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We propose machine learning (ML) models to predict the electron density -- the fundamental unknown of a material's ground state -- across the composition space of concentrated alloys. From this, other physical properties can be inferred,…

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

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

The theorems of density functional theory (DFT) and reduced density matrix functional theory (RDMFT) establish a bijective map between the external potential of a many-body system and its electron density or one-particle reduced density…

Chemical Physics · Physics 2023-02-22 Xuecheng Shao , Lukas Paetow , Mark E. Tuckerman , Michele Pavanello

Representation learning for the electronic structure problem is a major challenge of machine learning in computational condensed matter and materials physics. Within quantum mechanical first principles approaches, Kohn-Sham density…

Materials Science · Physics 2024-04-24 Bowen Hou , Jinyuan Wu , Diana Y. Qiu

Kohn-Sham density functional theory (KS-DFT) has found widespread application in accurate electronic structure calculations. However, it can be computationally demanding especially for large-scale simulations, motivating recent efforts…

Computational Physics · Physics 2024-06-25 Feitong Song , Ji Feng

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 study the accuracy of Kohn-Sham density functional theory (DFT) for warm- and hot-dense matter (WDM and HDM). Specifically, considering a wide range of systems, we perform accurate ab initio molecular dynamics simulations with…

Computational Physics · Physics 2024-11-21 Phanish Suryanarayana , Arpit Bhardwaj , Xin Jing , Shashikant Kumar , John E. Pask

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

The predictive accuracy of density functional theory (DFT) for alloy formation enthalpies is often limited by intrinsic energy resolution errors, particularly in ternary phase stability calculations. In this work, we present a machine…

Materials Science · Physics 2025-03-10 Sergei I. Simak , Erna K. Delczeg-Czirjak , Olle Eriksson

Machine learning (ML) of kinetic energy functionals (KEF) for orbital-free density functional theory (OF-DFT) holds the promise of addressing an important bottleneck in large-scale ab initio materials modeling where sufficiently accurate…

Materials Science · Physics 2025-04-10 Sergei Manzhos , Johann Luder , Pavlo Golub , Manabu Ihara

Hohenberg and Kohn have proven that the electronic energy and the one-particle electron density can, in principle, be obtained by minimizing an energy functional with respect to the density. While decades of theoretical work have produced…

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

Density functional theory underlies the most successful and widely used numerical methods for electronic structure prediction of solids. However, it has the fundamental shortcoming that the universal density functional is unknown. In…

Disordered Systems and Neural Networks · Physics 2020-09-23 M. Michael Denner , Mark H. Fischer , Titus Neupert

The formally exact framework of equilibrium Density Functional Theory (DFT) is capable of simultaneously and consistently describing thermodynamic and structural properties of interacting many-body systems in arbitrary external potentials.…

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

Understanding many processes, e.g. fusion experiments, planetary interiors and dwarf stars, depends strongly on microscopic physics modeling of warm dense matter (WDM) and hot dense plasma. This complex state of matter consists of a…

Computational Physics · Physics 2020-08-05 Alexander J. White , Lee A. Collins

The electronic density of states (DOS) quantifies the distribution of the energy levels that can be occupied by electrons in a quasiparticle picture, and is central to modern electronic structure theory. It also underpins the computation…

Materials Science · Physics 2021-01-04 Chiheb Ben Mahmoud , Andrea Anelli , Gábor Csányi , Michele Ceriotti

Machine learning of kinetic energy functionals (KEF), in particular kinetic energy density (KED) functionals, has recently attracted attention as a promising way to construct KEFs for orbital-free density functional theory (OF-DFT). Neural…

Materials Science · Physics 2025-08-11 Sergei Manzhos , Johann Lüder , Manabu Ihara

Orbital-free density functional theory (OF-DFT) holds the promise to compute ground state molecular properties at minimal cost. However, it has been held back by our inability to compute the kinetic energy as a functional of the electron…

Chemical Physics · Physics 2023-10-25 Roman Remme , Tobias Kaczun , Maximilian Scheurer , Andreas Dreuw , Fred A. Hamprecht