model based on DFT calculations to better represent Br adsorption on Au(100), surpassing lattice-gas limitations.

Findings

Model accurately reproduces experimental data

Parameters derived from DFT improve model reliability

Off-lattice approach captures incommensurate phases

Abstract

Since Br adsorption on Au(100) displays an incommensurate ordered phase, a lattice-gas treatment of the adlayer configurations is not reliable. We therefore use density functional theory slab calculations to determine the parameters necessary for the construction of an off-lattice model. We compute and analyze the total energy and electron density as the lateral Br position and coverage are varied. This allows the calculation of the corrugation potential, the short-range lateral interactions, the dipole moment (long-range interactions), and the residence charge. From these parameters, we construct an off-lattice model with no freely adjustable parameters. The simulation results compare remarkably well with experimental results.