Related papers: Interfacial water asymmetry at ideal electrochemic…
Most of the performances of electrochemical devices are governed by molecular processes taking place at the solution-electrode interfaces and molecular simulation are the main way to study these processes. Aqueous electrochemical systems…
Manipulation of the charge of the dielectric interface between two bulk liquids not only enables the adjustment of the interfacial tension but also controls the storage capacity of ions in the ionic double layers adjacent to each side of…
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…
The distribution of electric fields within the electrochemical double layer depends on both the electrode and electrolyte in complex ways. These fields strongly influence chemical dynamics in the electrode-electrolyte interface, but cannot…
Why kinetically stable oil droplets in water spontaneously acquire a negative charge remains one of the most vigorously debated questions in interfacial science. Here, we combine neural-network based deep potential molecular dynamics with a…
How does an electrochemical interface respond to changes in the electrode potential? How does the response affect the key properties of the system - energetics, excess charge, capacitance? Essential questions key to ab-initio simulations of…
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…
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…
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…
The renewable energy sector critically needs low-cost and environmentally neutral energy storage solutions throughout the entire device life cycle. However, the limited performance of standard water-based electrochemical systems prevents…
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…
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…
Understanding the performance of electrochemical energy storage systems requires probing the electrochemical properties at each layer and interface during cell operation. While traditional onboard and operando methods can measure impedance,…
Ab initio modeling of electrochemical systems is becoming a key tool for understanding and predicting electrochemical behavior. Development and careful benchmarking of computational electrochemical methods are essential to ensure their…
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…
The surface charge of a water interface determines many fundamental processes in physical chemistry and interface science, and it has been intensively studied for over a hundred years. We summarize experimental methods to characterize the…
While first-principles calculations of electrode-molecule binding play an indispensable role in obtaining atomic-level understanding in surface science and electrochemistry, a significant challenge remains because the adsorption energy is…
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…
Charge hydration asymmetry (CHA)--a characteristic dependence of hydration free energy on the sign of the solute charge--quantifies the asymmetric response of water to electric field at microscopic level. Accurate estimates of CHA are…
We present the coupling of two frameworks -- the pseudo-open boundary simulation method known as constant potential Molecular Dynamics simulations (C$\mu$MD), combined with QMMD calculations -- to describe the properties of graphene…