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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 report the development of a combined machine-learning and high-throughput density functional theory (DFT) framework to accelerate the search for new ferroelectric materials. The framework can predict potential ferroelectric compounds…

Locality of compact one-electron orbitals expanded strictly in terms of local subsets of basis functions can be exploited in density functional theory (DFT) to achieve linear growth of computation time with systems size, crucial in…

Computational Physics · Physics 2021-10-01 Yifei Shi , Jessica Karaguesian , Rustam Z. Khaliullin

We propose a framework to learn the time-dependent Hartree-Fock (TDHF) inter-electronic potential of a molecule from its electron density dynamics. Though the entire TDHF Hamiltonian, including the inter-electronic potential, can be…

Chemical Physics · Physics 2024-12-05 Harish S. Bhat , Prachi Gupta , Christine M. Isborn

Density functional theory (DFT) can run into serious difficulties with localized states in elements such as transition metals with occupied-d states and oxygen. In contrast, Hartree-Fock (HF) method can be a better approach for such…

Materials Science · Physics 2018-08-01 Hengxin Tan , Yuanchang Li , S. B. Zhang , Wenhui Duan

The calculation of electron density distribution using density functional theory (DFT) in materials and molecules is central to the study of their quantum and macro-scale properties, yet accurate and efficient calculation remains a…

Computational Physics · Physics 2024-05-15 Teddy Koker , Keegan Quigley , Eric Taw , Kevin Tibbetts , Lin Li

Current neural networks for predictions of molecular properties use quantum chemistry only as a source of training data. This paper explores models that use quantum chemistry as an integral part of the prediction process. This is done by…

Chemical Physics · Physics 2018-08-22 Haichen Li , Christopher Collins , Matteus Tanha , Geoffrey J. Gordon , David J. Yaron

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.…

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

Density-corrected density functional theory (DC-DFT) is enjoying substantial success in improving semilocal DFT calculations in a wide variety of chemical problems. This paper provides the formal theoretical framework and assumptions for…

Chemical Physics · Physics 2019-08-19 Stefan Vuckovic , Suhwan Song , John Kozlowski , Eunji Sim , Kieron Burke

Ab initio calculations are fundamentally bottlenecked for large systems by the steep computational scaling of solving self-consistent field (SCF) equations. While machine learning offers potential accelerations, existing methods often…

Chemical Physics · Physics 2026-05-12 Jiankun Wu , Jinming Fan , Chao Qian , Shaodong Zhou

Kohn-Sham density functional theory (DFT) is the standard method for first-principles calculations in computational chemistry and materials science. More accurate theories such as the random-phase approximation (RPA) are limited in…

Materials Science · Physics 2023-10-25 Stefan Riemelmoser , Carla Verdi , Merzuk Kaltak , Georg Kresse

We present a numerical modeling workflow based on machine learning (ML) which reproduces the the total energies produced by Kohn-Sham density functional theory (DFT) at finite electronic temperature to within chemical accuracy at negligible…

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

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

Localized basis sets in the projector augmented wave formalism allow for computationally efficient calculations within density functional theory (DFT). However, achieving high numerical accuracy requires an extensive basis set, which also…

Materials Science · Physics 2020-11-18 G. Gandus , A. Valli , D. Passerone , R. Stadler

Quantum mechanical calculations for material modelling using Kohn-Sham density functional theory (DFT) involve the solution of a nonlinear eigenvalue problem for $N$ smallest eigenvector-eigenvalue pairs with $N$ proportional to the number…

Computational Physics · Physics 2023-09-26 Sameer Khadatkar , Phani Motamarri

Understanding how structural flexibility affects the properties of metal-organic frameworks (MOFs) is crucial for the design of better MOFs for targeted applications. Flexible MOFs can be studied with molecular dynamics simulations, whose…

Materials Science · Physics 2024-05-13 Abhishek Sharma , Stefano Sanvito

Deep learning techniques have opened a new venue for electronic structure theory in recent years. In contrast to traditional methods, deep neural networks provide much more expressive and flexible wave function ansatz, resulting in better…

Chemical Physics · Physics 2021-09-08 Xiang Li , Cunwei Fan , Weiluo Ren , Ji Chen

We introduce DeepDFT, a deep learning model for predicting the electronic charge density around atoms, the fundamental variable in electronic structure simulations from which all ground state properties can be calculated. The model is…

Computational Physics · Physics 2020-11-09 Peter Bjørn Jørgensen , Arghya Bhowmik