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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…

Chemical Physics · Physics 2022-03-10 Abhishek Shandilya , Kathleen Schwarz , Ravishankar Sundararaman

The theory of interfacial properties in liquid-liquid or liquid-vapour systems is nearly 200 years old. The advent of computational tools has greatly advanced the field, mainly through the use of Molecular Dynamics simulations. Despite the…

The surfaces of most metals immersed in aqueous electrolytes have a several-nanometer-thick oxide/hydroxide surface layer. This gives rise to the existence of both metal|oxide and oxide|liquid electrotlyte interfaces, and makes it…

Materials Science · Physics 2022-10-13 Kevin Leung

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

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…

Chemical Physics · Physics 2019-03-22 Thomas Sayer , Michiel Sprik , Chao Zhang

The Poisson Boltzmann equation is known for its success in describing the Debye layer that arises from the charge separation phenomenon at the silica/water interface. However, by treating only the mobile ionic charges in the liquid, the…

Soft Condensed Matter · Physics 2019-07-30 Maijia Liao , Li Wan , Shixin Xu , Chun Liu , Ping Sheng

For a film of liquid on a solid surface, the binding potential $g(h)$ gives the free energy as a function of the film thickness $h$ and also the closely related structural disjoining pressure $\Pi = - \partial g / \partial h$. The wetting…

Soft Condensed Matter · Physics 2018-07-24 Adam P. Hughes , Uwe Thiele , Andrew J. Archer

The properties of the interface between solid and melt are key to solidification and melting, as the interfacial free energy introduces a kinetic barrier to phase transitions. This makes solidification happen below the melting temperature,…

Statistical Mechanics · Physics 2015-12-02 Bingqing Cheng , Gareth A. Tribello , Michele Ceriotti

Water/solid interfaces are relevant to a broad range of physicochemical phenomena and technological processes such as corrosion, lubrication, heterogeneous catalysis and electrochemistry. Although many fields have contributed to rapid…

Materials Science · Physics 2013-01-31 Javier Carrasco , Andrew Hodgson , Angelos Michaelides

The surface or contact potential at the water liquid-vapor interface is discussed in relation to determinations of absolute ion hydration free energies and distributions of ions near the interface. It is shown that, rather than the surface…

Soft Condensed Matter · Physics 2012-09-21 Thomas L. Beck

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

The possibility to extract properties of an interface between two immiscible liquids, e.g., electrolyte solutions or polyelectrolyte multilayers, by means of impedance spectroscopy is investigated theoretically within a dynamic density…

Soft Condensed Matter · Physics 2013-11-22 Andreas Reindl , Markus Bier

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…

Chemical Physics · Physics 2023-11-07 Margherita Buraschi , Andrew P. Horsfield , Clotilde S. Cucinotta

We present a study of the structure and differential capacitance of electric double layers of aqueous electrolytes. We consider Electric Double Layer Capacitors (EDLC) composed of spherical cations and anions in a dielectric continuum…

Soft Condensed Matter · Physics 2021-07-21 Peter Cats , Ranisha S. Sitlapersad , Wouter K. den Otter , Anthony R. Thornton , René van Roij

The influence of a chemically or electrically heterogeneous distribution of interaction sites at a planar substrate on the number density of an adjacent fluid is studied by means of classical density functional theory (DFT). In the case of…

Soft Condensed Matter · Physics 2018-05-25 Maximilian Mußotter , Markus Bier , S. Dietrich

Embedded density functional theory (e-DFT) is used to describe the electronic structure of strongly interacting molecular subsystems. We present a general implementation of the Exact Embedding (EE) method [J. Chem. Phys. 133, 084103 (2010)]…

Other Condensed Matter · Physics 2011-07-27 Jason D. Goodpaster , Taylor A. Barnes , Thomas F. Miller

The work reviews on a general level various modified Poisson-Boltzmann equations and demonstrates their use on the specific system of charged particles at an interface. This system is special, first, because it exhibits the long-range…

Soft Condensed Matter · Physics 2012-11-14 Derek Frydel , Martin Oettel

In the last decade, computational studies of liquid water have mostly concentrated on ground state properties. However recent spectroscopic measurements have been used to infer the structure of water, and the interpretation of optical and…

Materials Science · Physics 2016-08-31 David Prendergast , Jeffrey C. Grossman , Giulia Galli

Understanding the structure and chemical composition at the liquid-nanoparticle (NP) interface is crucial for a wide range of physical, chemical and biological processes. In this study, direct imaging of the liquid-NP interface by atom…

Heterogeneous interfaces are central to many energy-related applications in the nanoscale. From the first-principles electronic structure perspective, one of the outstanding problems is accurately and efficiently calculating how the…

Materials Science · Physics 2023-08-29 Zhen-Fei Liu
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