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Importance of intersite Hubbard interactions in β-MnO2: A first-principles DFT+U+V study

Ruchika Mahajan1*, Iurii Timrov2*, Nicola Marzari2*, Arti Kashyap3*

1 School of Basic Sciences, Indian Institute of Technology Mandi, Himachal Pradesh 175075, India

2 Theory and Simulation of Materials (THEOS), and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland

3 School of Basic Sciences, Indian Institute of Technology Mandi, Himachal Pradesh 175075, India

* Corresponding authors emails: ruchika_mahajan@students.iitmandi.ac.in, iurii.timrov@epfl.ch, nicola.marzari@epfl.ch, arti@iitmandi.ac.in
DOI10.24435/materialscloud:bf-cz [version v1]

Publication date: Jul 16, 2021

How to cite this record

Ruchika Mahajan, Iurii Timrov, Nicola Marzari, Arti Kashyap, Importance of intersite Hubbard interactions in β-MnO2: A first-principles DFT+U+V study, Materials Cloud Archive 2021.109 (2021), doi: 10.24435/materialscloud:bf-cz.

Description

We present a first-principles investigation of the structural, electronic, and magnetic properties of pyrolusite (β-MnO2) using conventional and extended Hubbard-corrected density-functional theory (DFT+U and DFT+U+V). The onsite U and intersite V Hubbard parameters are computed using linear-response theory in the framework of density-functional perturbation theory. We show that while the inclusion of the onsite U is crucial to describe the localized nature of the Mn(3d) states, the intersite V is key to capture accurately the strong hybridization between neighboring Mn(3d) and O(2p) states. In this framework, we stabilize the simplified collinear antiferromagnetic (AFM) ordering (suggested by the Goodenough-Kanamori rule) that is commonly used as an approximation to the experimentally-observed noncollinear screw-type spiral magnetic ordering. A detailed investigation of the ferromagnetic and of other three collinear AFM spin configurations is also presented. The findings from Hubbard-corrected DFT are discussed using two kinds of Hubbard manifolds -- nonorthogonalized and orthogonalized atomic orbitals -- showing that special attention must be given to the choice of the Hubbard projectors, with orthogonalized manifolds providing more accurate results than nonorthogonalized ones within DFT+U+V. This work paves the way for future studies of complex transition-metal compounds containing strongly localized electrons in the presence of pronounced covalent interactions.

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External references

Preprint (Preprint where the data is discussed)
Journal reference (Paper where the data is discussed)
Ruchika Mahajan, Iurii Timrov, Nicola Marzari, Arti Kashyap, Phys. Rev. Materials 5, 104402 (2021).

Keywords

MnO2 DFT+U DFT+U+V crystal structure density of states density-functional theory Hubbard parameters CSCS MARVEL/OSP SNSF self-interactions magnetic moment band gap spin configuration Goodenough-Kanamori rule Hubbard projectors orthogonalized atomic orbitals nonorthogonalized atomic orbitals

Version history:

2021.109 (version v1) [This version] Jul 16, 2021 DOI10.24435/materialscloud:bf-cz