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Modeling microstructure evolution in electrochemical systems is vital for understanding the mechanism of various electrochemical processes. In this work, we propose a general phase field framework that is fully variational and thus…

Materials Science · Physics 2023-12-12 Jin Zhang , Alexander F. Chadwick , Peter W. Voorhees

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…

Materials Science · Physics 2017-09-13 Céline Merlet , Benjamin Rotenberg , Paul Madden , Mathieu Salanne

Simulating electrified metal/water interfaces with explicit solvent under constant potential is essential for understanding electrochemical processes, yet remains prohibitively expensive with ab initio methods. We present TRECI, a…

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…

Chemical Physics · Physics 2025-07-08 Jia-Xin Zhu , Jun Cheng

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…

Electrolyte solutions play critical role in a vast range of important applications, yet an accurate and scalable method of predicting their properties without fitting to experiment has remained out of reach, despite over a century of…

Chemical Physics · Physics 2024-11-18 Junji Zhang , Joshua Pagotto , Tim Gould , Timothy T. Duignan

Electrochemical interfaces are crucial in catalysis, energy storage, and corrosion, where their stability and reactivity depend on complex interactions between the electrode, adsorbates, and electrolyte. Predicting stable surface structures…

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…

Materials Science · Physics 2023-05-26 Shern Ren Tee , Debra J. Searles

The interfaces between metal electrodes and liquid electrolytes are prototypical in electrochemistry. That is why it is crucial to have a molecular and dynamical understating of such interfaces for both electrical properties and chemical…

Chemical Physics · Physics 2023-10-06 Linnéa Andersson , Chao Zhang

Chemical potential of species in solution is essential for understanding various chemical processes at interfaces. Molecular dynamics (MD) simulations, constrained by fixed compositions, cannot satisfy a constant chemical potential…

Chemical Physics · Physics 2025-06-03 Ademola Soyemi , Khagendra Baral , Tibor Szilvasi

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 reactivity and spectroscopy of aqueous solutions at the atomistic level is crucial for the elucidation and design of chemical processes. However, the simulation of these systems requires addressing the formidable…

Chemical Physics · Physics 2017-02-28 Ondrej Marsalek , Thomas E. Markland

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…

Chemical Physics · Physics 2022-07-29 Ludwig J. V. Ahrens-Iwers , Mathijs Janssen , Shern R. Tee , Robert H. Meißner

Simulation techniques based on accurate and efficient representations of potential energy surfaces are urgently needed for the understanding of complex aqueous systems such as solid-liquid interfaces. Here, we present a machine learning…

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…

Materials Science · Physics 2019-11-13 Thomas Dufils , Guillaume Jeanmairet , Benjamin Rotenberg , Michiel Sprik , Mathieu Salanne

The construction of a reaction network containing all relevant intermediates and elementary reactions is necessary for the accurate description of chemical processes. In the case of a complex chemical reaction (involving, for instance, many…

Chemical Physics · Physics 2017-12-19 Gregor N. Simm , Markus Reiher

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

Reactive chemistry of molecular hydrogen at surfaces, notably dissociative sticking and hydrogen evolution, plays a crucial role in energy storage and fuel cells. Theoretical studies can help to decipher underlying mechanisms and reaction…

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…

Chemical Physics · Physics 2025-06-13 Chaoqiang Feng , Bin Jiang

New computational tools for solid-state synthesis recipe design are needed in order to accelerate the experimental realization of novel functional materials proposed by high-throughput materials discovery workflows. This work contributes a…

Materials Science · Physics 2024-07-30 Max C. Gallant , Matthew J. McDermott , Bryant Li , Kristin A. Persson
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