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We propose a new molecular simulation framework that combines the transferability, robustness and chemical flexibility of an ab initio method with the accuracy and efficiency of a machine learned force field. The key to achieve this mix is…

Computational Physics · Physics 2020-01-08 Sebastian Dick , Marivi Fernandez-Serra

Machine learning has emerged as a powerful tool for predicting molecular properties in chemical reaction networks with reduced computational cost. However, accurately predicting energies of transition state (TS) structures remains a…

Chemical Physics · Physics 2025-04-29 Stefan Gugler , Markus Reiher

Two types of approaches to modeling molecular systems have demonstrated high practical efficiency. Density functional theory (DFT), the most widely used quantum chemical method, is a physical approach predicting energies and electron…

Chemical Physics · Physics 2020-03-02 Anton V. Sinitskiy , Vijay S. Pande

Computational chemistry has come a long way over the course of several decades, enabling subatomic level calculations particularly with the development of Density Functional Theory (DFT). Recently, machine-learned potentials (MLP) have…

Machine learning techniques have found their way into computational chemistry as indispensable tools to accelerate atomistic simulations and materials design. In addition, machine learning approaches hold the potential to boost the…

Chemical Physics · Physics 2025-10-03 Johannes Voss

Simulating water from first principles remains a significant computational challenge due to the slow dynamics of the underlying system. Although machine-learned interatomic potentials (MLPs) can accelerate these simulations, they often fail…

Chemical Physics · Physics 2026-01-30 Tobias Hilpert , Georg Kresse

The properties of electrons in matter are of fundamental importance. They give rise to virtually all molecular and material properties and determine the physics at play in objects ranging from semiconductor devices to the interior of giant…

Simulating liquid water to an accuracy that matches its wealth of available experimental data requires both precise electronic structure methods and reliable sampling of nuclear (quantum) motion. This is challenging because applying the…

Standard forms of density-functional theory (DFT) have good predictive power for many materials, but are not yet fully satisfactory for solid, liquid and cluster forms of water. We use a many-body separation of the total energy into its…

Materials Science · Physics 2013-03-05 M. J. Gillan , D. Alfè , A. P. Bartók , G. Csányi

We study a generalization performance of the machine learning (ML) model to predict the atomic forces within the density functional theory (DFT). The targets are the Si and Ge single component systems in the liquid state. To train the…

Computational Physics · Physics 2019-03-27 Ryo Tamura , Jianbo Lin , Tsuyoshi Miyazaki

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

Density functional theory (DFT) is one of the main methods in Quantum Chemistry that offers an attractive trade off between the cost and accuracy of quantum chemical computations. The electron density plays a key role in DFT. In this work,…

Chemical Physics · Physics 2018-09-11 Anton V. Sinitskiy , Vijay S. Pande

The accuracy of the training data limits the accuracy of bulk properties from machine-learned potentials. For example, hybrid functionals or wave-function-based quantum chemical methods are readily available for cluster data but effectively…

Computational Physics · Physics 2023-12-05 Viktor Zaverkin , David Holzmüller , Robin Schuldt , Johannes Kästner

Obtaining the atomistic structure and dynamics of disordered condensed phase systems from first principles remains one of the forefront challenges of chemical theory. Here we exploit recent advances in periodic electronic structure to show…

The ground state electron density -- obtainable using Kohn-Sham Density Functional Theory (KS-DFT) simulations -- contains a wealth of material information, making its prediction via machine learning (ML) models attractive. However, the…

Quantum mechanics/molecular mechanics (QM/MM) molecular dynamics (MD) simulations have been developed to simulate molecular systems, where an explicit description of changes in the electronic structure is necessary. However, QM/MM MD…

Chemical Physics · Physics 2021-04-15 Lennard Böselt , Moritz Thürlemann , Sereina Riniker

Large scale Density Functional Theory (DFT) based electronic structure calculations are highly time consuming and scale poorly with system size. While semi-empirical approximations to DFT result in a reduction in computational time versus…

Materials Science · Physics 2016-12-21 Ganesh Hegde , R. Chris Bowen

With the growth of computational resources, the scope of electronic structure simulations has increased greatly. Artificial intelligence and robust data analysis hold the promise to accelerate large-scale simulations and their analysis to…

Materials Science · Physics 2023-07-27 Lenz Fiedler , Karan Shah , Michael Bussmann , Attila Cangi

Molecular dynamics simulations have been used in different scientific fields to investigate a broad range of physical systems. However, the accuracy of calculation is based on the model considered to describe the atomic interactions. In…

Statistical Mechanics · Physics 2023-02-08 Márcio S. Gomes-Filho , Alberto Torres , Alexandre Reily Rocha , Luana S. Pedroza

Machine learning (ML) models utilizing structure-based features provide an efficient means for accurate property predictions across diverse chemical spaces. However, obtaining equilibrium crystal structures typically requires expensive…

Materials Science · Physics 2021-04-22 Yunxing Zuo , Mingde Qin , Chi Chen , Weike Ye , Xiangguo Li , Jian Luo , Shyue Ping Ong
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