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The water/electrode interface under an applied bias potential is a challenging out-of-equilibrium phenomenon, which is difficult to accurately model at the atomic scale. In this study, we employ a combined approach of Density Functional…

Materials Science · Physics 2025-03-14 Graciele M. Arvelos , Marivi Fernández-Serra , Alexandre R. Rocha , Luana S. Pedroza

The nanoscopic mass and charge distribution within the double layer at electrified interfaces plays a key role in electrochemical phenomena of huge technological relevance for energy production and conversion. However, in spite of its…

Chemical Physics · Physics 2019-05-29 Remi Khatib , Ashwinee Kumar , Stefano Sanvito , Marialore Sulpizi , Clotilde S. Cucinotta

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…

Chemical Physics · Physics 2019-12-12 Guillaume Jeanmairet , Benjamin Rotenberg , Daniel Borgis , Mathieu Salanne

Density Functional Theory (DFT) calculations of electrode material properties in high energy density storage devices like lithium batteries have been standard practice for decades. In contrast, DFT modelling of explicit interfaces in…

Materials Science · Physics 2020-06-24 Kevin Leung

Unraveling the atomistic and the electronic structure of solid-liquid interfaces is the key to the design of new materials for many important applications, from heterogeneous catalysis to battery technology. Density functional theory (DFT)…

Materials Science · Physics 2022-01-25 Marco Eckhoff , Jörg Behler

Accurate ab initio modelling of surfaces and interfaces, especially under an applied external potential bias, is important for describing and characterizing various phenomena that occur in electronic, catalytic, and energy storage devices.…

Materials Science · Physics 2025-06-10 Kartick Ramakrishnan , Gopalakrishnan Sai Gautam , Phani Motamarri

Understanding the local structure of water at the interfaces of metallic electrodes is a key problem in aqueous-based electrochemistry. Nevertheless, a realistic simulation of such setup is challenging, particularly when the electrodes are…

The electric double layer (EDL) governs electrocatalysis, energy conversion, and storage, yet its atomic structure, capacitance, and reactivity remain elusive. Here we introduce a machine learning interatomic potential framework that…

Chemical Physics · Physics 2025-09-18 Xiaoyu Wang , Junmin Chen , Zezhu Zeng , Frederick Stein , Junho Lim , Bingqing Cheng

Platinum step edges dominate electrocatalytic activity in fuel cells and electrolysers, yet their atomistic electrochemical behaviour remains poorly understood. Here, we employ \textit{ab initio} molecular dynamics under controlled…

Materials Science · Physics 2025-10-15 Matthew T. Darby , Muhammad Saleh , Marialore Sulpizi , Clotilde S. Cucinotta

The ab-initio computational treatment of electrochemical systems requires an appropriate treatment of the solid/liquid interfaces. A fully quantum mechanical treatment of the interface is computationally demanding due to the large number of…

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…

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…

Chemical Physics · Physics 2021-09-23 Yuki Uematsu

First-principles simulations of electronic properties of hybrid inorganic/organic interfaces are challenging, as common density-functional theory (DFT) approximations target specific material classes like bulk semiconductors or gas-phase…

Materials Science · Physics 2023-02-13 Jannis Krumland , Caterina Cocchi

An accurate prediction of the surface potential at the air-water interface is critical to calculating ion hydration free energies and electrochemical half-cell potentials. Using Density Functional Theory (DFT), model interfacial…

Materials Science · Physics 2010-09-22 Kevin Leung

The electrical double layer (EDL) at aqueous solution-metal oxide interfaces critically affects many fundamental processes in electrochemistry, geology and biology, yet understanding its microscopic structure is challenging for both theory…

Implicit solvation is an effective, highly coarse-grained approach in atomic-scale simulations to account for a surrounding liquid electrolyte on the level of a continuous polarizable medium. Originating in molecular chemistry with finite…

Chemical Physics · Physics 2021-08-06 Stefan Ringe , Nicolas G. Hörmann , Harald Oberhofer , Karsten Reuter

Surfaces of metal oxides at working conditions are usually electrified due to the acid-base chemistry. The charged interface compensated with counterions forms the so-called electric double layer. The coupling of surface chemistry and…

Soft Condensed Matter · Physics 2019-07-02 Chao Zhang , Jürg Hutter , Michiel Sprik

It has been widely reported that as water contacts hydrophobic materials such as air or hydrocarbons (liquid or solid), the interfaces acquire a negative charge. It is not entirely clear whether this occurs due to the nature of water, or…

Soft Condensed Matter · Physics 2025-09-15 Yinfeng Xu , Himanshu Mishra

The electric double layer is an important structure that appears at charged liquid interfaces, and it determines the performance of various electrochemical devices such as supercapacitors and electrokinetic energy converters. Here the…

Soft Condensed Matter · Physics 2023-08-15 Haruto Iwasaki , Yasuyuki Kimura , Yuki Uematsu

We assess the capabilities of hydrodynamic density functional theory (DFT) to predict mass transfer across vapor-liquid interfaces by studying the response of an initially equilibrated pure component vapor-liquid system to the localized…

Chemical Physics · Physics 2025-07-08 B. Bursik , F. Bender , R. Stierle , G. Bauer , J. Gross
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