Hubbard U through polaronic defect states

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{
  "revision": 5, 
  "id": "1587", 
  "created": "2022-12-15T20:58:48.755030+00:00", 
  "metadata": {
    "doi": "10.24435/materialscloud:g7-0z", 
    "status": "published", 
    "title": "Hubbard U through polaronic defect states", 
    "mcid": "2023.4", 
    "license_addendum": null, 
    "_files": [
      {
        "description": "Atomic structures of the materials considered in this work", 
        "key": "structures.zip", 
        "size": 32706, 
        "checksum": "md5:e1e309ddf0677ecdd72016bc8202f810"
      }, 
      {
        "description": "README file", 
        "key": "README.txt", 
        "size": 998, 
        "checksum": "md5:8621ca6cfc6a5afb32bdca8422a49b76"
      }
    ], 
    "owner": 143, 
    "_oai": {
      "id": "oai:materialscloud.org:1587"
    }, 
    "keywords": [
      "Polarons", 
      "density-functional theory", 
      "DFT+U", 
      "hybrid functionals", 
      "self-interaction"
    ], 
    "conceptrecid": "1586", 
    "is_last": true, 
    "references": [
      {
        "type": "Journal reference", 
        "doi": "10.1038/s41524-022-00958-6", 
        "url": "https://doi.org/10.1038/s41524-022-00958-6", 
        "comment": "Paper in which the method is described", 
        "citation": "Falletta, S., Pasquarello, A. Hubbard U through polaronic defect states, npj Computational Materials 8, 263 (2022)"
      }
    ], 
    "publication_date": "Jan 06, 2023, 11:10:29", 
    "license": "Creative Commons Attribution 4.0 International", 
    "id": "1587", 
    "description": "Since the preliminary work of Anisimov and co-workers, the Hubbard corrected DFT+U functional has been used for predicting properties of correlated materials by applying on-site effective Coulomb interactions to specific orbitals. However, the determination of the Hubbard U parameter has remained under intense discussion despite the multitude of approaches proposed. Here, we define a selection criterion based on the use of polaronic defect states for the enforcement of the piecewise linearity of the total energy upon electron occupation. A good agreement with results from piecewise-linear hybrid functionals is found for the electronic and structural properties of polarons, including the formation energies. The values of U determined in this way are found to give a robust description of the polaron energetics upon variation of the considered state. In particular, we also address a polaron hopping pathway, finding that the determined value of U leads to accurate energetics without requiring a configurational-dependent U. It is emphasized that the selection of U should be based on physical properties directly associated with the orbitals to which U is applied, rather than on more global properties such as band gaps and band widths.  For comparison, we also determine U through a well-established linear-response scheme finding noticeably different values of U and consequently different formation energies. Possible origins of these discrepancies are discussed. As case studies, we consider the self-trapped electron in BiVO\u2084, the self-trapped hole in MgO, the Li-trapped hole in MgO, and the Al-trapped hole in \ud835\udefc-SiO\u2082.", 
    "version": 1, 
    "contributors": [
      {
        "email": "stefano.falletta@epfl.ch", 
        "affiliations": [
          "Chaire de Simulation \u00e0 l'Echelle Atomique (CSEA), Ecole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland"
        ], 
        "familyname": "Falletta", 
        "givennames": "Stefano"
      }, 
      {
        "email": "alfredo.pasquarello@epfl.ch", 
        "affiliations": [
          "Chaire de Simulation \u00e0 l'Echelle Atomique (CSEA), Ecole Polytechnique F\u00e9d\u00e9rale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland"
        ], 
        "familyname": "Pasquarello", 
        "givennames": "Alfredo"
      }
    ], 
    "edited_by": 576
  }, 
  "updated": "2023-01-06T10:10:30.007198+00:00"
}