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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…

Chemical Physics · Physics 2017-03-01 Ravishankar Sundararaman , Kathleen Schwarz

Understanding the electrodes' surface morphology influence on the ions' distribution is essential for designing the supercapacitors with enhanced energy density characteristics. We develop a model for the structure of electrolytes near the…

Statistical Mechanics · Physics 2021-06-30 Timur Aslyamov , Konstantin Sinkov , Iskander Akhatov

The interactions of ionic liquids (ILs) with organic solutes are of interest to many applications involving the use of ILs as task-specific solvents, such as in sensing devices or catalysis. However, currently little is known about these…

Chemical Physics · Physics 2023-11-06 Clare Xie Yijia , Julian Becker , Tom Welton , Patricia Hunt

Battery electrode surfaces are generally coated with electronically insulating solid films of thickness 1-50 nm. Both electrons and Li+ can move at the electrode-surface film interface in response to the voltage, which adds complexity to…

Materials Science · Physics 2015-07-10 Kevin Leung , Andrew Leenheer

We show that classical molecular density functional theory (MDFT), here in the homogeneous reference fluid approximation in which the functional is inferred from the properties of the bulk solvent, is a powerful new tool to study, at a…

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.…

Soft Condensed Matter · Physics 2026-05-01 Zachary A. H. Goodwin

In this paper for the first time we report the results of molecular dynamics simulation of electrode/electrolyte interface of Li-O2 cathode under potential close to experimental values in 1M dimethyl sulfoxide (DMSO) solution of LiPF6 salt.…

Chemical Physics · Physics 2017-01-10 Artem Sergeev , Alexander Chertovich , Daniil Itkis , Anik Sen , Axel Gross , Alexei Khokhlov

The electrified solid-liquid interface plays an essential role in many renewable energy-related applications, including hydrogen production and utilization. Limitations in computational modelling of the electrified solid-liquid interface…

High electric fields can significantly alter catalytic environments and the resultant chemical processes. Such fields arise naturally in biological systems but can also be artificially induced through localized excitations at nanoscale.…

Understanding the molecular and electronic structure of electrolytes at interfaces requires an analysis of the interactions between the electrode surface, the ions, and the solvent environment on equal footing. Here, we tackle this…

Mesoscale and Nanoscale Physics · Physics 2023-03-16 Christopher Penschke , John Thomas , Cord Bertram , Angelos Michaelides , Karina Morgenstern , Peter Saalfrank , Uwe Bovensiepen

We present the theory and implementation of a Poisson-Boltzmann implicit solvation model for electrolyte solutions. This model can be combined with arbitrary electronic structure methods that provide an accurate charge density of the…

Computational Physics · Physics 2020-01-08 Christopher J. Stein , John M. Herbert , Martin Head-Gordon

Liquid structure at solid-liquid interfaces is critical for many natural and engineered processes ranging from biological signal transduction to electrochemical energy conversion. Advanced experimental and computational methods have…

We introduce a field-theoretic electrolyte model composed of structured solvent molecules and salt ions coupled by electrostatic and hard-core interactions. Within this explicit solvent theory, we characterize the salt-driven dielectric…

Soft Condensed Matter · Physics 2022-06-09 Sahin Buyukdagli

This review describes the theory and implementation of implicit solvation models based on continuum electrostatics. Within quantum chemistry this formalism is sometimes synonymous with the polarizable continuum model, a particular…

Chemical Physics · Physics 2022-03-15 John M. Herbert

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…

Disordered Systems and Neural Networks · Physics 2009-11-11 C. R. Mariappan , T. P. Heins , B. Roling

Implicit electron-density solvation models based on joint density-functional theory offer a computationally efficient solution to the problem of calculating thermodynamic quantities of solvated systems from firstprinciples quantum…

Chemical Physics · Physics 2015-02-12 Deniz Gunceler , T. A. Arias

Recent studies on the solvation of atomistic and nanoscale solutes indicate that a strong coupling exists between the hydrophobic, dispersion, and electrostatic contributions to the solvation free energy, a facet not considered in current…

Statistical Mechanics · Physics 2009-11-11 J. Dzubiella , J. M. J. Swanson , J. A. McCammon

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 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

A wide range of electrochemical reactions of practical importance occur at the interface between a semiconductor and an electrolyte. We present an embedded density-functional theory method using the recently released self-consistent…

Materials Science · Physics 2017-07-21 Quinn Campbell , Ismaila Dabo