Related papers: First-principles theory of electrochemical capacit…
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…
The electric double layer is an important structure that appears at charged liquid interfaces, and it determines the performance of various electrochemical devices such as supercapacitors and electrokinetic energy converters. Here the…
We report a detailed theoretical investigation on electrochemical capacitance of a nanoscale capacitor where there is a DC coupling between the two conductors. For this ``leaky'' quantum capacitor, we have derived general analytic…
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…
Time-dependent density-functional theory (TDDFT) is widely used to describe electronic excitations in complex finite systems with large numbers of atoms, such as biomolecules and nanocrystals. The first part of this paper will give a simple…
Understanding the electrical double layer (EDL), i.e, the distribution of electrolyte at an electrified interface, in concentrated electrolytes is important for various technologies, such as supercapacitors, batteries and electrocatalysis.…
The ongoing scientific interest in the properties and structure of electric double layers (EDLs) stems from their pivotal role in (super)capacitive energy storage, energy harvesting, and water treatment technologies. Classical density…
Many references exist in the density functional theory (DFT) literature to the chemical potential of the electrons in an atom or a molecule. The origin of this notion has been the identification of the Lagrange multiplier $\mu = \partial…
Understanding electrochemical interfaces at a microscopic level is essential for elucidating important electrochemical processes in electrocatalysis, batteries and corrosion. While \textit{ab initio} simulations have provided valuable…
As a first step to meet the challenge to calculate the electronic structure and total energy of charged states of atoms and molecules adsorbed on ultrathin-insulating films supported by a metallic substrate using density functional theory…
Controlling electrochemical reactivity requires a detailed understanding of the charging behavior and thermodynamics of the electrochemical interface. Experiments can independently probe the overall charge response of the electrochemical…
Density Functional Theory (DFT) is one of the most widely used methods for "ab initio" calculations of the structure of atoms, molecules, crystals, surfaces, and their interactions. Unfortunately, the customary introduction to DFT is often…
We study the electrode polarization behaviour of different Na-Ca-phosphosilicate glasses by measuring the differential capacitance between blocking Pt electrodes. At low applied dc bias voltages, we detect a linear capacitance regime with…
We propose a new molecular simulation framework that combines the transferability, robustness and chemical flexibility of an ab initio method with the accuracy and efficiency of a machine learned force field. The key to achieve this mix is…
We apply first principles computational techniques to analyze the two-electron, multi-step, electrochemical reduction of CO2 to CO in water using cobalt porphyrin as a catalyst. Density Functional Theory calculations with hybrid functionals…
We present the first application of phase field modeling to electrochemistry. A free energy functional that includes the electrostatic effect of charged particles leads to rich interactions between concentration, electrostatic potential,…
The structure and thickness of the electrical double layer (EDL) at carbon electrodes strongly influence electrochemical performance, yet remain poorly understood in super-concentrated aqueous electrolytes. Here we combine classical and…
A major challenge in modelling interfacial processes in electrochemical (EC) devices is performing simulations at constant potential. This requires an open-boundary description of the electrons, so that they can enter and leave the…
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…
A Poisson-Boltzmann approach is used to determine the double-layer integral and differential capacitances in a finite-length situation for an electrolytic cell. By means of simple analytical calculations, it is shown how these quantities…