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We study static correlation and delocalisation errors and show that even methods with good energies can yield significant delocalization errors that affect the density, leading to large errors in predicting {\em e.g.} dipole moments. We…

Chemical Physics · Physics 2020-06-01 Maria Hellgren , Tim Gould

Density Functional Theory (DFT) is a pivotal method within quantum chemistry and materials science, with its core involving the construction and solution of the Kohn-Sham Hamiltonian. Despite its importance, the application of DFT is…

We study the accuracy of Kohn-Sham density functional theory (DFT) for warm- and hot-dense matter (WDM and HDM). Specifically, considering a wide range of systems, we perform accurate ab initio molecular dynamics simulations with…

Computational Physics · Physics 2024-11-21 Phanish Suryanarayana , Arpit Bhardwaj , Xin Jing , Shashikant Kumar , John E. Pask

Embedded density functional theory (e-DFT) is used to describe the electronic structure of strongly interacting molecular subsystems. We present a general implementation of the Exact Embedding (EE) method [J. Chem. Phys. 133, 084103 (2010)]…

Other Condensed Matter · Physics 2011-07-27 Jason D. Goodpaster , Taylor A. Barnes , Thomas F. Miller

Quasiparticle energies and fundamental band gaps in particular are critical properties of molecules and materials. It was rigorously established that the generalized Kohn-Sham HOMO and LUMO orbital energies are the chemical potentials of…

Chemical Physics · Physics 2019-03-06 Yuncai Mei , Chen Li , Neil Qiang Su , Weitao Yang

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

Within exact electron density-functional theory, we investigate Kohn-Sham (KS) potentials, orbital energies, and non-interacting kinetic energies of the fractional ions of Li, C and F. We use quantum Monte Carlo densities as input, which…

Chemical Physics · Physics 2014-11-14 Tim Gould , Julien Toulouse

A system of electrons in a local or nonlocal external potential can be studied with 1-matrix functional theory (1MFT), which is similar to density functional theory (DFT) but takes the one-particle reduced density matrix (1-matrix) instead…

Strongly Correlated Electrons · Physics 2008-07-23 Ryan Requist , Oleg Pankratov

We introduce an orbital-optimized double-hybrid (DH) scheme using the optimized-effective-potential (OEP) method. The orbitals are optimized using a local potential corresponding to the complete exchange-correlation energy expression…

In order to obtain a reasonably accurate and easily implemented approach to many-electron calculations, we will develop a new Density Functional Theory (DFT). Specifically, we derive an approximation to electron density, the first term of…

Materials Science · Physics 2010-04-23 Gregory C. Dente

In the present work, we introduce a Self-Consistent Density-Functional Embedding technique, which leaves the realm of standard energy-functional approaches in Density Functional Theory and targets directly the density-to-potential mapping…

Computational Physics · Physics 2019-07-17 Uliana Mordovina , Teresa E. Reinhard , Iris Theophilou , Heiko Appel , Angel Rubio

We present in full detail a newly developed formalism enabling density functional perturbation theory (DFPT) calculations from a DFT+$U$ ground state. The implementation includes ultrasoft pseudopotentials and is valid for both insulating…

Strongly Correlated Electrons · Physics 2020-02-21 Andrea Floris , Iurii Timrov , Burak Himmetoglu , Nicola Marzari , Stefano de Gironcoli , Matteo Cococcioni

We formulate the Kohn-Sham density functional theory (KS-DFT) as a statistical theory in which the electron density is deter-mined from an average of correlated stochastic densities in a trace formula. The key idea is that it is sufficient…

Materials Science · Physics 2015-06-15 Roi Baer , Daniel Neuhauser , Eran Rabani

A detailed convex analysis-based formulation of density-functional theory for periodic systems in arbitrary dimensions is presented. The electron-electron interaction is taken to be of Yukawa type, harmonising with underlying function…

Chemical Physics · Physics 2026-02-23 Oliver M. Bohle , Maryam Lotfigolian , Andre Laestadius , Erik I. Tellgren

This is a comprehensive review of the strong-interaction limit of density functional theory. It covers the derivation of the limiting strictly correlated electrons (SCE) functional from exact Hohenberg-Kohn DFT, basic aspects of SCE physics…

Chemical Physics · Physics 2022-02-22 Gero Friesecke , Augusto Gerolin , Paola Gori-Giorgi

We present an atomic orbital based approximate scheme for self-interaction correction (SIC) to the local density approximation of density functional theory. The method, based on the idea of Filippetti and Spaldin [Phys. Rev. B 67, 125109…

Strongly Correlated Electrons · Physics 2013-05-29 C. D. Pemmaraju , T. Archer , D. Sanchez-Portal , S. Sanvito

Strongly correlated systems have long been a central and highly non-trivial topic in condensed matter physics. At the non-interacting level, strong correlation can be associated with powerful (near) degeneracies between occupied and…

Strongly Correlated Electrons · Physics 2026-04-29 Daniel D. Rivera , Gustavo M. Dalpian , John P. Perdew

We explore a new formalism to study the nonlinear electronic density response based on Kohn-Sham density functional theory (KS-DFT) at partially and strongly quantum degenerate regimes. It is demonstrated that the KS-DFT calculations are…

Plasma Physics · Physics 2022-05-10 Zhandos Moldabekov , Jan Vorberger , Tobias Dornheim

Electronic structure calculation of atoms and molecules, in the past few decades has largely been dominated by density functional methods. This is primarily due to the fact that this can account for electron correlation effects in a…

Chemical Physics · Physics 2013-07-12 Amlan K. Roy

This work presents a new class of hybrid density functional theory (DFT) approximations, incorporating nonlocal exact exchange in predefined states such as core atomic orbitals (AOs). These projected hybrid density functionals are a…

Chemical Physics · Physics 2023-05-16 Benjamin G. Janesko