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Continuum electrolyte models represent a practical tool to account for the presence of the diffuse layer at electrochemical interfaces. However, despite the increasing popularity of these in the field of materials science it remains unclear…

Computational Physics · Physics 2019-01-18 Francesco Nattino , Matthew Truscott , Nicola Marzari , Oliviero Andreussi

Understanding the response of the surface of metallic solids to external electric field sources is crucial to characterize electrode-electrolyte interfaces. Continuum electrostatics offer a simple description of the induced charge density…

Chemical Physics · Physics 2021-12-14 Giovanni Pireddu , Laura Scalfi , Benjamin Rotenberg

Surfaces are able to control physical-chemical processes in multi-component solution systems and, as such, find application in a wide range of technological devices. Understanding the structure, dynamics and thermodynamics of non-ideal…

Soft Condensed Matter · Physics 2023-09-29 Aaron R. Finney , Matteo Salvalaglio

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…

Materials Science · Physics 2019-11-13 Thomas Dufils , Guillaume Jeanmairet , Benjamin Rotenberg , Michiel Sprik , Mathieu Salanne

Ionic liquids are widely used as electrolytes in electrochemical devices. In this context, many experimental and theoretical approaches have been recently developed for characterizing their interface with electrodes. In this perspective…

Materials Science · Physics 2017-09-13 Céline Merlet , Benjamin Rotenberg , Paul Madden , Mathieu Salanne

Many key industrial processes, from electricity production, conversion and storage to electrocatalysis or electrochemistry in general, rely on physical mechanisms occurring at the interface between a metallic electrode and an electrolyte…

Computational Physics · Physics 2021-09-03 Laura Scalfi , Mathieu Salanne , Benjamin Rotenberg

Modelling electrolytes accurately on both a nanoscale and cell level can contribute to improving battery chemistries.[Armand and Tarascon, Nature, 2008, 451, 652-657] We previously presented a thermodynamic continuum model for…

Chemical Physics · Physics 2024-08-09 Constantin Schwetlick , Max Schammer , Arnulf Latz , Birger Horstmann

A diffuse interface (phase field) model for an electrochemical system is developed. We describe the minimal set of components needed to model an electrochemical interface and present a variational derivation of the governing equations. With…

Materials Science · Physics 2007-05-23 J. E. Guyer , W. J. Boettinger , J. A. Warren , G. B. McFadden

Electrochemical interfaces are of fundamental importance in electrocatalysis, batteries, and metal corrosion. Finite-field methods are one of most reliable approaches for modeling electrochemical interfaces in complete cells under realistic…

Chemical Physics · Physics 2025-06-13 Chaoqiang Feng , Bin Jiang

A kinetic model of the electron transfer at the electrode / electrolyte solution interface is developed, implemented in a Monte Carlo framework, and applied to simulate this process in idealised systems consisting of the primitive model of…

A crucial aspect in the simulation of electrochemical interfaces consists in treating the distribution of electronic charge of electrode materials that are put in contact with an electrolyte solution. Recently, it has been shown how a…

Materials Science · Physics 2024-07-16 Andrea Grisafi , Mathieu Salanne

Surface charge controls many static and dynamic properties of soft matter and micro/nanofluidic systems, but its unambiguous measurement forms a challenge. Standard characterization methods typically probe an effective surface charge, which…

Soft Condensed Matter · Physics 2018-08-28 Remco Hartkamp , Anne-Laure Biance , Li Fu , Jean-François Dufrêche , Oriane Bonhomme , Laurent Joly

We present a simulation method to study electrolyte solutions in a dielectric slab geometry using a modified 3D Ewald summation. The method is fast and easy to implement, allowing us to rapidly resum an infinite series of image charges. In…

Soft Condensed Matter · Physics 2015-08-12 Alexandre P. dos Santos , Yan Levin

Electrochemical interfaces are crucial in catalysis, energy storage, and corrosion, where their stability and reactivity depend on complex interactions between the electrode, adsorbates, and electrolyte. Predicting stable surface structures…

We review recent ab initio molecular dynamics studies of electrode/electrolyte interfaces in lithium ion batteries. Our goals are to introduce experimentalists to simulation techniques applicable to models which are arguably most faithful…

Materials Science · Physics 2013-04-23 Kevin Leung

Reliable first-principles calculations of electrochemical processes require accurate prediction of the interfacial capacitance, a challenge for current computationally-efficient continuum solvation methodologies. We develop a model for the…

Chemical Physics · Physics 2018-04-12 Ravishankar Sundararaman , Kendra Letchworth-Weaver , Kathleen Schwarz

The ion distribution of electrolytes near interfaces with dielectric contrast has important consequences for electrochemical processes and many other applications. To date, most studies of such systems have focused on geometrically simple…

Soft Condensed Matter · Physics 2018-11-14 Huanxin Wu , Honghao Li , Francisco J. Solis , Monica Olvera de la Cruz , Erik Luijten

Implicit solvation is an effective, highly coarse-grained approach in atomic-scale simulations to account for a surrounding liquid electrolyte on the level of a continuous polarizable medium. Originating in molecular chemistry with finite…

Chemical Physics · Physics 2021-08-06 Stefan Ringe , Nicolas G. Hörmann , Harald Oberhofer , Karsten Reuter

Many important applications of electronic structure methods involve molecules or solid surfaces in a solvent medium. Since explicit treatment of the solvent in such methods is usually not practical, calculations often employ continuum…

Chemical Physics · Physics 2015-02-12 Ravishankar Sundararaman , William A. Goddard

High-concentration aqueous electrolytes have shown promise as candidates for a safer, lower-cost battery system. Ionic conductivity is a key property required in high performing electrolytes; the Advanced Electrolyte Model (AEM) has…

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