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The Journal of Chemical Physics
Article . 2022 . Peer-reviewed
License: CC BY
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https://dx.doi.org/10.48550/ar...
Article . 2022
License: arXiv Non-Exclusive Distribution
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Article . 2022
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Article . 2022
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ELECTRODE: An electrochemistry package for atomistic simulations

Authors: Ludwig J. V. Ahrens-Iwers; Mathijs Janssen; Shern R. Tee; Robert H. Meißner;
APC: 4,065 EUR

ELECTRODE: An electrochemistry package for atomistic simulations

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.

Country
Norway
Keywords

Chemical Physics (physics.chem-ph), Science & Technology, Physics, General Physics and Astronomy, FOS: Physical sciences, Computational Physics (physics.comp-ph), 540, Atomic, Molecular & Chemical, Physical sciences, Chemistry, Engineering, Chemical sciences, Physics - Chemical Physics, Physical, 3100 Physics and Astronomy, Physical and Theoretical Chemistry, 1606 Physical and Theoretical Chemistry, Physics - Computational Physics

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selected citations
These citations are derived from selected sources.
This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Citations provided by BIP!
popularity
This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.
BIP!Popularity provided by BIP!
influence
This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Influence provided by BIP!
impulse
This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.
BIP!Impulse provided by BIP!
84
Top 1%
Top 10%
Top 1%
Green
hybrid