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We report a new Quantum Mechanical/Molecular Dynamics (QM/MD) simulation loop to model the coupling between the electron and atom dynamics in solid/liquid interfacial systems. The method can describe simultaneously both the quantum…

材料科学 · 物理学 2021-02-03 Joshua D Elliott , Alessandro Troisi , Paola Carbone

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…

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…

材料科学 · 物理学 2021-09-03 Aaron R. Finney , Ian J. McPherson , Patrick R. Unwin , Matteo Salvalaglio

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…

软凝聚态物质 · 物理学 2023-09-29 Aaron R. Finney , Matteo Salvalaglio

A major challenge in the molecular simulation of electric double layer capacitors (EDLCs) is the choice of an appropriate model for the electrode. Typically, in such simulations the electrode surface is modeled using a uniform fixed charge…

计算物理 · 物理学 2015-06-22 Zhenxing Wang , Yang Yang , David L. Olmsted , Mark Asta , Brian B. Laird

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…

材料科学 · 物理学 2023-05-26 Shern Ren Tee , Debra J. Searles

Whether or not specific ion effects determine the charge storage properties of aqueous graphene and graphite-based supercapacitors remains a highly debated topic. In this work we present a multiscale quantum mechanics classical molecular…

材料科学 · 物理学 2022-11-10 Joshua D. Elliott , Mara Chiricotto , Alessandro Troisi , Paola Carbone

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…

化学物理 · 物理学 2019-12-12 Guillaume Jeanmairet , Benjamin Rotenberg , Daniel Borgis , Mathieu Salanne

Molecular dynamics (MD) simulations of complex electrochemical systems, such as ionic liquid supercapacitors, are increasingly including the constant potential method (CPM) to model conductive electrodes at specified potential difference,…

材料科学 · 物理学 2022-05-13 Shern R. Tee , Debra J. Searles

Ionic liquids (IL) are promising electrolytes for electrochemical applications due to their remarkable stability and high charge density. Molecular dynamics simulations are essential for better understanding the complex phenomena occurring…

Increasing the energy density in electric double layer capacitors (EDLCs), also known as supercapacitors, remains an active area of research. Specifically, there is a need to design and discover electrode and electrolyte materials with…

软凝聚态物质 · 物理学 2022-10-25 Tarun Maity , Mounika Gosika , Tod A. Pascal , Prabal K. Maiti

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…

材料科学 · 物理学 2017-09-13 Céline Merlet , Benjamin Rotenberg , Paul Madden , Mathieu Salanne

Electrical double layers play a key role in a variety of electrochemical systems. The mean free path of secondary electrons in aqueous solutions is on the order of a nanometer, making them suitable for probing of ultrathin electrical double…

We study the ground-state properties of a double layer graphene system with the Coulomb interlayer electron-electron interaction modeled within the random phase approximation. We first obtain an expression of the quantum capacitance of a…

材料科学 · 物理学 2017-09-06 Fariborz Parhizgar , Alireza Qaiumzadeh , Reza Asgari

Supercapacitors store energy via the formation of an electric double layer, which generates a strong electric field at the electrode-electrolyte interface. Unlike conventional metallic electrodes, graphene-derived materials suffer from a…

材料科学 · 物理学 2015-03-12 Maxwell D. Radin , Tadashi Ogitsu , Minoru Otani , Juergen Biener , Brandon C. Wood

Graphene quantum dots (GQDs) represent single layers up to dozens of graphene layers smaller than 30 nm. GQDs are newish molecules that have aroused great interest in research because of their exceptional and manageable optical, electrical,…

材料科学 · 物理学 2021-01-20 Setianto Setianto , Liu Kin Men , Camellia Panatarani , I Made Joni

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…

The structure and thickness of the electrical double layer (EDL) at carbon electrodes strongly influence electrochemical performance, yet remain poorly understood in super-concentrated aqueous electrolytes. Here we combine classical and…

The influence of hydrated cation-{\pi} interaction forces on the adsorption and filtration capabilities of graphene-based membrane materials is significant. However, the lack of interaction potential between hydrated Cs+ and graphene limits…

计算物理 · 物理学 2024-12-02 Yangjun Qin , Liuhua Mu , Xiao Wan , Zhicheng Zong , Tianhao Li , Nuo Yang

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…

化学物理 · 物理学 2022-07-29 Ludwig J. V. Ahrens-Iwers , Mathijs Janssen , Shern R. Tee , Robert H. Meißner
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