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This chapter concerns with the recent development of a new DFT methodology for accurate, reliable prediction of many-electron systems. Background, need for such a scheme, major difficulties encountered, as well as their potential remedies…

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

Density functional theory is currently the most widely applied method in electronic structure theory. The Kohn-Sham method, based on a fictitious system of non-interacting particles, is the work horse of the theory. The particular form of…

Chemical Physics · Physics 2016-06-01 Hubertus J J van Dam

Density Functional Theory (DFT) is one of the most widely used methods for "ab initio" calculations of the structure of atoms, molecules, crystals, surfaces, and their interactions. Unfortunately, the customary introduction to DFT is often…

Physics Education · Physics 2010-12-07 Nathan Argaman , Guy Makov

Prediction of the stable crystal structure for multinary (ternary or higher) compounds with unexplored compositions demands fast and accurate evaluation of free energies in exploring the vast configurational space. The machine-learning…

Computational Physics · Physics 2021-01-04 Changho Hong , Jeong Min Choi , Wonseok Jeong , Sungwoo Kang , Suyeon Ju , Kyeongpung Lee , Jisu Jung , Yong Youn , Seungwu Han

The Hohenberg-Kohn (HK) theorem -- the bedrock of density functional theory (DFT) -- establishes a universal map from the external potential to the energy. It also relates the electron density and atomic forces to the variation of the…

Chemical Physics · Physics 2025-12-15 Sambit Das , Bikash Kanungo , Arghadwip Paul , Vikram Gavini

Recently, sophisticated deep learning-based approaches have been developed for generating efficient initial guesses to accelerate the convergence of density functional theory (DFT) calculations. While the actual initial guesses are often…

Chemical Physics · Physics 2026-03-24 Zhe Liu , Yuyan Ni , Zhichen Pu , Qiming Sun , Siyuan Liu , Wen Yan

Historically, materials discovery has been driven by a laborious trial-and-error process. The growth of materials databases and emerging informatics approaches finally offer the opportunity to transform this practice into data- and…

Materials Science · Physics 2017-06-28 Olexandr Isayev , Corey Oses , Cormac Toher , Eric Gossett , Stefano Curtarolo , Alexander Tropsha

Density functional theory is a successful branch of numerical simulations of quantum systems. While the foundations are rigorously defined, the universal functional must be approximated resulting in a `semi'-ab initio approach. The search…

Quantum Physics · Physics 2017-11-22 James Daniel Whitfield , Norbert Schuch , Frank Verstraete

Density functional theory (DFT) is a fundamental method for simulating quantum chemical properties, but it remains expensive due to the iterative self-consistent field (SCF) process required to solve the Kohn-Sham equations. Recently, deep…

Computational Physics · Physics 2025-10-23 Seongsu Kim , Nayoung Kim , Dongwoo Kim , Sungsoo Ahn

The stochastic density functional theory (DFT) [Phys. Rev. Lett. 111, 106402 (2013)] is a valuable linear scaling approach to Kohn-Sham DFT that does not rely on the sparsity of the density matrix. Linear (and often sub-linear) scaling is…

Chemical Physics · Physics 2019-02-20 Ming Chen , Roi Baer , Daniel Neuhauser , Eran Rabani

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 the existence of a nuclear Energy…

Nuclear Theory · Physics 2020-03-03 G. Accorto , P. Brandolini , F. Marino , A. Porro , A. Scalesi , G. Colò , X. Roca-Maza , E. Vigezzi

The accuracy of density-functional theory (DFT) is determined by the quality of the approximate functionals, such as exchange-correlation in electronic DFT and the excess functional in the classical DFT formalism of fluids. The exact…

First-principles simulations of electronic properties of hybrid inorganic/organic interfaces are challenging, as common density-functional theory (DFT) approximations target specific material classes like bulk semiconductors or gas-phase…

Materials Science · Physics 2023-02-13 Jannis Krumland , Caterina Cocchi

This work presents a theory to unify the two independent theoretical frameworks of Kohn-Sham (KS) density functional theory (DFT) and reduced density matrix functional theory (RDMFT). The generalization of the KS orbitals to hypercomplex…

Chemical Physics · Physics 2021-11-18 Neil Qiang Su

Total energies of crystal structures can be calculated to high precision using quantum-based density functional theory (DFT) methods, but the calculations can be time consuming and scale badly with system size. Cluster expansions of total…

Materials Science · Physics 2015-12-31 Qin Gao , Sanxi Yao , Jeff Schneider , Michael Widom

Kohn-Sham density functional theory (KS-DFT) is a powerful method to obtain key materials' properties, but the iterative solution of the KS equations is a numerically intensive task, which limits its application to complex systems. To…

Materials Science · Physics 2023-05-29 Bruno Focassio , Michelangelo Domina , Urvesh Patil , Adalberto Fazzio , Stefano Sanvito

Spherical density functional theory (DFT) is a reformulation of the classic theorems of DFT, in which the role of the total density of a many-electron system is replaced by a set of sphericalized densities, constructed by…

Chemical Physics · Physics 2025-11-17 Sol Samuels , Chance M. Baxter , Susan R. Atlas

Density functional theory underlies the most successful and widely used numerical methods for electronic structure prediction of solids. However, it has the fundamental shortcoming that the universal density functional is unknown. In…

Disordered Systems and Neural Networks · Physics 2020-09-23 M. Michael Denner , Mark H. Fischer , Titus Neupert

The calculation of electronic properties of materials is an important task of solid state theory, albeit particularly difficult if electronic correlations are strong, for example in transition metals, their oxides and in f-electron systems.…

Strongly Correlated Electrons · Physics 2009-09-29 K. Held

In the last few years several ``universal'' interatomic potentials have appeared, using machine-learning approaches to predict energy and forces of atomic configurations with arbitrary composition and structure, with an accuracy often…