相关论文: Brownian dynamics simulations of electric double-l…

We present a study of the structure and differential capacitance of electric double layers of aqueous electrolytes. We consider Electric Double Layer Capacitors (EDLC) composed of spherical cations and anions in a dielectric continuum…

Spurred by the increasing needs in electrochemical energy storage devices, the electrode/electrolyte interface has received a lot of interest in recent years. Molecular dynamics simulations play a proeminent role in this field since they…

We study the charge induced in a Thomas-Fermi metal by an ion in vacuum, using an atomistic description employed in constant-potential molecular dynamics simulations, and compare the results with the predictions from continuum…

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…

Classical molecular dynamics simulations have recently become a standard tool for the study of electrochemical systems. State-of-the-art approaches represent the electrodes as perfect conductors, modelling their responses to the charge…

We formulate a time-dependent density functional theory for the coupled dynamics of electrons and nuclei that goes beyond the Born-Oppenheimer (BO) approximation. We prove that the time-dependent marginal nuclear probability density…

Of relevance to energy storage, electrochemistry and catalysis, ionic and dipolar liquids display unexpected behaviours-especially in confinement. Beyond adsorption, over-screening and crowding effects, experiments have highlighted novel…

In order to obtain a reasonably accurate and easily implemented approach to many-electron calculations, we will develop a new Density Functional Theory (DFT). Specifically, we derive an approximation to electron density, the first term of…

Electric double layer supercapacitors are a fast-rising class of high-power energy storage devices based on porous electrodes immersed in a concentrated electrolyte or ionic liquid. As of yet there is no microscopic theory to describe their…

The structure of the double-layer formed at the surface of carbon electrodes is governed by the interactions between the electrode and the electrolyte species. However, carbon is notoriously difficult to simulate accurately, even with…

We investigate the coupled dynamics of concentration and charge in asymmetric 1:1 electrolytes, focusing on the interplay between diffusion asymmetry and external electric fields. Using Brownian dynamics simulations and linearized…

The geometric properties of $\mathrm{Pb-MnO_2}$ composite electrodes are studied, and a general formula is presented for the length of the triple phase boundary (TPB) on two dimensional (2D) composite electrodes using sphere packing and…

The electrostatic screening length predicted by Debye-H\"uckel theory decreases with increasing ionic strength, but recent experiments have found that the screening length can instead increase in concentrated electrolytes. This phenomenon,…

Using Brownian dynamics simulations, we investigate the effects of confinement, adsorption on surfaces and ion-ion interactions on the response of confined electrolyte solutions to oscillating electric fields in the direction perpendicular…

We present a comparative study of two computer simulation methods to obtain static and dynamic properties of dilute polymer solutions. The first approach is a recently established hybrid algorithm based upon dissipative coupling between…

Ion partitioning between different compartments (\emph{e.g.} a porous material and a bulk solution reservoir), known as Donnan equilibrium, plays a fundamental role in various contexts such as energy, environment, or water treatment. The…

Using the Wentzel-Kramers-Brillouin method, we derive a modified form of the Thomas-Fermi approximation to electron density. This new result enables us to calculate the details of the self-consistent ion cores, as well as the ionization…

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…

In Born-Oppenheimer molecular dynamics (BOMD) simulations based on density functional theory (DFT), the potential energy and the interatomic forces are calculated from an electronic ground state density that is determined by an iterative…

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…