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Modern density functional theory (DFT) calculations employ the Kohn-Sham (KS) system of non-interacting electrons as a reference, with all complications buried in the exchange-correlation energy (Exc). The adiabatic connection formula gives…

Other Condensed Matter · Physics 2009-10-02 Zhenfei Liu , Kieron Burke

We report density-functional studies of several small molecules ($H_{2}, N_{2}, CO, H_{2}O$, and $CH_{4}$) within the Krieger-Li-Iafrate (KLI) approximation to the exact Kohn-Sham local exchange potential, using a three-dimensional…

Chemical Physics · Physics 2009-10-31 Yong-Hoon Kim , Martin Städele , Richard M. Martin

Machine learning of kinetic energy functionals (KEF), in particular kinetic energy density (KED) functionals, has recently attracted attention as a promising way to construct KEFs for orbital-free density functional theory (OF-DFT). Neural…

Materials Science · Physics 2025-08-11 Sergei Manzhos , Johann Lüder , Manabu Ihara

The present work demonstrates a robust protocol for probing localized electronic structure in condensed-phase systems, operating in terms of a recently proposed theory for decomposing the results of Kohn-Sham density functional theory in a…

Chemical Physics · Physics 2021-06-29 Janus J. Eriksen

Functionals of the meta-generalized gradient approximation (MGGA) are nowadays widely used in chemistry and solid-state physics for the simulation of electronic systems like molecules, solids, or surfaces. Due to their dependency on the…

Materials Science · Physics 2022-05-31 Jan Doumont , Fabien Tran , Peter Blaha

It is known that the adiabatic approximation in time-dependent density functional theory usually provides a good description of low-lying excitations of molecules. In the present work, the capability of the adiabatic nonempirical…

Materials Science · Physics 2009-11-13 Jianmin Tao , Sergei Tretiak , Jian-Xin Zhu

Density functional theory (DFT) offers an exceptional balance between accuracy and efficiency, but practical density functional approximations face an unavoidable trade-off among simplicity, accuracy, and transferability. A systematic…

Chemical Physics · Physics 2026-03-25 Jiashu Liang , Martin Head-Gordon

We present a Gaussian-basis implementation of orbital-free density-functional theory (OF-DFT) in which the trust-region image method (TRIM) is used for optimization. This second-order optimization scheme has been constructed to provide…

Chemical Physics · Physics 2021-09-15 Matthew S. Ryley , Michael Withnall , Tom J. P. Irons , Trygve Helgaker , Andrew M. Teale

Machine learning (ML) of kinetic energy functionals (KEF) for orbital-free density functional theory (OF-DFT) holds the promise of addressing an important bottleneck in large-scale ab initio materials modeling where sufficiently accurate…

Materials Science · Physics 2025-04-10 Sergei Manzhos , Johann Luder , Pavlo Golub , Manabu Ihara

We calculate the optical spectra of silicon and germanium in the adiabatic time-dependent density functional formalism, making use of kinetic energy density-dependent (meta-GGA) exchange-correlation functionals. We find excellent agreement…

Strongly Correlated Electrons · Physics 2011-11-16 V. U. Nazarov , G. Vignale

Orbital-free density functional theory promises to deliver linear-scaling electronic structure calculations. This requires the knowledge of the non-interacting kinetic-energy density functional (KEDF), which should be accurate and must…

Materials Science · Physics 2024-12-12 Michael A. J. Mitchell , Teresa Del Aguila Ferrandis , Stefano Sanvito

The random phase approximation (RPA) for the electron correlation energy, combined with the exact-exchange energy, represents the state-of-the-art exchange-correlation functional within density-functional theory (DFT). However, the standard…

Other Condensed Matter · Physics 2015-05-20 Xinguo Ren , Patrick Rinke , Alexandre Tkatchenko , Matthias Scheffler

Due to several attractive features, the meta-generalized-gradient approximations (meta-GGAs) are considered to be the most advanced and potentially accurate semilocal exchange-correlation functionals in the rungs of the Jacob's ladder of…

Atomic and Molecular Clusters · Physics 2020-04-28 Abhilash Patra , Subrata Jana , Lucian A. Constantin , Prasanjit Samal

Orbital-free density functional theory (OFDFT) is a quantum chemistry formulation that has a lower cost scaling than the prevailing Kohn-Sham DFT, which is increasingly desired for contemporary molecular research. However, its accuracy is…

Machine Learning · Statistics 2024-03-12 He Zhang , Siyuan Liu , Jiacheng You , Chang Liu , Shuxin Zheng , Ziheng Lu , Tong Wang , Nanning Zheng , Bin Shao

We report the first wholly non-empirical generalized gradient approximation, non-interacting free energy functional for orbital-free density functional theory and use that new functional to provide forces for finite-temperature molecular…

Materials Science · Physics 2013-11-26 Valentin V. Karasiev , Debajit Chakraborty , Olga A. Shukruto , S. B. Trickey

During the last few years, it has become more and more clear that functionals of the meta generalized gradient approximation (MGGA) are more accurate than GGA functionals for the geometry and energetics of electronic systems. However, MGGA…

Materials Science · Physics 2019-11-04 Fabien Tran , Jan Doumont , Peter Blaha , Miguel A. L. Marques , Silvana Botti , Albert P. Bartók

A novel approach to electronic correlations and magnetism of crystals based on realistic electronic structure calculations is reviewed. In its simplest form it is a combination of the ``local density approximation'' (LDA) and the dynamical…

Strongly Correlated Electrons · Physics 2007-05-23 A. I. Lichtenstein , M. I. Katsnelson , G. Kotliar

The description of realistic strongly correlated systems has recently advanced through the combination of density functional theory in the local density approximation (LDA) and dynamical mean field theory (DMFT). This LDA+DMFT method is…

Strongly Correlated Electrons · Physics 2009-11-13 B. Amadon , F. Lechermann , A. Georges , F. Jollet , T. O. Wehling , A. I. Lichtenstein

Under a certain scaling, the electron densities of finite systems become both large and slowly-varying, so that the gradient expansions of the density functionals for the Kohn-Sham kinetic and exchange energies become asymptotically exact…

Quantum Physics · Physics 2009-11-13 John P. Perdew , Lucian A. Constantin , Espen Sagvolden , Kieron Burke

Using a linear combination of atomic orbitals approach, we report a systematic comparison of various Density Functional Theory (DFT) and hybrid exchange-correlation functionals for the prediction of the electronic and structural properties…

Materials Science · Physics 2008-05-07 D. I. Bilc , R. Orlando , R. Shaltaf , G. -M. Rignanese , Jorge Íñiguez , Ph. Ghosez