ELECTRODE: An electrochemistry package for atomistic simulations

Ludwig J. V. Ahrens-Iwers; Mathijs Janssen; Shern R. Tee; Robert H. Meißner

doi:10.1063/5.0099239

journal article Open Access Aug 25, 2022

ELECTRODE: An electrochemistry package for atomistic simulations

Ludwig J. V. Ahrens-Iwers

Mathijs Janssen

Shern R. Tee

Robert H. Meißner

The Journal of Chemical Physics Vol. 157 No. 8 · AIP Publishing

View at Publisher Save 10.1063/5.0099239

Abstract

Constant potential methods (CPMs) enable computationally efficient simulations of the solid–liquid interface at conducting electrodes in molecular dynamics. They have been successfully used, for example, to realistically model the behavior of ionic liquids or water-in-salt electrolytes in supercapacitors and batteries. CPMs model conductive electrodes by updating charges of individual electrode atoms according to the applied electric potential and the (time-dependent) local electrolyte structure. Here, we present a feature-rich CPM implementation, called ELECTRODE, for the Large-scale Atomic/Molecular Massively Parallel Simulator, which includes a constrained charge method and a thermo-potentiostat. The ELECTRODE package also contains a finite-field approach, multiple corrections for nonperiodic boundary conditions of the particle–particle particle–mesh solver, and a Thomas–Fermi model for using nonideal metals as electrodes. We demonstrate the capabilities of this implementation for a parallel-plate electrical double-layer capacitor, for which we have investigated the charging times with the different implemented methods and found an interesting relationship between water and ionic dipole relaxations. To prove the validity of the one-dimensional correction for the long-range electrostatics, we estimated the vacuum capacitance of two coaxial carbon nanotubes and compared it to structureless cylinders, for which an analytical expression exists. In summary, the ELECTRODE package enables efficient electrochemical simulations using state-of-the-art methods, allowing one to simulate even heterogeneous electrodes. Moreover, it allows unveiling more rigorously how electrode curvature affects the capacitance with the one-dimensional correction.

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Details

Published: Aug 25, 2022
Vol/Issue: 157(8)
License: View

Authors

L

Ludwig J. V. Ahrens-Iwers

Institute of Advanced Ceramics, Hamburg University of Technology 1 , Hamburg, Germany

M

Mathijs Janssen

Mechanics Division, Department of Mathematics, University of Oslo 2 , N-0851 Oslo, Norway

S

Shern R. Tee

Australian Institute for Bioengineering and Nanotechnology, The University of Queensland 3 , Brisbane, Queensland, Australia

R

Robert H. Meißner

Institute of Polymers and Composites, Hamburg University of Technology 4 , Hamburg, Germany; Helmholtz-Zentrum Hereon, Institute of Surface Science 5 , Geesthacht, Germany

Funding

Deutsche Forschungsgemeinschaft Award: 192346071

Cite This Article

Ludwig J. V. Ahrens-Iwers, Mathijs Janssen, Shern R. Tee, et al. (2022). ELECTRODE: An electrochemistry package for atomistic simulations. The Journal of Chemical Physics, 157(8). https://doi.org/10.1063/5.0099239

ELECTRODE: An electrochemistry package for atomistic simulations

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