Recommended by

Indexed by

On-site and inter-site Hubbard corrections in magnetic monolayers: The case of FePS₃ and CrI₃

Fatemeh Haddadi1,2*, Edward Linscott1*, Iurii Timrov1,2*, Nicola Marzari1,2*, Marco Gibertini3,4*

1 Theory and Simulation of Materials (THEOS), Ecole Polytechnique Federale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland

2 National Centre for Computational Design and Discovery of Novel Materials (MARVEL)

3 Dipartimento di Scienze Fisiche, Informatiche e Matematiche, University of Modena and Reggio Emilia, I-41125 Modena, Italy

4 Centro S3, CNR-Istituto Nanoscienze, I-41125 Modena, Italy

* Corresponding authors emails: fatemeh.haddadi@epfl.ch, edward.linscott@epfl.ch, iurii.timrov@epfl.ch, nicola.marzari@epfl.ch, marco.gibertini@unimore.it
DOI10.24435/materialscloud:ez-6k [version v1]

Publication date: Jan 30, 2024

How to cite this record

Fatemeh Haddadi, Edward Linscott, Iurii Timrov, Nicola Marzari, Marco Gibertini, On-site and inter-site Hubbard corrections in magnetic monolayers: The case of FePS₃ and CrI₃, Materials Cloud Archive 2024.18 (2024), https://doi.org/10.24435/materialscloud:ez-6k


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.

Materials Cloud sections using this data

No Explore or Discover sections associated with this archive record.


File name Size Description
459.6 MiB This repository contains input files, output files to reproduce the figures and the results of the manuscript
3.9 KiB Description of how the data are provided


Files and data are licensed under the terms of the following license: Creative Commons Attribution 4.0 International.
Metadata, except for email addresses, are licensed under the Creative Commons Attribution Share-Alike 4.0 International license.


DFT DFT+U DFT+U+V first principles Hubbard 2D materials 2D magnets cscs MARVEL/DD3 EPFL Quantum ESPRESSO

Version history:

2024.18 (version v1) [This version] Jan 30, 2024 DOI10.24435/materialscloud:ez-6k