2026-05-17T13:56:49Z https://archive.materialscloud.org/oai2d

oai:materialscloud.org:938 2021-07-16T11:56:15Z openaire_data community-mcarchive

Mahajan, Ruchika Timrov, Iurii Marzari, Nicola Kashyap, Arti Mahajan, Ruchika Timrov, Iurii Marzari, Nicola Kashyap, Arti 2021-07-16 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. text/plain application/x-bzip2 text/markdown https://doi.org/10.24435/materialscloud:bf-cz oai:materialscloud.org:938 mcid:2021.109 eng Materials Cloud https://arxiv.org/abs/2106.00520 https://doi.org/10.1103/PhysRevMaterials.5.104402 https://archive.materialscloud.org/communities/mcarchive https://doi.org/10.24435/materialscloud:32-xv info:eu-repo/semantics/openAccess Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode 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 Importance of intersite Hubbard interactions in β-MnO2: A first-principles DFT+U+V study info:eu-repo/semantics/other