Efficient periodic density functional theory calculations of charged molecules and surfaces using Coulomb kernel truncation
Fuente:
arXiv
Gespeichert in:
| Hauptverfasser: | , , , , , , |
|---|---|
| Format: | Preprint |
| Veröffentlicht: |
2025
|
| Schlagworte: | |
| Online-Zugang: | |
| Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
| _version_ | 1866910773529280512 |
|---|---|
| author | Vijay, Sudarshan Schlipf, Martin Miranda, Henrique Karsai, Ferenc Kaltak, Merzuk Marsman, Martijn Kresse, Georg |
| author_facet | Vijay, Sudarshan Schlipf, Martin Miranda, Henrique Karsai, Ferenc Kaltak, Merzuk Marsman, Martijn Kresse, Georg |
| contents | Density functional theory (DFT) calculations of charged molecules and surfaces are critical to applications in electro-catalysis, energy materials and related fields of materials science. DFT implementations such as the Vienna ab-initio Simulation Package (VASP) compute the electrostatic potential under 3D periodic boundary conditions, necessitating charge neutrality. In this work, we implement 0D and 2D periodic boundary conditions to facilitate DFT calculations of charged molecules and surfaces respectively. We implement these boundary conditions using the Coulomb kernel truncation method. Our implementation computes the potential under 0D and 2D boundary conditions by selectively subtracting unwanted long-range interactions in the potential computed under 3D boundary conditions. By combining the Coulomb kernel truncation method with a computationally efficient padding approach, we remove nonphysical potentials from vacuum in 0D and 2D systems. To illustrate the computational efficiency of our method, we perform large supercell calculations of the formation energy of a charged chlorine defect on a sodium chloride (001) surface and perform long time-scale molecular dynamics simulations on a stepped gold (211) | water electrode-electrolyte interface. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2501_02435 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Efficient periodic density functional theory calculations of charged molecules and surfaces using Coulomb kernel truncation Vijay, Sudarshan Schlipf, Martin Miranda, Henrique Karsai, Ferenc Kaltak, Merzuk Marsman, Martijn Kresse, Georg Materials Science Chemical Physics Density functional theory (DFT) calculations of charged molecules and surfaces are critical to applications in electro-catalysis, energy materials and related fields of materials science. DFT implementations such as the Vienna ab-initio Simulation Package (VASP) compute the electrostatic potential under 3D periodic boundary conditions, necessitating charge neutrality. In this work, we implement 0D and 2D periodic boundary conditions to facilitate DFT calculations of charged molecules and surfaces respectively. We implement these boundary conditions using the Coulomb kernel truncation method. Our implementation computes the potential under 0D and 2D boundary conditions by selectively subtracting unwanted long-range interactions in the potential computed under 3D boundary conditions. By combining the Coulomb kernel truncation method with a computationally efficient padding approach, we remove nonphysical potentials from vacuum in 0D and 2D systems. To illustrate the computational efficiency of our method, we perform large supercell calculations of the formation energy of a charged chlorine defect on a sodium chloride (001) surface and perform long time-scale molecular dynamics simulations on a stepped gold (211) | water electrode-electrolyte interface. |
| title | Efficient periodic density functional theory calculations of charged molecules and surfaces using Coulomb kernel truncation |
| topic | Materials Science Chemical Physics |
| url | https://arxiv.org/abs/2501.02435 |