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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…
Density Functional Theory (DFT) calculations of electrode material properties in high energy density storage devices like lithium batteries have been standard practice for decades. In contrast, DFT modelling of explicit interfaces in…
The ab-initio computational treatment of electrochemical systems requires an appropriate treatment of the solid/liquid interfaces. A fully quantum mechanical treatment of the interface is computationally demanding due to the large number of…
Solid-liquid interfaces are at the heart of many modern-day technologies and provide a challenge to many materials simulation methods. A realistic first-principles computational study of such systems entails the inclusion of solvent…
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…
Surfaces of ionic solids interacting with an ionic solution can build up charge by exchange of ions. The surface charge is compensated by a strip of excess charge at the border of the electrolyte forming an electric double layer. These…
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…
The distribution of ions at the air/water interface plays a decisive role in many natural processes. It is generally understood that polarizable ions with low charge density are surface-active, implying they sit on top of the water surface.…
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…
Density functional theory is used to describe electrolyte solutions in contact with electrodes of planar or spherical shape. For the electrolyte solutions we consider the so-called civilized model, in which all species present are treated…
The electrical double layer (EDL) at aqueous solution-metal oxide interfaces critically affects many fundamental processes in electrochemistry, geology and biology, yet understanding its microscopic structure is challenging for both theory…
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…
Electrical double layers play a key role in a variety of electrochemical systems. The mean free path of secondary electrons in aqueous solutions is on the order of a nanometer, making them suitable for probing of ultrathin electrical double…
A numerical method using implicit surface representations is proposed to solve the linearized Poisson-Boltzmann equations that arise in mathematical models for the electrostatics of molecules in solvent. The proposed method used an implicit…
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…
The standard Maxwell formulation of the problem of polarized dielectrics suffers from a number of difficulties, both conceptual and practical. These difficulties are particularly significant in the case of liquid interfaces, where the…
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…
A level-set method is developed for numerically capturing the equilibrium solute-solvent interface that is defined by the recently proposed variational implicit solvent model (Dzubiella, Swanson, and McCammon, Phys. Rev. Lett. {\bf 104},…
Tasker type III polar terminations of ionic crystals carry a net surface charge as well as a dipole moment and are fundamentally unstable. In contact with electrolytes, such polar surfaces can be stabilized by adsorption of counter ions…
Recent measurements of microsphere interactions in diverse media suggest that the standard dielectric-continuum models of solution-phase interactions are fundamentally incomplete. Experiments indicate that the interactions of charged…