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Water molecules are traditionally regarded as passive dielectric media in electrochemical systems. In this work, we challenge this conventional perspective using molecular dynamics simulations and theoretical analysis. We show that…

Chemical Physics · Physics 2025-05-21 Peiyao Wang , Gengping Jiang , Yuan Yan , Longbing Qu , Xiaoyang Du , Dan Li , Jefferson Zhe Liu

Graphite is a ubiquitous electrode material with particular promise for use in e.g., energy storage and desalination devices, but very little is known about the properties of the graphite-electrolyte double layer at technologically relevant…

Materials Science · Physics 2021-09-03 Aaron R. Finney , Ian J. McPherson , Patrick R. Unwin , Matteo Salvalaglio

Electric double layers (EDL) with counterions only, say electrons with the elementary charge $-e$, in thermal equilibrium at the inverse temperature $\beta$ are considered. In particular, we study the effect of the surface charge modulation…

Statistical Mechanics · Physics 2022-07-26 Ladislav Šamaj

We consider equilibrium statistical mechanics of a simplified model for the ideal conductor electrode in an interface contact with a classical semi-infinite electrolyte, modeled by the two-dimensional Coulomb gas of pointlike $\pm$ unit…

Statistical Mechanics · Physics 2009-11-11 L. Samaj , Z. Bajnok

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…

The capacitance of the electric double layer has potential applications in supercapacitors, and theoretical investigations of the double-layer capacitance in binary mixtures are important. In this work, we develop the theory of the electric…

Chemical Physics · Physics 2025-09-01 Yuki Uematsu

To improve the understanding of the relation between electrode curvature and energy storage mechanisms, a systematic investigation of the correlation between convex and concave electrode surfaces and the differential capacitance of an…

Computational Physics · Physics 2020-03-04 Jannes Seebeck , Peter Schiffels , Sabine Schweizer , Jörg-Rüdiger Hill , Robert Horst Meißner

The differential capacitance comprises the most relevant thermodynamic information about an electrochemical system. Classical approaches to describe electrochemical capacitance have difficulties to combine the treatment of the ionic…

Chemical Physics · Physics 2023-02-17 Tobias Binninger

The response of oxide thin films to polar discontinuities at interfaces and surfaces has generated an enormous activity due to the variety of interesting effects it gives rise to. A case in point is the discovery of the electron gas at the…

Mesoscale and Nanoscale Physics · Physics 2014-03-21 N C Bristowe , Philippe Ghosez , P B Littlewood , Emilio Artacho

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

Knowledge of atomic-level details of structure, chemistry, and electronic states is paramount for a comprehensive understanding of emergent properties at oxide interfaces. We utilise a novel methodology based on atomic-scale electron energy…

Electrochemical devices often consist of multicomponent electrolyte solutions. Two processes influence the overall dynamics of these devices: the formation of electrical double layers and chemical conversion due to redox reactions. However,…

Chemical Physics · Physics 2022-06-20 Nathan Jarvey , Filipe Henrique , Ankur Gupta

The electrical double layer for three different topologies of nanopore electrodes is studied, i.e., the interior and exterior electrical double layers of planar, cylindrical and spherical nanopores immersed into a point-ions electrolyte,…

Soft Condensed Matter · Physics 2025-06-10 A. Silva-Caballero , A. Lozada-Hidalgo , M. Lozada-Cassou

We use Monte Carlo simulations to examine the simplest model of an ionic liquid, called the restricted primitive model, at a metal surface. We find that at moderately low temperatures the capacitance of the metal/ionic liquid interface is…

Chemical Physics · Physics 2010-11-19 M. S. Loth , Brian Skinner , B. I. Shklovskii

Progress in electrochemical applications of ionic liquids builds on an understanding of electrical double-layer. This computational study focuses on structure-determined quantities -- maximum packing density, potentials and capacitances --…

It is well-known that room temperature ionic liquids (RTILs) often adopt a charge-separated layered structure, i.e., with alternating cation- and anion-rich layers, at electrified interfaces. However, the dynamic response of the layered…

Recent advances in experimental and computational techniques have allowed for an accurate description of the adsorption of ionic liquids on metallic electrodes. It is now well established that they adopt a multi-layered structure, and that…

Materials Science · Physics 2016-03-15 Benjamin Rotenberg , Mathieu Salanne

We formulate a general mean-field theory of a flat electric double layer in ionic liquids and electrolyte solutions with ions possessing static polarizability and a permanent dipole moment on a charged electrode. We establish a new…

Statistical Mechanics · Physics 2021-08-17 Yu. A. Budkov , S. V. Zavarzin , A. L. Kolesnikov

Two-dimensional electron systems with fascinating properties exist in multilayers of standard semiconductors, on helium surfaces, and in oxides. Compared to the two-dimensional (2D) electron gases of semiconductors, the 2D electron systems…

Strongly Correlated Electrons · Physics 2016-06-22 J. Zabaleta , V. S. Borisov , R. Wanke , H. O. Jeschke , S. C. Parks , B. Baum , A. Teker , T. Harada , K. Syassen , T. Kopp , N. Pavlenko , R. Valentí , J. Mannhart

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…

Chemical Physics · Physics 2018-04-12 Ravishankar Sundararaman , Kendra Letchworth-Weaver , Kathleen Schwarz