Charged Adsorbates on Metallic Surfaces from Periodic to Open Boundary Conditions
Nicéphore Bonnet, Nicola Marzari
TL;DR
This paper introduces a method to accurately calculate the energy of charged particles on metal surfaces using computational models.
Contribution
The paper presents an analytical correction for finite-cell calculations of charged adsorbates on metallic surfaces.
Findings
The method is demonstrated using Li+, Na+, and K+ adsorption on graphite.
Periodic calculations show slow convergence with system size, emphasizing the need for infinite limit corrections.
Abstract
Understanding the thermodynamics of adsorbates on surfaces is central to many (electro)catalysis applications. In first-principles calculations, additional challenges arise when considering charged adsorbates owing to long-range electrostatic interactions in the in-plane and normal directions. Here, we derive an analytical correction to obtain the energy profiles of individual charged adsorbates on metallic surfaces from finite-cell calculations in periodic boundary conditions. The method is illustrated by calculating the adsorption energy profiles of Li+, Na+, and K+ on graphite from first-principles, highlighting the very slow convergence with system size of the periodic calculations and the need to correctly recover the infinite limit.
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Taxonomy
Topicsnanoparticles nucleation surface interactions · Advanced Chemical Physics Studies · Surface and Thin Film Phenomena