2026-05-27T15:37:44Z https://archive.materialscloud.org/oai2d

oai:materialscloud.org:1743 2024-01-30T16:00:36Z openaire_data community-mcarchive

Haddadi, Fatemeh Linscott, Edward Timrov, Iurii Marzari, Nicola Gibertini, Marco Haddadi, Fatemeh Linscott, Edward Timrov, Iurii Marzari, Nicola Gibertini, Marco 2024-01-30 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 FePS₃ and ferromagnetic CrI₃, 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 FePS₃ 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. For ferromagnetic CrI₃, 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 — that is, applying different (first-principles) values to the spin-up and spin-down manifolds — recovers a more physical picture of the electronic bands and delivers the best comparison with experiments. application/gzip text/markdown text/plain https://doi.org/10.24435/materialscloud:ez-6k oai:materialscloud.org:1743 mcid:2024.18 eng Materials Cloud https://doi.org/10.1103/PhysRevMaterials.8.014007 https://doi.org/10.48550/arXiv.2306.06286 https://archive.materialscloud.org/communities/mcarchive https://doi.org/10.24435/materialscloud:ce-bp info:eu-repo/semantics/openAccess Creative Commons Attribution 4.0 International https://creativecommons.org/licenses/by/4.0/legalcode DFT DFT+U DFT+U+V first principles Hubbard 2D materials 2D magnets cscs MARVEL/DD3 EPFL Quantum ESPRESSO On-site and inter-site Hubbard corrections in magnetic monolayers: The case of FePS₃ and CrI₃ info:eu-repo/semantics/other