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Approximate functionals used in practical density functional theory (DFT) deviate from the piecewise linear behavior of the exact functional for fractional charges. This deviation causes excess charge delocalization, which leads to…

Chemical Physics · Physics 2018-10-23 Diptarka Hait , Martin Head-Gordon

Orbital-free density functional theory (OF-DFT) runs at low computational cost that scales linearly with the number of simulated atoms, making it suitable for large-scale material simulations. It is generally considered that OF-DFT strictly…

Materials Science · Physics 2022-04-05 Qiang Xu , Cheng Ma , Wenhui Mi , Yanchao Wang , Yanming Ma

We formulate the on-site occupation dependent exchange correlation energy and effective potential of hybrid functionals for localized states and connect them to the on-site correction term of the DFT+U method. Our derivation provides a…

Strongly Correlated Electrons · Physics 2015-05-22 Viktor Ivády , Rickard Armiento , Krisztián Szász , Erik Janzén , Adam Gali , Igor A. Abrikosov

Developing reliable pseudopotentials for orbital-free density functional theory (OF-DFT), especially for transition metals, remains a significant challenge. In this study, we provide a theoretical framework for analyzing pseudization…

The density functional theory (DFT)+$U$ method is a pragmatic and effective approach for calculating the ground-state properties of strongly-correlated systems, and linear response calculations are widely used to determine the requisite…

Strongly Correlated Electrons · Physics 2018-12-31 Edward B. Linscott , Daniel J. Cole , Michael C. Payne , David D. O'Regan

The combination of density functional theory with dynamical mean-field theory (DFT+DMFT) has become a powerful first-principles approach to tackle strongly correlated materials in condensed matter physics. The wide use of this approach…

Strongly Correlated Electrons · Physics 2022-05-10 Xin Qu , Peng Xu , Rusong Li , Gang Li , Lixin He , Xinguo Ren

Dynamical Mean-Field Theory (DMFT) has established itself as a reliable and well-controlled approximation to study correlation effects in bulk solids and also two-dimensional systems. In combination with standard density-functional theory…

Atomic and Molecular Clusters · Physics 2015-05-30 V. Turkowski , A. Kabir , N. Nayyar , Talat S. Rahman

We present a formulation and implementation of the DFT+\textit{U} method within the framework of linear combination of numerical atomic orbitals (NAO). Our implementation not only enables single-point total energy and electronic-structure…

Materials Science · Physics 2022-06-29 Xin Qu , Peng Xu , Hong Jiang , Lixin He , Xinguo Ren

Multipolar magnetic phases in correlated insulators represent a great challenge for Density Functional Theory (DFT) due to the coexistence of intermingled interactions, typically spin-orbit coupling, crystal field and complex non-collinear…

Strongly Correlated Electrons · Physics 2022-07-27 Dario Fiore Mosca , Leonid V. Pourovskii , Cesare Franchini

We present an approach to the DFT+U method (Density Functional Theory + Hubbard model) within which the computational effort for calculation of ground state energies and forces scales linearly with system size. We employ a formulation of…

Strongly Correlated Electrons · Physics 2012-02-14 David D. O'Regan , Nicholas D. M. Hine , Mike C. Payne , Arash A. Mostofi

Density functional theory (DFT) embedding provides a formally exact framework for interfacing correlated wave-function theory (WFT) methods with lower-level descriptions of electronic structure. Here, we report techniques to improve the…

Chemical Physics · Physics 2015-06-12 Jason D. Goodpaster , Taylor A. Barnes , Frederick R. Manby , Thomas F. Miller

Quantum mechanical methods based on the density functional theory (DFT) offer a realistic possibility of first-principles design of organic donor-acceptor systems and engineered band-gap materials. This promise is contingent upon the…

Chemical Physics · Physics 2013-12-03 Marcin Modrzejewski , Grzegorz Chałasiński , Małgorzata M. Szczęśniak

Accurately modeling compounds with partially filled $d$ and $f$ shells remains a hard challenge for density-functional theory, due to large self-interaction errors stemming from local or semi-local exchange-correlation functionals. Hubbard…

Materials Science · Physics 2026-01-19 Kinga Warda , Eric Macke , Iurii Timrov , Lucio Colombi Ciacchi , Piotr M. Kowalski

A detailed exploration of the $f$-atomic orbital occupancy space for UO$_2$ is performed using a first principles approach based on density functional theory (DFT), employing a full hybrid functional within a systematic basis set.…

Strongly Correlated Electrons · Physics 2022-01-05 Laura E. Ratcliff , Luigi Genovese , Hyowon Park , Peter B. Littlewood , Alejandro Lopez-Bezanilla

Density functional theory (DFT) underpins modern atomistic simulations of transition-metal surfaces. It can predict key properties linked to catalytic performance, such as adsorption energies and barrier heights, enabling new paradigms in…

Materials Science · Physics 2026-03-23 Benjamin X. Shi , Timothy C. Berkelbach

Density functional theory (DFT) provides a theoretical framework for efficient and fairly accurate calculations of the electronic structure of molecules and crystals. The main features of density functional theory are described and DFT…

Chemical Physics · Physics 2012-06-12 Hauke Paulsen , Alfred Xaver Trautwein

In this article we introduce a generalization of the popular DFT+U method based on the extended Hubbard model that includes on-site and inter-site electronic interactions. The novel corrective Hamiltonian is designed to study systems for…

Strongly Correlated Electrons · Physics 2015-05-13 Vivaldo Leiria Campo , Matteo Cococcioni

Orbital-optimized density functional theory (DFT) has emerged as an alternative to time-dependent (TD) DFT capable of describing difficult excited states with significant electron density redistribution, such as charge-transfer, Rydberg,…

Chemical Physics · Physics 2025-01-22 Hanh D. M. Pham , Rustam Z. Khaliullin

Contradictory theoretical results for oxygen vacancies in SrTiO$_3$ (STO) were often related to the peculiar properties of STO, which is a $d^0$ transition metal oxide with mixed ionic-covalent bonding. Here, we apply, for the first time,…

Materials Science · Physics 2020-07-01 Chiara Ricca , Iurii Timrov , Matteo Cococcioni , Nicola Marzari , Ulrich Aschauer

We present and discuss results of a density functional theory (DFT) study of a perfect UO2 crystals and He atoms in octahedral interstitial positions. We have calculated basic bulk crystal properties and He incorporation energies into the…

Materials Science · Physics 2019-03-27 Denis Gryaznov , Eugene Heifets , Eugene Kotomin