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arXiv · 2306.06286

On-site and inter-site Hubbard corrections in magnetic monolayers: The case of FePS$_3$ and CrI$_3$

Fatemeh Haddadi·Edward Linscott·Iurii Timrov·Nicola Marzari·Marco Gibertini
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Abstract

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.

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Fatemeh Haddadi, Edward Linscott, Iurii Timrov, Nicola Marzari, Marco Gibertini. 2023-06-09. On-site and inter-site Hubbard corrections in magnetic monolayers: The case of FePS$_3$ and CrI$_3$. https://doi.org/10.1103/physrevmaterials.8.014007

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