by Nelson Naveas, Ruth Pulido, Carlo Marini, Jacobo Hernández-Montelongo and Miguel Manso Silván
Abstract:
Owing to the confined Fe-3d orbitals and self-interaction error of exchange-correlation functionals, approximate DFT fails to describe iron oxides electronic structure and magnetic properties accurately. Hybrid DFT or DFT + U can solve these problems, but the former is expensive, and the latter only considers on-site interactions. Here, we used DFT + U + V, a DFT + U extension including inter-site interactions, to simulate the structural, magnetic, and electronic properties, along with Fe and O K-edge XAS spectra of α-Fe2O3. Two types of atomic orbital projectors were studied, orthogonalized and non-orthogonalized. DFT + U + V improves the description of the structural, magnetic, and electronic properties of α-Fe2O3 compared to approximate DFT. The accuracy of the correction depends on the orbital projector used. DFT + U + V with orthogonalized projectors achieves the best experimental agreement at a fraction of hybrid DFT cost. This work emphasizes the importance of inter-site interactions and the type of atomic orbital projectors used in the theoretical research of α-Fe2O3.
Reference:
Nelson Naveas, Ruth Pulido, Carlo Marini, Jacobo Hernández-Montelongo and Miguel Manso Silván, “First-principles calculations of hematite (α-Fe2O3) by self-consistent DFT+U+V”, iScience, vol. 26, no. 2, pp. 106033.
Bibtex Entry:
@article{naveas_first-principles_2023,
title = {First-principles calculations of hematite (α-{Fe2O3}) by self-consistent {DFT}+{U}+{V}},
volume = {26},
issn = {2589-0042},
url = {https://www.sciencedirect.com/science/article/pii/S2589004223001104},
doi = {10.1016/j.isci.2023.106033},
abstract = {Owing to the confined Fe-3d orbitals and self-interaction error of exchange-correlation functionals, approximate DFT fails to describe iron oxides electronic structure and magnetic properties accurately. Hybrid DFT or DFT + U can solve these problems, but the former is expensive, and the latter only considers on-site interactions. Here, we used DFT + U + V, a DFT + U extension including inter-site interactions, to simulate the structural, magnetic, and electronic properties, along with Fe and O K-edge XAS spectra of α-Fe2O3. Two types of atomic orbital projectors were studied, orthogonalized and non-orthogonalized. DFT + U + V improves the description of the structural, magnetic, and electronic properties of α-Fe2O3 compared to approximate DFT. The accuracy of the correction depends on the orbital projector used. DFT + U + V with orthogonalized projectors achieves the best experimental agreement at a fraction of hybrid DFT cost. This work emphasizes the importance of inter-site interactions and the type of atomic orbital projectors used in the theoretical research of α-Fe2O3.},
number = {2},
urldate = {2023-12-15},
journal = {iScience},
author = {Naveas, Nelson and Pulido, Ruth and Marini, Carlo and Hernández-Montelongo, Jacobo and Silván, Miguel Manso},
month = feb,
year = {2023},
keywords = {Magnetism, Computational physics, Condensed matter properties},
pages = {106033},
file = {ScienceDirect Snapshot:E:\Usuarios\Administrator\Zotero\storage\JZ4Q6AU9\S2589004223001104.html:text/html;Texto completo:E:\Usuarios\Administrator\Zotero\storage\A3KJIVE7\Naveas et al. - 2023 - First-principles calculations of hematite (α-Fe2O3.pdf:application/pdf},
}