Efficient electron open boundaries for simulating electrochemical cells
File(s)paper-for-spiral.pdf (616.38 KB)
Accepted version
Author(s)
Zauchner, Mario
Horsfield, AP
todorov, Tchavdar
Type
Journal Article
Abstract
Nonequilibrium electrochemistry raises new challenges for atomistic simulation: we need to perform molecular dynamics for the nuclear degrees of freedom with an explicit description of the electrons, which in turn must be free to enter and leave the computational cell. Here we present a limiting form for electron open boundaries that we expect to apply when the magnitude of the electric current is determined by the drift and diffusion of ions in a solution and which is sufficiently computationally efficient to be used with molecular dynamics. We present tight-binding simulations of a parallel-plate capacitor with nothing, a dimer, or an atomic wire situated in the space between the plates. These simulations demonstrate that this scheme can be used to perform molecular dynamics simulations when there is an applied bias between two metal plates with, at most, weak electronic coupling between them. This simple system captures some of the essential features of an electrochemical cell, suggesting this approach might be suitable for simulations of electrochemical cells out of equilibrium.
Date Issued
2018-01-15
Date Acceptance
2018-01-02
Citation
Physical Review B: Condensed Matter and Materials Physics, 2018, 97 (4), pp.1-1
ISSN
1098-0121
Publisher
American Physical Society
Start Page
1
End Page
1
Journal / Book Title
Physical Review B: Condensed Matter and Materials Physics
Volume
97
Issue
4
Copyright Statement
©2018 American Physical Society
Sponsor
The Leverhulme Trust
Identifier
https://journals.aps.org/prb/abstract/10.1103/PhysRevB.97.045116
Grant Number
RPG-2014-125
Subjects
Science & Technology
Technology
Physical Sciences
Materials Science, Multidisciplinary
Physics, Applied
Physics, Condensed Matter
Materials Science
Physics
ANO BASIS-SETS
02 Physical Sciences
03 Chemical Sciences
09 Engineering
Fluids & Plasmas
Publication Status
Published
Article Number
045116
Date Publish Online
2018-01-12