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The magnetic ground state of FeRh is highly sensitive towards the lattice constant. This, in addition to partially filled d-shells of Fe and Rh, posed a significant challenge for Density Functional Theory (DFT) calculations in the past.…

Materials Science · Physics 2024-01-24 Shishir Kumar Pandey , Saikat Debnath , Zhanghao Zhouyina , Qiangqiang Gu

The semilocal meta generalized gradient approximation (MGGA) for the exchange-correlation functional of Kohn-Sham (KS) density functional theory can yield accurate ground-state energies simultaneously for atoms, molecules, surfaces, and…

Chemical Physics · Physics 2012-05-04 Jianwei Sun , Bing Xiao , Adrienn Ruzsinszky

Transition-metal compounds (TMCs) with open-shell d-electrons are characterized by a complex interplay of lattice, charge, orbital, and spin degrees of freedom, giving rise to a diverse range of fascinating applications. Often exhibiting…

Materials Science · Physics 2025-03-19 Yubo Zhang , Akilan Ramasamy , Kanun Pokharel , James W. Furness , Jinliang Ning , Ruiqi Zhang , Jianwei Sun

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 design of better exchange-correlation functionals for Density Functional Theory (DFT) is a central challenge of modern electronic structure theory. However, current developments are limited by the mathematical form of the functional,…

Chemical Physics · Physics 2024-08-19 Kyle Bystrom , Boris Kozinsky

A hybrid Kohn-Sham Density Functional Theory (KS-DFT) and 1-electron Reduced Density Matrix Functional Theory (1-RDMFT) has recently been developed to describe strongly correlated systems at mean-field computational cost. This approach…

Computational Physics · Physics 2025-04-14 Daniel Gibney , Jan-Niklas Boyn

The Jacob's ladder of density functional theory (DFT) proposes the compelling view that by extending the form of successful approximations -- being guided by exact conditions and selected (least empirical) norms -- upper rungs will do…

Materials Science · Physics 2025-02-25 Jacques K. Desmarais , Alessandro Erba , Giovanni Vignale , Stefano Pittalis

Mejia-Rodriguez and Trickey recently proposed a procedure for removing the explicit dependence of meta-GGA exchange-correlation energy functionals $E_{\rm xc}$ on the kinetic energy density $\tau$. We present a simple modification to this…

Materials Science · Physics 2024-04-22 Pietro Bonfà , Sangeeta Sharma , John Kay Dewhurst

Density Functional Theory (DFT) underpins much of modern computational chemistry and materials science. Yet, the reliability of DFT-derived predictions of experimentally measurable properties remains fundamentally limited by the need to…

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

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

During the past decades, approximate Kohn-Sham density-functional theory schemes garnered many successes in computational chemistry and physics; yet the performance in the prediction of spin state energetics is often unsatisfactory. By…

Other Condensed Matter · Physics 2023-05-05 Joao Paulo Almeida de Mendonca , Lorenzo A. Mariano , Emilie Devijver , Noel Jakse , Roberta Poloni

Practical density functional theory (DFT) owes its success to the groundbreaking work of Kohn and Sham that introduced the exact calculation of the non-interacting kinetic energy of the electrons using an auxiliary mean-field system.…

Chemical Physics · Physics 2023-11-17 P. del Mazo-Sevillano , J. Hermann

Improving the predictive capability of molecular properties in ab initio simulations is essential for advanced material discovery. Despite recent progress making use of machine learning, utilizing deep neural networks to improve quantum…

Chemical Physics · Physics 2021-09-22 Muhammad F. Kasim , Sam M. Vinko

Deorbitalization of a conventional meta-generalized-gradient exchange-correlation approximation replaces its dependence upon the Kohn-Sham kinetic energy density with a dependence on the density gradient and Laplacian. In principle, that…

Materials Science · Physics 2026-02-13 H. Francisco , B. Thapa , S. B. Trickey , A. C. Cancio

The widespread use of (generalized) Kohn-Sham density functional theory (KS-DFT) lies in the fact that hierarchical sets of approximations of the exchange-correlation (XC) energy functional can be designed, offering versatile choices to…

Materials Science · Physics 2023-01-31 Igor Ying Zhang , Xinguo Ren

The accurate description of open-shell molecules, in particular of transition metal complexes and clusters, is still an important challenge for quantum chemistry. While density-functional theory (DFT) is widely applied in this area, the…

Chemical Physics · Physics 2012-10-26 Christoph R. Jacob , Markus Reiher

The Kohn-Sham gaps of density functional theory (DFT) obtained in terms of local density approximation (LDA) or generalized gradient approximation (GGA) cannot be directly linked to the fundamental gaps of semiconductors, but in engineering…

Materials Science · Physics 2024-09-17 Hanli Cui , Shengxin Yang , Jun-Hui Yuan , Li-Heng Li , Fan Ye , Jinhai Huang , Kan-Hao Xue , Xiangshui Miao

In density functional theory (DFT), exact constraints, fundamental mathematical properties of the exchange-correlation (XC) energy and its underlying XC hole, along with paradigm systems such as the uniform electron gas and the hydrogen…

Materials Science · Physics 2026-03-13 Yan Oueis , Akilan Ramasamy , James W. Furness , Jamin Kidd , Timo Lebeda , Jianwei Sun

Rare-earth oxides (REOs) are an important class of materials owing to their unique properties, including high ionic conductivities, large dielectric constants, and elevated melting temperatures, making them relevant to several technological…