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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

We present an orbital-resolved extension of the Hubbard $U$ correction to density-functional theory (DFT). Compared to the conventional shell-averaged approach, the prediction of energetic, electronic and structural properties is strongly…

Materials Science · Physics 2024-09-18 Eric Macke , Iurii Timrov , Nicola Marzari , Lucio Colombi Ciacchi

We develop a generalization of the Kohn-Sham density functional theory (KS-DFT) + Hubbard $U$ (DFT+$U$) method to the excited-state regime. This has the form of Hubbard $U$ corrected linear-response time-dependent DFT, or `TDDFT+$U$'.…

Strongly Correlated Electrons · Physics 2019-04-24 Okan K. Orhan , David D. O'Regan

Locality of compact one-electron orbitals expanded strictly in terms of local subsets of basis functions can be exploited in density functional theory (DFT) to achieve linear growth of computation time with systems size, crucial in…

Computational Physics · Physics 2021-10-01 Yifei Shi , Jessica Karaguesian , Rustam Z. Khaliullin

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

A recently proposed linear-scaling scheme for density-functional pseudopotential calculations is described in detail. The method is based on a formulation of density functional theory in which the ground state energy is determined by…

mtrl-th · Physics 2009-10-28 E. Hernandez , C. M. Goringe , M. J. Gillan

Accurate computational predictions of band gaps are of practical importance to the modeling and development of semiconductor technologies, such as (opto)electronic devices and photoelectrochemical cells. Among available electronic-structure…

Materials Science · Physics 2021-03-16 Nicole E. Kirchner-Hall , Wayne Zhao , Yihuang Xiong , Iurii Timrov , Ismaila Dabo

The magnetic, noncollinear parametrization of Dudarev's DFT+$U$ method is generalized to fully-relativistic ultrasoft pseudopotentials. We present the definition of the DFT+$U$ total energy functional, and the calculation of forces and…

Materials Science · Physics 2023-10-13 Luca Binci , Nicola Marzari

In electronic structure methods based on the correction of approximate density-functional theory (DFT) for systematic inaccuracies, Hubbard $U$ parameters may be used to quantify and amend the self-interaction errors ascribed to selected…

Strongly Correlated Electrons · Physics 2017-04-27 Glenn Moynihan , Gilberto Teobaldi , David D. O'Regan

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

We present a formulation of the density-functional theory + Hubbard model (DFT+U) method that is self-consistent over the choice of Hubbard projectors used to define the correlated subspaces. In order to overcome the arbitrariness in this…

Materials Science · Physics 2015-03-17 David D. O'Regan , Nicholas D. M. Hine , Mike C. Payne , Arash A. Mostofi

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

Several methods have been developed to improve the predictions of density functional theory (DFT) in the case of strongly correlated electron systems. Out of these approaches, DFT+$U$, which corresponds to a static treatment of the local…

Strongly Correlated Electrons · Physics 2025-04-01 Alberto Carta , Iurii Timrov , Peter Mlkvik , Alexander Hampel , Claude Ederer

Linear scaling density functional theory approaches to electronic structure are often based on the tendency of electrons to localize even in large atomic and molecular systems. However, in many cases of actual interest, for example in…

Chemical Physics · Physics 2022-03-25 Marcel David Fabian , Ben Shpiro , Roi Baer

Linear scaling methods for density-functional theory (DFT) simulations are formulated in terms of localised orbitals in real-space, rather than the delocalised eigenstates of conventional approaches. In local-orbital methods, relative to…

Materials Science · Physics 2011-05-30 N. D. M. Hine , M. Robinson , P. D. Haynes , C. -K. Skylaris , M. C. Payne , A. A. Mostofi

We present a tensor-structured algorithm for efficient large-scale DFT calculations by constructing a Tucker tensor basis that is adapted to the Kohn-Sham Hamiltonian and localized in real-space. The proposed approach uses an additive…

Computational Physics · Physics 2021-01-12 Chih-Chuen Lin , Phani Motamarri , Vikram Gavini

Density Functional Theory (DFT) has become the quasi-standard for ab-initio simulations for a wide range of applications. While the intrinsic cubic scaling of DFT was for a long time limiting the accessible system size to some hundred…

Materials Science · Physics 2018-02-23 Stephan Mohr , Marc Eixarch , Maximilian Amsler , Mervi J. Mantsinen , Luigi Genovese

While density functional theory (DFT) is widely applied for its combination of cost and accuracy, corrections (e.g., DFT+U) that improve it are often needed to tackle correlated transition-metal chemistry. In principle, the functional form…

Chemical Physics · Physics 2021-03-12 Akash Bajaj , Heather J. Kulik

A density functional theory (DFT) approach to computing transition metal oxide heat of formation without adjustable parameters is presented. Different degrees of $d$-electron localization in oxides are treated within the DFT+$U$ approach…

Materials Science · Physics 2022-04-01 Johannes Voss

Approximate semi-local density functional theory (DFT) is known to underestimate surface formation energies yet paradoxically overbind adsorbates on catalytic transition-metal oxide surfaces due to delocalization error. The low-cost DFT+U…

Materials Science · Physics 2021-11-24 Akash Bajaj , Heather J. Kulik
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