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Unrestricted DFT methods are typically expected to describe the homolytic dissociation of nonpolar single bonds in neutral species with qualitative accuracy, due to the lack of significant delocalization error. We however find that many…

Chemical Physics · Physics 2019-03-15 Diptarka Hait , Adam Rettig , Martin Head-Gordon

Response calculations in density functional theory aim at computing the change in ground-state density induced by an external perturbation. At finite temperature these are usually performed by computing variations of orbitals, which involve…

Numerical Analysis · Mathematics 2023-04-04 Eric Cancès , Michael F. Herbst , Gaspard Kemlin , Antoine Levitt , Benjamin Stamm

We study both static and transport properties of model quantum dots, employing density functional theory as well as (numerically) exact methods. For the lattice model under consideration the accuracy of the local-density approximation…

Mesoscale and Nanoscale Physics · Physics 2011-04-11 S. Schenk , P. Schwab , M. Dzierzawa , U. Eckern

For the kinetic energy of 1d model finite systems the leading corrections to local approximations as a functional of the potential are derived using semiclassical methods. The corrections are simple, non-local functionals of the potential.…

Other Condensed Matter · Physics 2010-06-25 Attila Cangi , Donghyung Lee , Peter Elliott , Kieron Burke

The exchange-correlation energy in Kohn-Sham density functional theory is expressed as a functional of the electronic density and the Kohn-Sham orbitals. An alternative to Kohn-Sham theory is to express the energy as a functional of the…

Computational Physics · Physics 2009-10-31 S. Goedecker , C. Umrigar

This paper is designed to be a practical tool for constructing and investigating two-point correlation functions in defect conformal field theory, directly in physical space, between any two bulk primaries or between a bulk primary and a…

High Energy Physics - Theory · Physics 2021-05-12 Christopher P. Herzog , Abhay Shrestha

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

Machine learning is used to approximate density functionals. For the model problem of the kinetic energy of non-interacting fermions in 1d, mean absolute errors below 1 kcal/mol on test densities similar to the training set are reached with…

Computational Physics · Physics 2015-06-03 John C. Snyder , Matthias Rupp , Katja Hansen , Klaus-Robert Müller , Kieron Burke

The study of a machine learning problem is in many ways is difficult to separate from the study of the loss function being used. One avenue of inquiry has been to look at these loss functions in terms of their properties as scoring rules…

Machine Learning · Computer Science 2022-09-02 Zac Cranko , Robert C. Williamson , Richard Nock

The incorporation of a strong interaction regime within the approximate, semilocal exchange-correlation functionals still remains a very challenging task for density functional theory. One of the promising attempts in this direction is the…

Other Condensed Matter · Physics 2023-09-20 Subrata Jana , Szymon Smiga , Lucian A. Constantin , Prasanjit Samal

The exact form of the kinetic energy functional has remained elusive in orbital-free models of density functional theory (DFT). This has been the main stumbling block for the development of a general-purpose framework on this basis. Here,…

Mesoscale and Nanoscale Physics · Physics 2020-01-06 Thomas Pope , Werner Hofer

We present a first principles strategy for developing state-specific density functional approximations for excited states. We first clarify why approaches based on conventional ground state approximations miss density-driven correlations,…

Chemical Physics · Physics 2025-06-09 Tim Gould , Stephen G Dale , Leeor Kronik , Stefano Pittalis

The calculation of the band-gap by density-functional theory (DFT) methods is examined by considering the behavior of the energy as a function of number of electrons. It is found that the incorrect band-gap prediction with most approximate…

Materials Science · Physics 2009-11-13 Aron J. Cohen , Paula Mori-Sánchez , Weitao Yang

We determine the fully resolved equilibrium density profiles for two binary hard-sphere crystal structures using classical density functional theory through the White Bear II functional from fundamental measure theory. While for the…

Statistical Mechanics · Physics 2026-04-21 Alessandro Simon , Martin Oettel

Accurately describing strong electron correlation in complex systems remains a prominent challenge in computational chemistry as near-term quantum algorithms treating total correlation often require prohibitively deep circuits. Here we…

Computational Engineering, Finance, and Science · Computer Science 2026-04-21 Zhanou Liu , Yuhao Chen , Yingjin Ma , Xiao He , Yuxin Deng

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

The band-gap problem and other systematic failures of approximate functionals are explained from an analysis of total energy for fractional charges. The deviation from the correct intrinsic linear behavior in finite systems leads to…

Materials Science · Physics 2009-11-13 Paula Mori-Sánchez , Aron J. Cohen , Weitao Yang

Density-functional theory requires ever better exchange-correlation (xc) functionals for the ever more precise description of many-body effects on electronic structure. Universal constraints on the xc energy are important ingredients in the…

Chemical Physics · Physics 2009-11-13 Mariana M. Odashima , K. Capelle

We derive a generalized gradient approximation to the exchange energy to be used in density functional theory calculations of two-dimensional systems. This class of approximations has a long and successful history, but it has not yet been…

Strongly Correlated Electrons · Physics 2009-01-07 S. Pittalis , E. Rasanen , J. G. Vilhena , M. A. L. Marques

The adiabatic connection of density functional theory (DFT) for electronic systems is generalized here to negative values of the coupling strength $\alpha$ (with {\em attractive} electrons). In the extreme limit $\alpha\to-\infty$ a simple…

Other Condensed Matter · Physics 2015-05-14 Michael Seidl , Paola Gori-Giorgi