Nicephore Bonnet^1*, Nicola Marzari^1*

1 Theory and Simulation of Materials (THEOS), École Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland

* Corresponding authors emails: nicephore.bonnet@epfl.ch, nicola.marzari@epfl.ch

DOI10.24435/materialscloud:1n-sa [version v1]

Publication date: May 26, 2025

How to cite this record

Nicephore Bonnet, Nicola Marzari, Charged adsorbates on metallic surfaces from periodic to open boundary conditions, Materials Cloud Archive 2025.86 (2025), https://doi.org/10.24435/materialscloud:1n-sa

Description

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. In this record, we provide the generic input file used to generate the calculated energies of Fig. 4.

Materials Cloud sections using this data

Files

File name	Size	Description
input_file.in MD5md5:ca57a5d2898fae001831d0fa079a71af	4.0 KiB	Typical Quantum ESPRESSO input file of graphite slab + Li+ system used to generate the calculated energies of Fig. 4. Here the slab contains 3 layers in the 3x2 cell.

License

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External references

Keywords

DFT Electrochemistry Charged defects Surface / interface