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We present a critical analysis of the popular fragment-orbital density-functional theory (FO-DFT) scheme for the calculation of electronic coupling values. We discuss the characteristics of different possible formulations or 'flavors' of…

Materials Science · Physics 2016-02-17 Christoph Schober , Karsten Reuter , Harald Oberhofer

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

Density functional theory augmented with Hubbard-$U$ corrections (DFT+$U$) is currently one of the widely used methods for first-principles electronic structure modeling of insulating transition metal oxides (TMOs). Since $U$ is relatively…

Computational Physics · Physics 2018-05-09 Samara Keshavarz , Johan Schött , Andrew J. Millis , Yaroslav O. Kvashnin

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

Correct prediction of the behavior of UO2 crystal, which is an antiferromagnetic system with strongly-correlated electrons, is possible by using a modified density functional theory, the DFT+U method. In the context of DFT+U, the energy of…

Materials Science · Physics 2024-04-29 Mahmoud Payami

Approximate density functional theory (DFT) has become indispensable owing to its cost-accuracy trade-off in comparison to more computationally demanding but accurate correlated wavefunction theory. To date, however, no single density…

Chemical Physics · Physics 2022-07-25 Chenru Duan , Aditya Nandy , Ralf Meyer , Naveen Arunachalam , Heather J. Kulik

State-specific orbital optimized approaches are more accurate at predicting core-level spectra than traditional linear-response protocols, but their utility had been restricted on account of the risk of `variational collapse' down to the…

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

We introduce a practical hybrid approach that combines orbital-free density functional theory (DFT) with Kohn-Sham DFT for speeding up first-principles molecular dynamics simulations. Equilibrated ionic configurations are generated using…

We propose a hybrid approach which employs the dynamical mean-field theory (DMFT) self-energy for the correlated, typically rather localized orbitals and a conventional density functional theory (DFT) exchange-correlation potential for the…

Strongly Correlated Electrons · Physics 2021-06-16 Sumanta Bhandary , Karsten Held

In the Letter [J. Nucl. Mater. 444, 356 (2014)] and Comment [Phys Rev B 90, 157101 (2014)], Soderlind et al. argue that 1) DFT based on GGA already models U metal and U-Zr alloy accurately, and 2) DFT + U models them worse than DFT…

Materials Science · Physics 2016-02-01 Wei Xie , Chris A. Marianetti , Dane Morgan

Nuclear density functional theory (DFT) is the only microscopic, global approach to the structure of atomic nuclei. It is used in numerous applications, from determining the limits of stability to gaining a deep understanding of the…

Nuclear Theory · Physics 2015-02-06 Nicolas Schunck , Jordan D. McDonnell , Jason Sarich , Stefan M. Wild , Dave Higdon

Here, we report orbital-free density-functional theory (OF DFT) molecular dynamics simulations of the displacement cascade in aluminum. The electronic effect is our main concern. The displacement threshold energies are calculated using OF…

Materials Science · Physics 2017-09-26 Ruizhi Qiu

We study static correlation and delocalisation errors and show that even methods with good energies can yield significant delocalization errors that affect the density, leading to large errors in predicting {\em e.g.} dipole moments. We…

Chemical Physics · Physics 2020-06-01 Maria Hellgren , Tim Gould

Understanding how structural flexibility affects the properties of metal-organic frameworks (MOFs) is crucial for the design of better MOFs for targeted applications. Flexible MOFs can be studied with molecular dynamics simulations, whose…

Materials Science · Physics 2024-05-13 Abhishek Sharma , Stefano Sanvito

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

Density functional theory plus $U$ (DFT+$U$) is one of the most efficient first-principles methods to simulate the cold pressure properties of strongly-correlated materials. However, the applicability of DFT+$U$ at ultra-high pressure is…

The ab initio computational method known as Hubbard-corrected density functional theory (DFT+$U$) captures well ground electronic structures of a set of solids that are poorly described by standard DFT alone. Since lattice dynamical…

Materials Science · Physics 2025-06-17 Wooil Yang , Sabyasachi Tiwari , Feliciano Giustino , Young-Woo Son

Electron transfer with changing occupation in the 4f subshell poses a considerable challenge for quantitative predictions in quantum chemistry. Using the example of cerium oxide, we identify the main deficiencies of common…

Chemical Physics · Physics 2021-12-07 Tobias Schäfer , Nathan Daelman , Núria López

The formalism of electronic density-functional-theory, with Hubbard-U corrections (DFT+U), is employed in a computational study of the energetics of U_{1-x} Ce_x O_2 mixtures. The computational approach makes use of a procedure which…

Materials Science · Physics 2012-03-08 B. E. Hanken , C. R. Stanek , N. Grønbech-Jensen , M. Asta
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