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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

Double hybrid density functional theory arguably sits on the seamline between wavefunction methods and DFT: it represents a special case of Rung 5 on the "Jacobs Ladder" of John P. Perdew. For large and chemically diverse benchmarks such as…

Chemical Physics · Physics 2020-10-16 Jan M. L. Martin , Golokesh Santra

One of the great challenges of electronic structure theory is the quest for the exact functional of density functional theory. Its existence is proven, but it is a complicated multivariable functional that is almost impossible to…

Chemical Physics · Physics 2016-05-04 Aron J. Cohen , Paula Mori-Sánchez

We propose a multiconfigurational hybrid density-functional theory which rigorously combines a multiconfiguration self-consistent-field calculation with a density-functional approximation based on a linear decomposition of the…

Chemical Physics · Physics 2012-08-20 Kamal Sharkas , Andreas Savin , Hans Jørgen Aa. Jensen , Julien Toulouse

We use density functional theory (DFT) with non-empirically tuned screened range-separated hybrid (SRSH) functionals to calculate the electronic properties of native zinc and oxygen vacancy point defects in ZnO, and we predict their defect…

Materials Science · Physics 2025-04-21 Sijia Ke , Stephen E. Gant , Leeor Kronik , Jeffrey B. Neaton

We present a detailed study of the exact-exchange (EXX) kernel of time-dependent density functional theory with an emphasis on its discontinuity at integer particle numbers. It was recently found that this exact property leads to sharp…

Chemical Physics · Physics 2015-06-17 M. Hellgren , E. K. U. Gross

DFT calculations have become widespread in both chemistry and materials, because they usually provide useful accuracy at much lower computational cost than wavefunction-based methods. All practical DFT calculations require an approximation…

Chemical Physics · Physics 2022-03-15 Eunji Sim , Suhwan Song , Stefan Vuckovic , Kieron Burke

We discuss several aspects of the dielectric response theory application to the density functional theory. This field has been an unceasing source of confusion during several decades. The most frequent reasons for this confusion are (a)…

Condensed Matter · Physics 2008-02-03 I. I. Mazin , R. E. Cohen

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…

Understanding the properties of warm dense hydrogen is of key importance for the modeling of compact astrophysical objects and to understand and further optimize inertial confinement fusion (ICF) applications. The work horse of warm dense…

The crucial step in density-corrected Hartree-Fock density functional theory (DC(HF)-DFT) is to decide whether the density produced by the density functional for a specific calculation is erroneous and hence should be replaced by, in this…

Chemical Physics · Physics 2023-09-20 Daniel Graf , Alex J. W. Thom

Most approximate exchange-correlation functionals used within density functional theory are constructed as the sum of two distinct contributions for exchange and correlation. Separating the exchange component from the entire functional is…

Condensed Matter · Physics 2009-10-28 Claudia Filippi , C. J. Umrigar , Xavier Gonze

Density functional theory (DFT) exploits an independent-particle-system construction to replicate the densities and current of an interacting system. This construction is used here to access the exact effective potential and bias of…

Mesoscale and Nanoscale Physics · Physics 2018-03-30 Daniel Karlsson , Miroslav Hopjan , Claudio Verdozzi

Static correlation error(SCE) inevitably emerges when a dissociation of a covalent bond is described with a conventional denstiy-functional theory (DFT) for electrons. SCE gives rise to a serious overshoot in the potential energy at the…

Computational Physics · Physics 2020-08-10 Hideaki Takahashi

The general expectation that, in principle, time-dependent density functional theory (TDDFT) be an exact formulation of the time-evolution of an interacting N-electron system is critically reexamined. It is demonstrated that the previous…

Other Condensed Matter · Physics 2007-08-13 J. Schirmer , A. Dreuw

We present here novel insight into exchange-correlation functionals in density functional theory, based on the viewpoint of optimal transport. We show that in the case of two electrons and in the semiclassical limit, the exact…

Analysis of PDEs · Mathematics 2015-03-19 Codina Cotar , Gero Friesecke , Claudia Klüppelberg

Accurately modeling the electronic structure of materials is a persistent challenge to high-throughput screening. A promising means of balancing accuracy against computational cost are non-self-consistent calculations with hybrid…

Materials Science · Physics 2020-05-04 Jonathan M. Skelton , David S. D. Gunn , Sebastian Metz , Stephen C. Parker

Nowadays pseudopotential density-functional theory calculations constitute the standard approach to tackle solid-state electronic problems. These rely on distributed pseudopotential tables that were built from all-electron atomic…

Computational Physics · Physics 2020-03-24 Pedro Borlido , Jan Doumont , Fabien Tran , Miguel Marques , Silvana Botti

In recent years, "composite" density-functional-theory-based methods comprising specially optimized combinations of functionals, basis sets, and empirical corrections have become widely used owing to their robustness and computational…

Chemical Physics · Physics 2024-11-21 Corin C. Wagen , Jonathon E. Vandezande

Density scaling has a rich history in density functional theory, providing exact conditions for use in the construction of ever more accurate approximations to the unknown exchange-correlation functional. We define a conjugate potential…

Other Condensed Matter · Physics 2009-06-02 Peter Elliott , Kieron Burke