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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

Density functional theory (DFT) stands as a cornerstone method in computational quantum chemistry and materials science due to its remarkable versatility and scalability. Yet, it suffers from limitations in accuracy, particularly when…

While density functional theory (DFT) is widely applied for its combination of cost and accuracy, corrections (e.g., DFT+U) that improve it are often needed to tackle correlated transition-metal chemistry. In principle, the functional form…

Chemical Physics · Physics 2021-03-12 Akash Bajaj , Heather J. Kulik

Practical density functional theory (DFT) owes its success to the groundbreaking work of Kohn and Sham that introduced the exact calculation of the non-interacting kinetic energy of the electrons using an auxiliary mean-field system.…

Chemical Physics · Physics 2023-11-17 P. del Mazo-Sevillano , J. Hermann

Deep-learning density functional theory (DFT) shows great promise to significantly accelerate material discovery and potentially revolutionize materials research. However, current research in this field primarily relies on data-driven…

Computational Physics · Physics 2024-08-14 Yang Li , Zechen Tang , Zezhou Chen , Minghui Sun , Boheng Zhao , He Li , Honggeng Tao , Zilong Yuan , Wenhui Duan , Yong Xu

We present a substantial extension of our constraint-based approach for development of orbital-free (OF) kinetic-energy (KE) density functionals intended for the calculation of quantum-mechanical forces in multi-scale molecular dynamics…

Materials Science · Physics 2015-05-13 V. V. Karasiev , R. S. Jones , S. B. Trickey , Frank E. Harris

The accuracy of density-functional theory (DFT) is determined by the quality of the approximate functionals, such as exchange-correlation in electronic DFT and the excess functional in the classical DFT formalism of fluids. The exact…

Plane-wave electronic-structure predictions based upon orbital-dependent density-functional theory (OD-DFT) approximations, such as hybrid density-functional methods and self-interaction density-functional corrections, are severely affected…

Materials Science · Physics 2011-10-19 Yanli Li , Ismaila Dabo

Orbital-free density functional theory (OF-DFT) constitutes a computationally highly effective tool for modeling electronic structures of systems ranging from room-temperature materials to warm dense matter. Its accuracy critically depends…

The density functional theory (DFT) is used in a study of point defects on both UN (001) surface and sub-surface layers. We compare results for slabs of different thicknesses (both perfect and containing nitrogen or uranium vacancies) with…

Materials Science · Physics 2012-11-27 Dmitry Bocharov , Denis Gryaznov , Yuri F. Zhukovskii , Eugene A. Kotomin

We show that a lattice formulation of density-functional theory (DFT), guided by renormalization-group concepts, can be used to obtain numerical predictions of energy gaps, spin-density profiles, critical exponents, sound velocities,…

Strongly Correlated Electrons · Physics 2009-11-13 Francisco C. Alcaraz , Klaus Capelle

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

Density functional theory (DFT) is the de facto approach for predicting self-consistent-field electronic structures of ground-state configurations of complex atoms, molecules, and solids and providing their property data for materials…

Materials Science · Physics 2024-01-30 Zi-Kui Liu

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 present a $\Delta$-machine learning model for obtaining Kohn-Sham accuracy from orbital-free density functional theory (DFT) calculations. In particular, we employ a machine learned force field (MLFF) scheme based on the kernel method to…

Chemical Physics · Physics 2023-10-11 Shashikant Kumar , Xin Jing , John E. Pask , Andrew J. Medford , Phanish Suryanarayana

We propose a novel scheme to bring reduced density matrix functional theory (RDMFT) into the realm of density functional theory (DFT) that preserves the accurate density functional description at equilibrium, while incorporating accurately…

Chemical Physics · Physics 2014-11-07 Nektarios N. Lathiotakis , Nicole Helbig , Angel Rubio , Nikitas I. Gidopoulos

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

Density functional theory (DFT) based modeling of electronic excited states is of importance for investigation of the photophysical/photochemical properties and spectroscopic characterization of large systems. The widely used linear…

Chemical Physics · Physics 2021-05-11 Diptarka Hait , Martin Head-Gordon

Orbital-optimized density functional theory (DFT) has emerged as an alternative to time-dependent (TD) DFT capable of describing difficult excited states with significant electron density redistribution, such as charge-transfer, Rydberg,…

Chemical Physics · Physics 2025-01-22 Hanh D. M. Pham , Rustam Z. Khaliullin

Orbital-free density functional theory promises to deliver linear-scaling electronic structure calculations. This requires the knowledge of the non-interacting kinetic-energy density functional (KEDF), which should be accurate and must…

Materials Science · Physics 2024-12-12 Michael A. J. Mitchell , Teresa Del Aguila Ferrandis , Stefano Sanvito