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A crucial aspect in the simulation of electrochemical interfaces consists in treating the distribution of electronic charge of electrode materials that are put in contact with an electrolyte solution. Recently, it has been shown how a…

Materials Science · Physics 2024-07-16 Andrea Grisafi , Mathieu Salanne

We introduce a local machine-learning method for predicting the electron densities of periodic systems. The framework is based on a numerical, atom-centred auxiliary basis, which enables an accurate expansion of the all-electron density in…

Chemical Physics · Physics 2021-11-10 Alan M. Lewis , Andrea Grisafi , Michele Ceriotti , Mariana Rossi

We introduce a new functional for simulating ground-state and time-dependent electronic systems within density-functional theory. The functional combines an expression for the exact Kohn-Sham (KS) potential in the limit of complete electron…

Mesoscale and Nanoscale Physics · Physics 2021-01-15 M. J. P. Hodgson , J. D. Ramsden , T. R. Durrant , R. W. Godby

A current challenge in atomistic machine learning is that of efficiently predicting the response of the electron density under electric fields. We address this challenge with symmetry-adapted kernel functions that are specifically derived…

Materials Science · Physics 2025-02-26 Mariana Rossi , Kevin Rossi , Alan M. Lewis , Mathieu Salanne , Andrea Grisafi

The electron density of a molecule or material has recently received major attention as a target quantity of machine-learning models. A natural choice to construct a model that yields transferable and linear-scaling predictions is to…

Chemical Physics · Physics 2022-06-29 Andrea Grisafi , Alan M. Lewis , Mariana Rossi , Michele Ceriotti

Electron density is a fundamental quantity, which can in principle determine all ground state electronic properties of a given system. Although machine learning (ML) models for electron density based on either an atom-centered basis or a…

Chemical Physics · Physics 2024-10-08 Chaoqiang Feng , Yaolong Zhang , Bin Jiang

The Kohn-Sham scheme of density functional theory is one of the most widely used methods to solve electronic structure problems for a vast variety of atomistic systems across different scientific fields. While the method is fast relative to…

Understanding the response of the surface of metallic solids to external electric field sources is crucial to characterize electrode-electrolyte interfaces. Continuum electrostatics offer a simple description of the induced charge density…

Chemical Physics · Physics 2021-12-14 Giovanni Pireddu , Laura Scalfi , Benjamin Rotenberg

In simulations of metallic interfaces, a critical aspect of metallic behavior is missing from the some of the most widely used classical molecular dynamics force fields. We present a modification of the embedded atom method (EAM) which…

Materials Science · Physics 2019-04-02 Hemanta Bhattarai , Kathie E. Newman , J. Daniel Gezelter

In this paper, we investigate the energy minimization model of the ensemble Kohn-Sham density functional theory for metallic systems, in which a pseudo-eigenvalue matrix and a general smearing approach are involved. We study the invariance…

Numerical Analysis · Mathematics 2022-01-19 Xiaoying Dai , Stefano de Gironcoli , Bin Yang , Aihui Zhou

Spurred by the increasing needs in electrochemical energy storage devices, the electrode/electrolyte interface has received a lot of interest in recent years. Molecular dynamics simulations play a proeminent role in this field since they…

Materials Science · Physics 2021-05-17 Laura Scalfi , Thomas Dufils , Kyle Reeves , Benjamin rotenberg , Mathieu Salanne

One of the most powerful strategies to address properties of real many-body systems is to incorporate data obtained for models, for example, to use data of the homogeneous electron gas in order to build the Local Density Approximation for…

Materials Science · Physics 2026-05-05 Muhammed Hüseyin Güneş , Ayoub Aouina , Vitaly Gorelov , Matteo Gatti , Lucia Reining

Electron charge density distribution of materials is one of the key quantities in computational materials science as theoretically it determines the ground state energy and practically it is used in many materials analyses. However, the…

Computational Physics · Physics 2019-11-13 Sheng Gong , Tian Xie , Taishan Zhu , Shuo Wang , Eric R. Fadel , Yawei Li , Jeffrey C. Grossman

Electrochemical energy storage always involves the capacitive process. The prevailing electrode model used in the molecular simulation of polarizable electrode-electrolyte systems is the Siepmann-Sprik model developed for perfect metal…

Materials Science · Physics 2023-10-03 Thomas Dufils , Lisanne Knijff , Yunqi Shao , Chao Zhang

We present a local and transferable machine learning approach capable of predicting the real-space density response of both molecules and periodic systems to external homogeneous electric fields. The new method, SALTER, builds on the…

Chemical Physics · Physics 2023-07-19 Alan M Lewis , Paolo Lazzaroni , Mariana Rossi

The structural evolution of laser-excited systems of gold has previously been measured through ultrafast MeV electron diffraction. However, there has been a long-standing inability of atomistic simulations to provide a consistent picture of…

Materials Science · Physics 2024-06-19 J. M. Molina , T. G. White

Electron charge density is a fundamental physical quantity, determining various properties of matter. In this study, we have proposed a deep-learning model for accurate charge density prediction. Our model naturally preserves physical…

Materials Science · Physics 2023-09-27 Taoyuze Lv , Zhicheng Zhong , Yuhang Liang , Feng Li , Jun Huang , Rongkun Zheng

The density functional approach in the Kohn-Sham approximation is widely used to study properties of many-electron systems. Due to the nonlinearity of the Kohn-Sham equations, the general self-consistence searching method involves…

Materials Science · Physics 2015-05-13 D. V. Posvyanskii , A. Ya. Shul'man

A long-standing puzzle in density-functional theory is the issue of the long-range behavior of the Kohn-Sham exchange-correlation potential at metal surfaces. As an important step towards its solution, it is proved here, through a rigurouos…

Materials Science · Physics 2015-05-18 C. M. Horowitz , C. R. Proetto , J. M. Pitarke

Two of the most widely used electronic structure theory methods, namely Hartree-Fock and Kohn-Sham density functional theory, both requires the iterative solution of a set of Schr\"odinger-like equations. The speed of convergence of such…

Chemical Physics · Physics 2024-06-06 S. Hazra , U. Patil , S. Sanvito
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