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

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+$\text{U}$ and its extensions PBEsol+$\text{U}$+$\text{V}$ 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 $\text{U}$ and inter-site $\text{V}$) 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 $\text{U}$ 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.

References in corpus (45)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Restoring the density-gradient expansion for exchange in solids and surfaces
• Generalized gradient approximation for solids and their surfaces
• Advanced capabilities for materials modelling with Quantum ESPRESSO
• Quantum ESPRESSO toward the exascale
• Magnetic 2D materials and heterostructures
• Ising-Type Magnetic Ordering in Atomically Thin FePS3
• Density functional theory in transition-metal chemistry: a self-consistent Hubbard U approach
• Van der Waals heterostructures for spintronics and opto-spintronics
• Suppression of magnetic ordering in XXZ-type antiferromagnetic monolayer NiPS3
• Self-consistent hybrid functional for condensed systems
• The GW compendium: A practical guide to theoretical photoemission spectroscopy
• Two dimensional magnets: Forgotten history and recent progress towards spintronic applications
• Self-consistent Hubbard parameters from density-functional perturbation theory in the ultrasoft and projector-augmented wave formulations
• Magnon transport in quasi-two-dimensional van der Waals antiferromagnets
• Antiferromagnetic ordering in van der Waals two-dimensional magnetic material MnPS3 probed by Raman spectroscopy
• Physical origin of giant excitonic and magneto-optical responses in two-dimensional ferromagnetic insulators
• Magnetic Two-Dimensional Chromium Trihalides: A Theoretical Perspective
• Extensive Benchmarking of DFT+U Calculations for Predicting Band Gaps
• Tuning Inelastic Light Scattering via Symmetry Control in 2D Magnet CrI${}_3$
• Non-uniform sampling schemes of the Brillouin zone for many-electron perturbation-theory calculations in reduced dimensionality
• Chirality selective magnon-phonon hybridization and magnon-induced chiral phonons in a layered zigzag antiferromagnet
• Hubbard-corrected density functional perturbation theory with ultrasoft pseudopotentials
• Magnetic anisotropy and exchange interactions of two-dimensional FePS${}_3$, NiPS${}_3$ and MnPS${}_3$ from first principles calculations
• Microscopic origin of ferromagnetism in trihalides CrCl${}_3$ and CrI${}_3$
• Magnetic order induced polarization anomaly of Raman scattering in 2D magnet CrI${}_3$
• Magnon-polarons in van der Waals antiferromagnet FePS3
• General invariance and equilibrium conditions for lattice dynamics in 1D, 2D, and 3D materials
• Ab initio electron-phonon interactions in correlated electron systems
• Accurate electronic properties and intercalation voltages of olivine-type Li-ion cathode materials from extended Hubbard functionals
• A Combined First Principles Study of the Structural, Magnetic, and Phonon Properties of Monolayer CrI${}_3$
• Excitons in Bulk and Layered Chromium Tri-Halides: From Frenkel to the Wannier-Mott Limit
• Observation of giant surface second harmonic generation coupled to nematic orders in the van der Waals antiferromagnet FePS${}_3$
• Frequency splitting of chiral phonons from broken time reversal symmetry in CrI${}_3$
• Electronic Structure of Chromium Trihalides beyond Density Functional Theory
• Orbital and magnetic ordering in single-layer FePS3: A DFT+U study
• Optimizing accuracy and efficacy in data-driven materials discovery for the solar production of hydrogen
• Systematic DFT+U and Quantum Monte Carlo benchmark of magnetic two-dimensional (2D) CrX${}_3$ (X = I, Br, Cl, F)
• Importance of intersite Hubbard interactions in $\beta$-MnO${}_2$: A first-principles DFT+$U$+$V$ study
• koopmans: an open-source package for accurately and efficiently predicting spectral properties with Koopmans functionals
• Pivotal Role of Intersite Hubbard Interactions in Fe-doped $\alpha$-MnO${}_2$
• Unraveling the effects of inter-site Hubbard interactions in spinel Li-ion cathode materials
• Prediction of topological phases in metastable ferromagnetic MPX${}_3$ monolayers
• Rashba-induced spin texture and spin-layer-locking effects in the antiferromagnetic CrI3 bilayer
• Pressure-induced transitions in FePS${}_3$: Structural, magnetic and electronic properties

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