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The prominence of density functional theory (DFT) in the field of electronic structure computation stems from its ability to usefully balance accuracy and computational effort. At the base of this ability is a functional of the electron…

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), 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

Standard approximations for the exchange-correlation (XC) functional in Kohn-Sham density functional theory (KS-DFT) typically lead to unacceptably large errors when applied to strongly-correlated electronic systems. Partition-DFT (PDFT) is…

Chemical Physics · Physics 2023-09-12 Yi Shi , Yuming Shi , Adam Wasserman

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

Density functional theory (DFT) embedding provides a formally exact framework for interfacing correlated wave-function theory (WFT) methods with lower-level descriptions of electronic structure. Here, we report techniques to improve the…

Chemical Physics · Physics 2015-06-12 Jason D. Goodpaster , Taylor A. Barnes , Frederick R. Manby , Thomas F. Miller

The demand for pseudopotentials constructed for a given exchange-correlation (XC) functional far exceeds the supply, necessitating the use of those commonly available. The number of XC functionals currently available is in the hundreds, if…

Materials Science · Physics 2024-11-01 Marcin Maździarz

Due to its favorable computational efficiency time-dependent (TD) density functional theory (DFT) enables the prediction of electronic spectra in a high-throughput manner across chemical space. Its predictions, however, can be quite…

Charge transfer plays a crucial role in many processes of interest in physics, chemistry, and bio-chemistry. In many applications the size of the systems involved calls for time-dependent density functional theory (TDDFT) to be used in…

Chemical Physics · Physics 2017-10-11 Neepa T. Maitra

A new density functional theory (DFT) exchange-correlation functional for the exploration of reaction mechanisms is proposed. This new functional, denoted BMK (Boese-Martin for Kinetics), has an accuracy in the 2 kcal/mol range for…

Chemical Physics · Physics 2007-05-23 A. Daniel Boese , Jan M. L. Martin

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

Motivated by the resurgence of electronic and optical property design in ordered fluoride and oxyfluoride compounds, we present a density functional theory (DFT) study on 19 materials with structures, ranging from simple to complex, and…

Materials Science · Physics 2016-11-23 Nenian Charles , James M. Rondinelli

Multi-center transition metal complexes (MCTMs) with magnetically interacting ions have been proposed as components for information processing devices and storage units. For any practical application of MCTMs as magnetic units, it is…

Chemical Physics · Physics 2023-04-03 Henry C. Fitzhugh , James W. Furness , Mark R. Pederson , Juan E. Peralta , Jianwei Sun

Density functional theory (DFT) in chemistry and materials science aims for "chemical accuracy," but this goal is challenged by the need to approximate the exact exchange-correlation (XC) energy functional. The r$^2$SCAN, meta-generalized…

Exchange interactions are a manifestation of the quantum mechanical nature of the electrons and play a key role in predicting the properties of materials from first principles. In density functional theory (DFT), a widely used approximation…

Materials Science · Physics 2020-03-27 Marco Bernardi

Density functional theory is the standard theory for computing the electronic structure of materials, which is based on a functional that maps the electron density to the energy. However, a rigorous form of the functional is not known and…

Materials Science · Physics 2021-12-02 Ryo Nagai , Ryosuke Akashi , Osamu Sugino

Accurate charge densities are essential for reliable electronic structure calculations because they significantly impact predictions of various chemical properties and in particular, according to the Hellmann-Feynman theorem, atomic forces.…

Chemical Physics · Physics 2025-03-12 Moritz Gubler , Moritz R. Schäfer , Jörg Behler , Stefan Goedecker

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

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

While in principle exact, Kohn-Sham density functional theory -- the workhorse of computational chemistry -- must rely on approximations for the exchange-correlation functional. Despite staggering successes, present-day approximations still…