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Machine learning is rapidly accelerating materials and chemical discovery, but most current models target energies, forces, or selected molecular properties rather than the underlying many-body electronic structure. Learning…

Density functional theory (DFT), one of the most widely utilized methods available to computational chemistry, fails to describe systems with statically correlated electrons. To address this shortcoming, in previous work we transformed DFT…

Chemical Physics · Physics 2023-01-02 Daniel Gibney , Jan-Niklas Boyn , David A. Mazziotti

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…

Density functional theory (DFT), the most widely adopted method in modern computational chemistry, fails to describe accurately the electronic structure of strongly correlated systems. Here we show that DFT can be formally and practically…

Chemical Physics · Physics 2022-04-18 Daniel Gibney , Jan-Niklas Boyn , David A. Mazziotti

We introduce surrogate functionals: machine-learned energy functionals for orbital-free density functional theory (OF-DFT) which are defined not by universal fidelity to a physical reference, but merely by the requirement that density…

Machine Learning · Computer Science 2026-04-23 Roman Remme , Fred A. Hamprecht

The combination of deep learning and ab initio materials calculations is emerging as a trending frontier of materials science research, with deep-learning density functional theory (DFT) electronic structure being particularly promising. In…

While density functional theory (DFT) serves as a prevalent computational approach in electronic structure calculations, its computational demands and scalability limitations persist. Recently, leveraging neural networks to parameterize the…

Computational Physics · Physics 2024-06-18 Yang Zhong , Hongyu Yu , Jihui Yang , Xingyu Guo , Hongjun Xiang , Xingao Gong

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

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…

We introduce machine learning (ML) models that predict the electronic structure of materials across a wide temperature range. Our models employ neural networks and are trained on density functional theory (DFT) data. Unlike most other ML…

Materials Science · Physics 2023-10-02 Lenz Fiedler , Normand A. Modine , Kyle D. Miller , Attila Cangi

Kohn-Sham density functional theory is the base of modern computational approaches to electronic structures. Their accuracy vitally relies on the exchange-correlation energy functional, which encapsulates electron-electron interaction…

Computational Physics · Physics 2019-11-04 Ryo Nagai , Ryosuke Akashi , Osamu Sugino

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

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

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

Machine learning (ML) plays an important role in quantum chemistry, providing fast-to-evaluate predictive models for various properties of molecules. However, most existing ML models for molecular electronic properties use density…

Chemical Physics · Physics 2024-06-26 Hao Tang , Brian Xiao , Wenhao He , Pero Subasic , Avetik R. Harutyunyan , Yao Wang , Fang Liu , Haowei Xu , Ju Li

We develop a method in which the electronic densities of small fragments determined by Kohn-Sham density functional theory (DFT) are embedded using stochastic DFT to form the exact density of the full system. The new method preserves the…

Chemical Physics · Physics 2015-06-19 Daniel Neuhauser , Roi Baer , Eran Rabani

Electronic density of states (DOS) is a key factor in condensed matter physics and material science that determines the properties of metals. First-principles density-functional theory (DFT) calculations have typically been used to obtain…

Materials Science · Physics 2019-04-12 Byung Chul Yeo , Donghun Kim , Chansoo Kim , Sang Soo Han

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

We present a systematic, quasi-automated methodology for generating electronic models in the framework of second-principles density functional theory (SPDFT). This approach enables the construction of accurate and computationally efficient…

We introduce new and robust decompositions of mean-field Hartree-Fock (HF) and Kohn-Sham density functional theory (KS-DFT) relying on the use of localized molecular orbitals and physically sound charge population protocols. The new…

Chemical Physics · Physics 2020-12-04 Janus J. Eriksen
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