Pivotal role of intersite Hubbard interactions in Fe-doped α-MnO₂


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  "metadata": {
    "publication_date": "Jun 23, 2022, 09:31:50", 
    "_oai": {
      "id": "oai:materialscloud.org:1392"
    }, 
    "license": "Creative Commons Attribution 4.0 International", 
    "description": "We present a first-principles investigation of the structural, electronic, and magnetic properties of the pristine and Fe-doped \u03b1-MnO\u2082 using density-functional theory with extended Hubbard functionals. The onsite U and intersite V Hubbard parameters are determined from first principles and self-consistently using density-functional perturbation theory in the basis of L\u00f6wdin-orthogonalized atomic orbitals. First, we analyze the pristine \u03b1-MnO\u2082 and show that the C2-AFM spin configuration is the most energetically favorable, in agreement with the experimentally observed antiferromagnetic state. For the Fe-doped \u03b1-MnO\u2082 two types of doping are considered: Fe insertion in the 2 \u00d7 2 tunnels and partial substitution of Fe for Mn. The calculated formation energies show that the experimentally observed Fe insertion is energetically favorable only when intersite Hubbard interactions are taken into account. Moreover, we find that both types of doping preserve the C2-AFM spin configuration of the host lattice only when Hubbard V corrections are included. The oxidation state of Fe is found to be +2 and +4 in the case of the interstitial and substitutional doping, respectively, while the oxidation state of Mn is +4 in both cases. This work opens a door for accurate studies of other Mn oxides and complex transition-metal compounds when the localization of 3d electrons occurs in the presence of strong covalent interactions with ligands.", 
    "contributors": [
      {
        "familyname": "Mahajan", 
        "affiliations": [
          "School of Basic Sciences, Indian Institute of Technology Mandi, Himachal Pradesh 175075, India"
        ], 
        "email": "ruchika_mahajan@students.iitmandi.ac.in", 
        "givennames": "Ruchika"
      }, 
      {
        "familyname": "Kashyap", 
        "affiliations": [
          "School of Basic Sciences, Indian Institute of Technology Mandi, Himachal Pradesh 175075, India"
        ], 
        "email": "arti@iitmandi.ac.in", 
        "givennames": "Arti"
      }, 
      {
        "familyname": "Timrov", 
        "affiliations": [
          "Theory and Simulation of Materials (THEOS), and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), \u00c9cole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland"
        ], 
        "email": "iurii.timrov@epfl.ch", 
        "givennames": "Iurii"
      }
    ], 
    "edited_by": 755, 
    "title": "Pivotal role of intersite Hubbard interactions in Fe-doped \u03b1-MnO\u2082", 
    "conceptrecid": "1345", 
    "license_addendum": null, 
    "doi": "10.24435/materialscloud:8n-bm", 
    "mcid": "2022.83", 
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    ], 
    "id": "1392", 
    "keywords": [
      "MnO2", 
      "DFT+U", 
      "DFT+U+V", 
      "crystal structure", 
      "density of states", 
      "density-functional theory", 
      "Hubbard parameters", 
      "self-interactions", 
      "magnetic moment", 
      "band gap", 
      "spin configuration", 
      "Hubbard projectors", 
      "orthogonalized atomic orbitals", 
      "Fe-doped MnO2", 
      "oxidation state", 
      "formation energy", 
      "Interstitial doping", 
      "substitutional doping", 
      "bond length", 
      "bond angles"
    ], 
    "is_last": true, 
    "status": "published", 
    "references": [
      {
        "type": "Journal reference", 
        "citation": "Ruchika Mahajan, Arti Kashyap and Iurii Timrov, Pivotal role of intersite Hubbard interactions in Fe-doped \u03b1-MnO\u2082 (submitted)"
      }
    ], 
    "version": 2, 
    "owner": 755
  }, 
  "id": "1392", 
  "created": "2022-06-23T04:49:11.858449+00:00", 
  "updated": "2022-07-04T13:09:33.702828+00:00"
}