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Machine learning-based neural network potentials have the ability to provide ab initio-level predictions while reaching large length and time scales often limited to empirical force fields. Traditionally, neural network potentials rely on a…

Chemical Physics · Physics 2023-01-19 Harender S. Dhattarwal , Ang Gao , Richard C. Remsing

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

We introduce a coarse-grained deep neural network model (CG-DNN) for liquid water that utilizes 50 rotational and translational invariant coordinates, and is trained exclusively against energies of ~30,000 bulk water configurations. Our…

Accurate ab-initio prediction of electronic energies is very expensive for macromolecules by explicitly solving post-Hartree-Fock equations. We here exploit the physically justified local correlation feature in compact basis of small…

Chemical Physics · Physics 2023-08-01 Wai-Pan Ng , Qiujiang Liang , Jun Yang

The widespread use of (generalized) Kohn-Sham density functional theory (KS-DFT) lies in the fact that hierarchical sets of approximations of the exchange-correlation (XC) energy functional can be designed, offering versatile choices to…

Materials Science · Physics 2023-01-31 Igor Ying Zhang , Xinguo Ren

Improving the predictive capability of molecular properties in ab initio simulations is essential for advanced material discovery. Despite recent progress making use of machine learning, utilizing deep neural networks to improve quantum…

Chemical Physics · Physics 2021-09-22 Muhammad F. Kasim , Sam M. Vinko

We show how machine learning techniques based on Bayesian inference can be used to reach new levels of realism in the computer simulation of molecular materials, focusing here on water. We train our machine-learning algorithm using…

Materials Science · Physics 2013-02-25 Albert P. Bartok , Michael J. Gillan , Frederick R. Manby , Gabor Csanyi

We train a neural network as the universal exchange-correlation functional of density-functional theory that simultaneously reproduces both the exact exchange-correlation energy and potential. This functional is extremely non-local, but…

Computational Physics · Physics 2019-10-10 Jonathan Schmidt , Carlos L. Benavides-Riveros , Miguel A. L. Marques

Accurate approximation of the exchange-correlation (XC) energy in density functional theory (DFT) calculations is essential for reliably modelling electronic systems. Many such approximations are developed from models of the XC hole;…

Chemical Physics · Physics 2024-11-27 Lin Hou , Tom J. P. Irons , Yanyong Wang , James W. Furness , Andrew M. Wibowo-Teale , Jianwei Sun

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

Machine learning (ML) has recently gained attention as a means to develop more accurate exchange-correlation (XC) functionals for density functional theory, but functionals developed thus far need to be improved on several metrics,…

Chemical Physics · Physics 2022-03-14 Kyle Bystrom , Boris Kozinsky

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…

The local density approximation (LDA) constructed through quantum Monte Carlo calculations of the homogeneous electron gas (HEG) is the most common approximation to the exchange-correlation functional in density functional theory. We…

Other Condensed Matter · Physics 2021-01-15 Mike Entwistle , Matthew Hodgson , Jack Wetherell , Bradley Longstaff , James Ramsden , Rex Godby

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

In a data-driven paradigm, machine learning (ML) is the central component for developing accurate and universal exchange-correlation (XC) functionals in density functional theory (DFT). It is well known that XC functionals must satisfy…

Ground-state Kohn-Sham density functional theory provides, in principle, the exact ground-state energy and electronic spin-densities of real interacting electrons in a static external potential. In practice, the exact density functional for…

Chemical Physics · Physics 2022-07-11 Aaron D. Kaplan , Mel Levy , John P. Perdew

Computational virtual high-throughput screening (VHTS) with density functional theory (DFT) and machine-learning (ML)-acceleration is essential in rapid materials discovery. By necessity, efficient DFT-based workflows are carried out with a…

Materials Science · Physics 2021-06-25 Chenru Duan , Shuxin Chen , Michael G. Taylor , Fang Liu , Heather J. Kulik

In this paper we investigate the performance of different machine learning potentials (MLPs) in predicting key thermodynamic properties of water using RPBE+D3. Specifically, we scrutinize kernel-based regression and high-dimensional neural…

We show that deep neural networks can be integrated into, or fully replace, the Kohn-Sham density functional theory scheme for multi-electron systems in simple harmonic oscillator and random external potentials with no feature engineering.…

Materials Science · Physics 2021-02-25 Kevin Ryczko , David Strubbe , Isaac Tamblyn

In density functional theory (DFT), exact constraints, fundamental mathematical properties of the exchange-correlation (XC) energy and its underlying XC hole, along with paradigm systems such as the uniform electron gas and the hydrogen…

Materials Science · Physics 2026-03-13 Yan Oueis , Akilan Ramasamy , James W. Furness , Jamin Kidd , Timo Lebeda , Jianwei Sun