On-site and inter-site Hubbard corrections in magnetic monolayers: The case of FePS$_3$ and CrI$_3$
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arXiv
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| Format: | Preprint |
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2023
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| _version_ | 1866929231324250112 |
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| author | Haddadi, Fatemeh Linscott, Edward Timrov, Iurii Marzari, Nicola Gibertini, Marco |
| author_facet | Haddadi, Fatemeh Linscott, Edward Timrov, Iurii Marzari, Nicola Gibertini, Marco |
| contents | 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+$\textit{U}$ and its extensions PBEsol+$\textit{U}$+$\textit{V}$ to investigate the electronic, structural, and vibrational properties of 2D antiferromagnetic FePS$_3$ and ferromagnetic CrI$_3$, and compare the monolayers with their bulk counterparts. Hubbard parameters (on-site $\textit{U}$ and inter-site $\textit{V}$) are computed self-consistently using density-functional perturbation theory, thus avoiding any empirical assumptions. We show that for FePS$_3$ 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. For ferromagnetic CrI$_3$, 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 $\textit{U}$ 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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2306_06286 |
| institution | arXiv |
| publishDate | 2023 |
| record_format | arxiv |
| spellingShingle | On-site and inter-site Hubbard corrections in magnetic monolayers: The case of FePS$_3$ and CrI$_3$ Haddadi, Fatemeh Linscott, Edward Timrov, Iurii Marzari, Nicola Gibertini, Marco Materials Science Mesoscale and Nanoscale Physics 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+$\textit{U}$ and its extensions PBEsol+$\textit{U}$+$\textit{V}$ to investigate the electronic, structural, and vibrational properties of 2D antiferromagnetic FePS$_3$ and ferromagnetic CrI$_3$, and compare the monolayers with their bulk counterparts. Hubbard parameters (on-site $\textit{U}$ and inter-site $\textit{V}$) are computed self-consistently using density-functional perturbation theory, thus avoiding any empirical assumptions. We show that for FePS$_3$ 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. For ferromagnetic CrI$_3$, 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 $\textit{U}$ 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. |
| title | On-site and inter-site Hubbard corrections in magnetic monolayers: The case of FePS$_3$ and CrI$_3$ |
| topic | Materials Science Mesoscale and Nanoscale Physics |
| url | https://arxiv.org/abs/2306.06286 |