Ruchika Mahajan^1*, Iurii Timrov^2*, Nicola Marzari^2*, Arti Kashyap^3*

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), https://doi.org/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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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