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Orbital-free density functional theory (OF-DFT) provides an alternative approach for calculating the molecular electronic energy, relying solely on the electron density. In OF-DFT, both the ground-state density is optimized variationally to…

Chemical Physics · Physics 2023-11-23 Alexandre de Camargo , Ricky T. Q. Chen , Rodrigo A. Vargas-Hernández

Dynamical Mean-Field Theory (DMFT) has opened new perspectives for the investigation of strongly correlated electron systems and greatly improved our understanding of correlation effects in models and materials. In contrast to…

Strongly Correlated Electrons · Physics 2020-07-16 Dieter Vollhardt

Static electric response properties of atoms and molecules are reported within the real-space Cartesian grid implementation of pseudopotential Kohn-Sham (KS) density functional theory (DFT). A detailed systematic investigation is made for a…

Chemical Physics · Physics 2019-04-26 Tanmay Mandal , Abhisek Ghosal , Amlan K. Roy

This chapter presents the development of a density functional theory (DFT)-based method for accurate, reliable treatment of various resonances in atoms. Many of these are known to be notorious for their strong correlation, proximity to more…

Chemical Physics · Physics 2019-04-19 Amlan K. Roy

The practical success of density functional theory (DFT) is largely credited to the Kohn-Sham approach, which enables the exact calculation of the non-interacting electron kinetic energy via an auxiliary noninteracting system. Yet, the…

Computational Physics · Physics 2025-03-21 Sangita Majumdar , Zekun Shi , Giovanni Vignale

We present a numerical modeling workflow based on machine learning (ML) which reproduces the the total energies produced by Kohn-Sham density functional theory (DFT) at finite electronic temperature to within chemical accuracy at negligible…

Quantum computers open up new avenues for modelling the physical properties of materials and molecules. Density Functional Theory (DFT) is the gold standard classical algorithm for predicting these properties, but relies on approximations…

Quantum Physics · Physics 2024-02-29 Evan Sheridan , Lana Mineh , Raul A. Santos , Toby Cubitt

Density functional theory (DFT) offers a desirable balance between quantitative accuracy and computational efficiency in practical many-electron calculations. Its central component, the exchange-correlation energy functional, has been…

This work continues a program to systematically generalize the Skyrme Hartree-Fock method for medium and heavy nuclei by applying effective field theory (EFT) methods to Kohn-Sham density functional theory (DFT). When conventional Kohn-Sham…

Nuclear Theory · Physics 2007-05-23 Anirban Bhattacharyya , R. J. Furnstahl

This article is part-I of a review of density-functional theory (DFT) that is the most widely used method for calculating electronic structure of materials. The accuracy and ease of numerical implementation of DFT methods has resulted in…

Materials Science · Physics 2023-05-25 Prashant Singh , Manoj K Harbola

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

The practical utility of M{\o}ller-Plesset (MP) perturbation theory is severely constrained by the use of Hartree-Fock (HF) orbitals. It has recently been shown that use of regularized orbital-optimized MP2 orbitals and scaling of MP3…

Chemical Physics · Physics 2021-01-06 Adam Rettig , Diptarka Hait , Luke W. Bertels , Martin Head-Gordon

The Hohenberg-Kohn theorem of density functional theory (DFT) for the case of electrons interacting with an external magnetic field (that couples to spin only) is examined in more detail than previously. A unexpected generalization is…

Strongly Correlated Electrons · Physics 2009-10-31 H. Eschrig , W. E. Pickett

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

We present a real-space formulation and higher-order finite-difference implementation of periodic Orbital-free Density Functional Theory (OF-DFT). Specifically, utilizing a local reformulation of the electrostatic and kernel terms, we…

Computational Physics · Physics 2015-12-23 Swarnava Ghosh , Phanish Suryanarayana

In this paper, we study a few theoretical issues in the discretized Kohn-Sham (KS) density functional theory (DFT). The equivalence between either a local or global minimizer of the KS total energy minimization problem and the solution to…

Computational Physics · Physics 2014-02-21 Xin Liu , Zaiwen Wen , Xiao Wang , Michael Ulbrich , Yaxiang Yuan

Kohn-Sham (KS) density functional theory (DFT) is a very efficient method for calculating various properties of solids as, for instance, the total energy, the electron density, or the electronic band structure. The KS-DFT method leads to…

Materials Science · Physics 2019-09-20 Fabien Tran , Jan Doumont , Leila Kalantari , Ahmad W. Huran , Miguel A. L. Marques , Peter Blaha

Our previously developed Constrained-Pairing Mean-Field Theory (CPMFT) is shown to map onto an Unrestricted Hartree-Fock (UHF) type method if one imposes a corresponding pair constraint to the correlation problem that forces occupation…

Strongly Correlated Electrons · Physics 2015-05-19 Takashi Tsuchimochi , Thomas M. Henderson , Gustavo E. Scuseria , Andreas Savin

Recent advances in X-ray free-electron laser diagnostics have enabled direct probing of the electronic structure under extreme pressures and temperatures, such as those encountered in stellar interiors and inertial confinement fusion…

Simulations in the warm dense matter regime using finite temperature Kohn-Sham density functional theory (FT-KS-DFT), while frequently used, are computationally expensive due to the partial occupation of a very large number of high-energy…

Materials Science · Physics 2018-04-04 Yael Cytter , Eran Rabani , Daniel Neuhauser , Roi Baer