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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

The effect of the Hund's J terms in various DFT+U+J corrections to semi-local spin-density functional theory is assessed for a series of four octahedrally coordinated Fe(II) spin-crossover molecules spanning the covalent end of the ligand…

Strongly Correlated Electrons · Physics 2025-08-05 Lórien MacEnulty , João Paulo Almeida de Mendonça , Roberta Poloni , David D. O'Regan

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

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

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

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

In this article, we propose an energy functional at the level of DFT+U+V that allows us to compute self-consistently the values of the on-site interaction, Hubbard U and Hund J, as well as the intersite interaction V. This functional…

Strongly Correlated Electrons · Physics 2020-10-21 Nicolas Tancogne-Dejean , Angel Rubio

In approximate density functional theory (DFT), the self-interaction error is an electron delocalization anomaly associated with underestimated insulating gaps. It exhibits a predominantly quadratic energy-density curve that is amenable to…

Chemical Physics · Physics 2016-12-21 Glenn Moynihan , Gilberto Teobaldi , David D. O'Regan

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 explore the interplay of electron-electron correlations and surface effects in the prototypical correlated insulating material, NiO. In particular, we compute the electronic structure, magnetic properties, and surface energies of the…

Strongly Correlated Electrons · Physics 2021-04-09 I. Leonov , S. Biermann

First principles density functional theory (DFT) is used to investigate the electronic structure of \beta-MnO2. From collinear spin polarized calculations we find that DFT+U_Eff predicts a gapless ferromagnet in contrast with experiment…

Strongly Correlated Electrons · Physics 2012-11-26 David A. Tompsett , Derek S. Middlemiss , M. Saiful Islam

We present the implementation of the Hubbard ($U$) and Hund ($J$) corrected Density Functional Theory (DFT+$U$+$J$) functionality in the Quickstep program, which is part of the CP2K suite. The tensorial and L\"owdin subspace representations…

Strongly Correlated Electrons · Physics 2024-11-14 Ziwei Chai , Rutong Si , Mingyang Chen , Gilberto Teobaldi , David D. O'Regan , Li-Min Liu

The existence of band gaps in Mott insulators such as perovskite oxides with partially filled 3d shells has been traditionally explained in terms of strong, dynamic inter-electronic repulsion codified by the on-site repulsion energy U in…

Materials Science · Physics 2019-07-24 Julien Varignon , Manuel Bibes , Alex Zunger

We present a first-principles investigation of the structural, electronic, and magnetic properties of pyrolusite ($\beta$-MnO$_2$) using conventional and extended Hubbard-corrected density-functional theory (DFT+$U$ and DFT+$U$+$V$). The…

Materials Science · Physics 2021-10-06 Ruchika Mahajan , Iurii Timrov , Nicola Marzari , Arti Kashyap

This study investigates the predictive capabilities of common DFT methods (GGA, GGA+$U$, and GGA+$U$+$V$) for determining the transition temperature of antiferromagnetic insulators. We utilize a dataset of 29 compounds and derive Heisenberg…

Computational Physics · Physics 2024-03-19 Zahra Mosleh , Mojtaba Alaei

In this study, we evaluate the predictive power of density functional theory (DFT) for the magnetic properties of MnBi\(_2\)Te\(_4\) (MBT), an intrinsically magnetic topological insulator with potential applications in spintronics and…

Accurate first-principles predictions of the structural, electronic, magnetic, and electrochemical properties of cathode materials can be key in the design of novel efficient Li-ion batteries. Spinel-type cathode materials Li$_x$Mn$_2$O$_4$…

Materials Science · Physics 2023-03-30 Iurii Timrov , Michele Kotiuga , Nicola Marzari

We use the constrained random phase approximation (cRPA) method to calculate the Hubbard $U$ parameter in four one-dimensional magnetic transition metal atom oxides of composition XO$_2$ (X = Mn, Fe, Co, Ni) on Ir(100). In addition to the…

Materials Science · Physics 2022-08-31 J. Goikoetxea , C. Friedrich , G. Bihlmayer , S. Blügel , A. Arnau , M. Blanco-Rey

We present a phase-resolved investigation of Ni-based oxides and hydroxides relevant to the oxygen evolution reaction (OER), combining ground-state DFT+U calculations with operando and in situ Raman spectroscopy, supported by…

We calculate the screened electron-electron interaction for the charge-disproportionated insulator CaFeO$_3$ using the constrained random-phase approximation (cRPA). While in many correlated materials, the formation of a Mott-insulating…

Strongly Correlated Electrons · Physics 2024-03-05 Maximilian E. Merkel , Claude Ederer