Perspective: Fifty years of density-functional theory in chemical physics.

  title={Perspective: Fifty years of density-functional theory in chemical physics.},
  author={Axel D. Becke},
  journal={The Journal of chemical physics},
  volume={140 18},
  • A. Becke
  • Published 1 April 2014
  • Physics
  • The Journal of chemical physics
Since its formal inception in 1964-1965, Kohn-Sham density-functional theory (KS-DFT) has become the most popular electronic structure method in computational physics and chemistry. Its popularity stems from its beautifully simple conceptual framework and computational elegance. The rise of KS-DFT in chemical physics began in earnest in the mid 1980s, when crucial developments in its exchange-correlation term gave the theory predictive power competitive with well-developed wave-function methods… 

Figures and Tables from this paper

Basics of the density functional theory
The density functional theory (DFT) established itself as a well reputed way to compute the electronic structure in most branches of chemistry and materials science. In the formulation given by Kohn,
Density Functional Theory : Past , present , . . . future ?
In little more than 20 years, the number of applications of the density functional (DF) formalism in chemistry and materials science has grown in astonishing fashion. The number of publications alone
DFT elucidation of materials properties.
This is the first Special Issue of Accounts of Chemical Research where density functional theory plays the central role, and it is commemorated by the cover displaying Fang Liu’s conception of the surfaces and clusters described here, along with the imaginative vision of ρ, the symbol of electron density upon which DFT is based, coalescing from small particles.
Density functional theory: Foundations reviewed
First step in the nuclear inverse Kohn-Sham problem: From densities to potentials
Nuclear Density Functional Theory (DFT) plays a prominent role in the understanding of nuclear structure, being the approach with the widest range of applications. Hohenberg and Kohn theorems warrant
Ultranonlocality in Density Functional Theory
The decisive advantage of density functional theory in comparison with other electronic structure methods is its favorable ratio of accuracy to computational cost. In its standard Kohn-Sham
Replacing hybrid density functional theory: motivation and recent advances.
Six modern attempts to go beyond classical DFT while maintaining hybrid DFT's relatively low computational cost are introduced: DFT+U, self-interaction corrections, localized orbital scaling corrections, local hybrid functionals, real-space nondynamical correlation, and the rung-3.5 approach.
Double and Charge-Transfer Excitations in Time-Dependent Density Functional Theory.
  • N. Maitra
  • Physics
    Annual review of physical chemistry
  • 2021
The fundamental challenges the approximate functionals have in describing double excitations and charge-transfer excitations are reviewed, which are two of the most common impediments for the theory to be applied in a black-box way.
Why the energy is sometimes not enough A dive into self-interaction corrected density functional theory
In electronic structure methods such as density functional theory (DFT) or closely related methods like self-interaction corrections (SIC), e.g., utilizing Fermi-Löwdin orbitals (FLO) [Schwalbe et


Developing the random phase approximation into a practical post-Kohn-Sham correlation model.
  • F. Furche
  • Physics
    The Journal of chemical physics
  • 2008
A physically appealing reformulation of the RPA correlation model is developed that substantially reduces its computational complexity and may become the long-sought robust and efficient zero order post-Kohn-Sham correlation model.
Electron correlation methods based on the random phase approximation
In the past decade, the random phase approximation (RPA) has emerged as a promising post-Kohn–Sham method to treat electron correlation in molecules, surfaces, and solids. In this review, we explain
Ab initio DFT and its role in electronic structure theory
Today's electronic structure theory depends equally upon density functional theory (DFT) and wavefunction theory (WFT). The interconnections between the two has long been of interest, but has not
Meta-generalized gradient approximation: explanation of a realistic nonempirical density functional.
It is suggested that satisfaction of additional exact constraints on higher rungs of a ladder of density functional approximations can lead to further progress in the meta-GGA.
Exchange and correlation in atoms, molecules, and solids by the spin-density-functional formalism
The aim of this paper is to advocate the usefulness of the spin-density-functional (SDF) formalism. The generalization of the Hohenberg-Kohn-Sham scheme to and SDF formalism is presented in its
Global Hybrid Functionals: A Look at the Engine under the Hood
Global hybrids, which add a typically modest fraction of the exact exchange energy to a complement of semilocal exchange−correlation energy, are among the most widely used density functionals in
Comparison of the performance of exact-exchange-based density functional methods.
This study reports a self-consistent RI implementation of the PSTS functional, and implements the Mori-Sanchez-Cohen-Yang-2 (MCY2) functional, a recent DFT method that includes full exact exchange and is found to be the only functional that yields qualitatively correct dissociation curves for two-center symmetric radicals like He(2)(+).
Efficient construction of exchange and correlation potentials by inverting the Kohn-Sham equations.
Given a set of canonical Kohn-Sham orbitals, orbital energies, and an external potential for a many-electron system, one can invert the Kohn-Sham equations in a single step to obtain the
Accurate calculation and modeling of the adiabatic connection in density functional theory.
The AC integrands in the present work are recommended as a basis for further work, generating functionals that avoid spurious error cancellations between exchange and correlation energies and give good accuracy for the range of densities and types of correlation contained in the systems studied here.
How tight is the Lieb-Oxford bound?
A survey of available exact or near-exact data on xc energies of atoms, ions, molecules, solids, and some model Hamiltonians finds all physically realistic density distributions investigated are consistent with the tighter limit C<or=1.68.