Related papers: Mass-zero constrained molecular dynamics for elect…
We revisit the statistical mechanics of charge fluctuations in capacitors. In constant-potential classical molecular simulations, the atomic charge of electrode atoms are treated as additional degrees of freedom which evolve in time so as…
Constant potential method molecular dynamics simulation (CPM MD) enables the accurate modelling of atomistic electrode charges when studying the electrode-electrolyte interface at the nanoscale. Here we extend the theoretical framework of…
Charged systems interacting via Coulomb forces can be efficiently simulated by introducing a local, diffusing degree of freedom for the electric field. This paper formulates the continuum electrodynamic equations corresponding to the…
A new molecular dynamics model in which the point charges on atomic sites are allowed to fluctuate in response to the environment is developed and applied to water. The idea for treating charges as variables is based on the concept of…
Fluctuating-charge models are computationally efficient methods of treating polarization and charge-transfer phenomena in molecular mechanics and classical molecular dynamics simulations. They are also theoretically appealing as they are…
A better understanding of interfacial mechanisms is needed to improve the performances of electrochemical devices. Yet, simulating an electrode surface at fixed electrolyte composition remains a challenge. Here we apply a finite electric…
Molecular dynamics simulations at a constant electric potential are an essential tool to study electrochemical processes, providing microscopic information on the structural, thermodynamic, and dynamical properties. Despite the numerous…
We study the mobility of a charged colloidal particle in a constant homogeneous electric field by means of computer simulations. The simulation method combines a lattice Boltzmann scheme for the fluid with standard Langevin dynamics for the…
The results of molecular dynamics simulations of the properties of water in an aqueous ionic solution close to an interface with a model metallic electrode are described. In the simulations the electrode behaves as an ideally polarizable…
Constant potential methods (CPM) enable computationally efficient simulations of the solid-liquid interface at conducting electrodes in molecular dynamics (MD). They have been successfully used, for example, to realistically model the…
A major challenge in the molecular simulation of electric double layer capacitors (EDLCs) is the choice of an appropriate model for the electrode. Typically, in such simulations the electrode surface is modeled using a uniform fixed charge…
The fluctuations of the charge on an electrode contain information on the microscopic correlations within the adjacent fluid and their effect on the electronic properties of the interface. We investigate these fluctuations using molecular…
We present a plane-wave basis set implementation of charge constrained density functional molecular dynamics (CDFT-MD) for simulation of electron transfer reactions in condensed phase systems. Following earlier work of Wu et al. Phys. Rev.…
Rechargeable battery electrodes have highly complex microstructures, consisting of nonuniform electrode particles, tortuous electrolyte channels, and irregular particle-electrolyte interfaces. Moreover, the electrochemical processes involve…
The frequency-dependent impedance is a fundamental property of electrical components. We show that it can be determined from the equilibrium dynamical fluctuations of the electrode charge in constant-potential molecular simulations,…
Constant potential molecular dynamics simulation plays important role for applications of electrochemical systems, yet the calculation of charge fluctuation on electrodes remains a computational bottleneck. We propose a highly scalable,…
The constant potential molecular dynamics simulation method proposed by Siepmann and Sprik and reformulated later by Reed (SR-CPM) has been widely employed to investigate the metallic electrolyte/electrode interfaces, especially for…
We present a broad family of high-order finite element algorithms for simulating the flow of electroneutral electrolytes. The governing partial differential equations that we solve are the electroneutral…
Using molecular dynamics simulation, we investigate transport properties of a classical two-dimensional electron system confined in a microchannel with a narrow constriction. As a function of the confinement strength of the constriction,…
Electrochemical energy storage always involves the capacitive process. The prevailing electrode model used in the molecular simulation of polarizable electrode-electrolyte systems is the Siepmann-Sprik model developed for perfect metal…