On-site and inter-site Hubbard corrections in magnetic monolayers: The case of FePS₃ and CrI₃
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{
"revision": 12,
"id": "1743",
"created": "2023-04-19T16:32:56.259514+00:00",
"metadata": {
"doi": "10.24435/materialscloud:ez-6k",
"status": "published",
"title": "On-site and inter-site Hubbard corrections in magnetic monolayers: The case of FePS\u2083 and CrI\u2083",
"mcid": "2024.18",
"license_addendum": null,
"_files": [
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"keywords": [
"DFT",
"DFT+U",
"DFT+U+V",
"first principles",
"Hubbard",
"2D materials",
"2D magnets",
"cscs",
"MARVEL/DD3",
"EPFL",
"Quantum ESPRESSO"
],
"conceptrecid": "1742",
"is_last": true,
"references": [
{
"type": "Journal reference",
"doi": "https://doi.org/10.1103/PhysRevMaterials.8.014007",
"url": "https://journals.aps.org/prmaterials/abstract/10.1103/PhysRevMaterials.8.014007",
"citation": "F. Haddadi, E. Linscott, I. Timrov, N. Marzari, M. Gibertini, Phys. Rev. Materials 8, 014007 (2024)"
},
{
"type": "Preprint",
"doi": "https://doi.org/10.48550/arXiv.2306.06286",
"url": "https://arxiv.org/abs/2306.06286",
"citation": "F. Haddadi, E. Linscott, I. Timrov, N. Marzari, M. Gibertini, arXiv:2306.06286"
}
],
"publication_date": "Jan 30, 2024, 16:00:36",
"license": "Creative Commons Attribution 4.0 International",
"id": "1743",
"description": "Hubbard-corrected density-functional theory has proven to be successful in addressing self-interaction errors in 3D magnetic materials. However, the effectiveness of this approach for 2D magnetic materials has not been extensively explored. Here, we use PBEsol+U and its extensions PBEsol+U+V to investigate the electronic, structural, and vibrational properties of 2D antiferromagnetic FePS\u2083 and ferromagnetic CrI\u2083, and compare the monolayers with their bulk counterparts. Hubbard parameters (on-site U and inter-site V) are computed self-consistently using density-functional perturbation theory, thus avoiding any empirical assumptions. We show that for FePS\u2083 the Hubbard corrections are crucial in obtaining the experimentally observed insulating state with the correct crystal symmetry, providing also vibrational frequencies in good agreement with Raman experiments. While empirical U can lead to an unstable ground-state (i.e. imaginary phonons), the system remains stable through the self-consistent process of calculating Hubbard parameters. \nFor ferromagnetic CrI\u2083, we discuss how a straightforward application of Hubbard corrections worsens the results and introduces a spurious separation between spin-majority and minority conduction bands. Promoting the Hubbard U to be a spin-resolved parameter \u2014 that is, applying different (first-principles) values to the spin-up and spin-down manifolds \u2014 recovers a more physical picture of the electronic bands and delivers the best comparison with experiments.",
"version": 1,
"contributors": [
{
"email": "fatemeh.haddadi@epfl.ch",
"affiliations": [
"Theory and Simulation of Materials (THEOS), Ecole Polytechnique Federale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland",
"National Centre for Computational Design and Discovery of Novel Materials (MARVEL)"
],
"familyname": "Haddadi",
"givennames": "Fatemeh"
},
{
"email": "edward.linscott@epfl.ch",
"affiliations": [
"Theory and Simulation of Materials (THEOS), Ecole Polytechnique Federale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland"
],
"familyname": "Linscott",
"givennames": "Edward"
},
{
"email": "iurii.timrov@epfl.ch",
"affiliations": [
"Theory and Simulation of Materials (THEOS), Ecole Polytechnique Federale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland",
"National Centre for Computational Design and Discovery of Novel Materials (MARVEL)"
],
"familyname": "Timrov",
"givennames": "Iurii"
},
{
"email": "nicola.marzari@epfl.ch",
"affiliations": [
"Theory and Simulation of Materials (THEOS), Ecole Polytechnique Federale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland",
"National Centre for Computational Design and Discovery of Novel Materials (MARVEL)"
],
"familyname": "Marzari",
"givennames": "Nicola"
},
{
"email": "marco.gibertini@unimore.it",
"affiliations": [
"Dipartimento di Scienze Fisiche, Informatiche e Matematiche, University of Modena and Reggio Emilia, I-41125 Modena, Italy",
"Centro S3, CNR-Istituto Nanoscienze, I-41125 Modena, Italy"
],
"familyname": "Gibertini",
"givennames": "Marco"
}
],
"edited_by": 576
},
"updated": "2024-01-30T15:00:36.867873+00:00"
}