MetalWalls: A Classical Molecular Dynamics Software Dedicated to the Simulation of Electrochemical Systems

Marin-Lafleche, A.; Haefele, Matthieu; Scalfi, Laura; Coretti, Alessandro; Dufils, Thomas; Jeanmairet, Guillaume; Reed, Stewart K.; Serva, Alessandra; Berthin, Roxanne; Bacon, Camille; Bonella, Sara; Rotenberg, Benjamin; Madden, Paul A.; Salanne, Mathieu

doi:10.26434/chemrxiv.12389777.v1

Cited by 38 publications

(43 citation statements)

References 5 publications

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“…A liquid slab composed by 3,481 water molecules between two planar Au(100) surfaces (each electrode made of five layers, 162 Au atoms each) was simulated using the MetalWalls code (41). Three simulations were performed at fixed applied potentials of 0, 1, and 2 V between the electrodes, respectively.…”

Section: Methodsmentioning

confidence: 99%

Size dependence of hydrophobic hydration at electrified gold/water interfaces

Serva

Salanne

Havenith

et al. 2021

Proc. Natl. Acad. Sci. U.S.A.

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Hydrophobic hydration at metal/water interfaces actively contributes to the energetics of electrochemical reactions, e.g. CO2 and N2 reduction, where small hydrophobic molecules are involved. In this work, constant applied potential molecular dynamics is employed to study hydrophobic hydration at a gold/water interface. We propose an adaptation of the Lum–Chandler–Weeks (LCW) theory to describe the free energy of hydrophobic hydration at the interface as a function of solute size and applied voltage. Based on this model we are able to predict the free energy cost of cavity formation at the interface directly from the free energy cost in the bulk plus an interface-dependent correction term. The interfacial water network contributes significantly to the free energy, yielding a preference for outer-sphere adsorption at the gold surface for ideal hydrophobes. We predict an accumulation of small hydrophobic solutes of sizes comparable to CO or N2, while the free energy cost to hydrate larger hydrophobes, above 2.5-Å radius, is shown to be greater at the interface than in the bulk. Interestingly, the transition from the volume dominated to the surface dominated regimes predicted by the LCW theory in the bulk is also found to take place for hydrophobes at the Au/water interface but occurs at smaller cavity radii. By applying the adapted LCW theory to a simple model addition reaction, we illustrate some implications of our findings for electrochemical reactions.

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Section: Methodsmentioning

confidence: 99%

Size dependence of hydrophobic hydration at electrified gold/water interfaces

Serva

Salanne

Havenith

et al. 2021

Proc. Natl. Acad. Sci. U.S.A.

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“…In addition, we will not discuss in detail the possibilities o↵ered by existing open source softwares for the classical molecular simulation of electrochemical interfaces with the methods described in the present review, but refer the reader to the corresponding descriptions of e.g. Metalwalls [79], which is dedicated to the simulation of such interfaces, or more generic simulation packages allowing such simulations (possibly with an open source modification not provided in the standard distribution) such as LAMMPS, OpenMM or ESPRESSO (see [80] for links).…”

Section: How To Simulate Polarized Electrode-solution Interfacesmentioning

confidence: 99%

Molecular Simulation of Electrode-Solution Interfaces

Scalfi

Salanne

Rotenberg

2021

Annu. Rev. Phys. Chem.

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Many key industrial processes, from electricity production, conversion, and storage to electrocatalysis or electrochemistry in general, rely on physical mechanisms occurring at the interface between a metallic electrode and an electrolyte solution, summarized by the concept of an electric double layer, with the accumulation/depletion of electrons on the metal side and of ions on the liquid side. While electrostatic interactions play an essential role in the structure, thermodynamics, dynamics, and reactivity of electrode-electrolyte interfaces, these properties also crucially depend on the nature of the ions and solvent, as well as that of the metal itself. Such interfaces pose many challenges for modeling because they are a place where quantum chemistry meets statistical physics. In the present review, we explore the recent advances in the description and understanding of electrode-electrolyte interfaces with classical molecular simulations, with a focus on planar interfaces and solvent-based liquids, from pure solvent to water-in-salt-electrolytes. Expected final online publication date for the Annual Review of Physical Chemistry, Volume 72 is April 2021. Please see http://www.annualreviews.org/page/journal/pubdates for revised estimates.

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“…At each time step, the simulation computes with a matrix-free conjugate gradient the charge density on electrodes such that they conserve a constant potential which is the heart of the mini-app studied in this paper. Details on the code and references to the model can be found in [29].…”

Section: B Supercapacitor Simulationmentioning

confidence: 99%

EXA2PRO: A Framework for High Development Productivity on Heterogeneous Computing Systems

Papadopoulos

Soudris

Keßler

et al. 2022

IEEE Trans. Parallel Distrib. Syst.

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Programming upcoming exascale computing systems is expected to be a major challenge. New programming models are required to improve programmability, by hiding the complexity of these systems from application developers. The EXA2PRO programming framework aims at improving developers' productivity for applications that target heterogeneous computing systems. It is based on advanced programming models and abstractions that encapsulate low-level platform-specific optimizations and it is supported by a runtime that handles application deployment on heterogeneous nodes. It supports a wide variety of platforms and accelerators (CPU, GPU, FPGAbased Data-Flow Engines), allowing developers to efficiently exploit heterogeneous computing systems, thus enabling more HPC applications to reach exascale computing. The EXA2PRO framework was evaluated using four HPC applications from different domains. By applying the EXA2PRO framework, the applications were automatically deployed and evaluated on a variety of computing architectures, enabling developers to obtain performance results on accelerators, test scalability on MPI clusters and productively investigate the degree by which each application can efficiently use different types of hardware resources.

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MetalWalls: A Classical Molecular Dynamics Software Dedicated to the Simulation of Electrochemical Systems

Cited by 38 publications

References 5 publications

Size dependence of hydrophobic hydration at electrified gold/water interfaces

Size dependence of hydrophobic hydration at electrified gold/water interfaces

Molecular Simulation of Electrode-Solution Interfaces

EXA2PRO: A Framework for High Development Productivity on Heterogeneous Computing Systems

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