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 (105)

• 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
• Phonons and related properties of extended systems from density-functional perturbation theory
• Advanced capabilities for materials modelling with Quantum ESPRESSO
• Layer-dependent Ferromagnetism in a van der Waals Crystal down to the Monolayer Limit
• Discovery of intrinsic ferromagnetism in 2D van der Waals crystals
• A linear response approach to the calculation of the effective interaction parameters in the LDA+U method
• Gate-tunable Room-temperature Ferromagnetism in Two-dimensional Fe${}_3$GeTe${}_2$
• Maximally-localized Wannier functions for entangled energy bands
• Quantum ESPRESSO toward the exascale
• Two-dimensional materials from high-throughput computational exfoliation of experimentally known compounds
• Magnetic 2D materials and heterostructures
• Pseudopotentials for high-throughput DFT calculations
• Electrical Control of 2D Magnetism in Bilayer CrI3
• Giant Tunneling Magnetoresistance in Spin-Filter van der Waals Heterostructures
• Ising-Type Magnetic Ordering in Atomically Thin FePS3
• Probing magnetism in 2D van der Waals crystalline insulators via electron tunneling
• Precision and efficiency in solid-state pseudopotential calculations
• Electric-field switching of two-dimensional van der Waals magnets
• Frequency-dependent local interactions and low-energy effective models from electronic structure calculations
• Robust Intrinsic Ferromagnetism and Half Semiconductivity in Stable Two-Dimensional Single-Layer Chromium Trihalides
• On the origin of magnetic anisotropy in two dimensional CrI${}_3$
• Density functional theory in transition-metal chemistry: a self-consistent Hubbard U approach
• Very Large Tunneling Magnetoresistance in Layered Magnetic Semiconductor CrI${}_3$
• Van der Waals heterostructures for spintronics and opto-spintronics
• Direct observation of van der Waals stacking dependent interlayer magnetism
• 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
• Electronic and magnetic properties of single-layer MPX${}_3$ metal phosphorous trichalcogenides
• Hubbard parameters from density-functional perturbation theory
• Ligand-field helical luminescence in a 2D ferromagnetic insulator
• Néel-type skyrmion in WTe2/Fe3GeTe2 van der Waals heterostructure
• One million percent tunnel magnetoresistance in a magnetic van der Waals heterostructure
• Intrinsic 2D-XY ferromagnetism in a van der Waals monolayer
• Two dimensional magnets: Forgotten history and recent progress towards spintronic applications
• Toward a realistic description of multilayer black phosphorus: from $GW$ approximation to large-scale tight-binding simulations
• Self-consistent Hubbard parameters from density-functional perturbation theory in the ultrasoft and projector-augmented wave formulations
• Extended DFT+U+V method with on-site and inter-site electronic interactions
• Néel-type skyrmions and their current-induced motion in van der Waals ferromagnet-based heterostructures
• Spin-flop transition in atomically thin MnPS${}_3$ crystals
• Magnon transport in quasi-two-dimensional van der Waals antiferromagnets
• Spin direction controlled electronic band structure in two dimensional ferromagnetic CrI3
• Antiferromagnetic ordering in van der Waals two-dimensional magnetic material MnPS3 probed by Raman spectroscopy
• Direct observation of 2D magnons in atomically thin CrI${}_3$
• Physical origin of giant excitonic and magneto-optical responses in two-dimensional ferromagnetic insulators
• Magnetic Two-Dimensional Chromium Trihalides: A Theoretical Perspective
• Nonempirical Range-separated Hybrid Functionals for Solids and Molecules
• Extensive Benchmarking of DFT+U Calculations for Predicting Band Gaps
• Breakdown of optical phonons' splitting in two-dimensional materials
• First principles study of electronic and structural properties of CuO
• Tuning Inelastic Light Scattering via Symmetry Control in 2D Magnet CrI${}_3$
• Calculating critical temperatures for ferromagnetic order in two-dimensional materials
• Structural and electronic phase transitions in FePS${}_3$ under the application of pressure
• Non-uniform sampling schemes of the Brillouin zone for many-electron perturbation-theory calculations in reduced dimensionality
• High throughput computational screening for 2D ferromagnetic materials: the critical role of anisotropy and local correlations
• Band gaps of crystalline solids from Wannier-localization based optimal tuning of a screened range-separated hybrid functional
• Distinct spin-lattice and spin-phonon interactions in monolayer magnetic CrI${}_3$
• Phonon and Thermal Properties of Quasi-Two-Dimensional FePS3 and MnPS3 Antiferromagnetic Semiconductor Materials
• High throughput computational screening for two-dimensional magnetic materials based on experimental databases of three-dimensional compounds
• Orbitally-resolved ferromagnetism of monolayer CrI${}_3$
• Distinct magneto-Raman signatures of spin-flip phase transitions in CrI3
• 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${}_3$
• The role of spin in the calculation of Hubbard $U$ and Hund's $J$ parameters from first principles
• Magnon-polarons in van der Waals antiferromagnet FePS3
• General invariance and equilibrium conditions for lattice dynamics in 1D, 2D, and 3D materials
• Magneto-optical response of chromium trihalide monolayers: chemical trends
• Curie Temperature of Emerging Two-Dimensional Magnetic Structures
• Lattice dynamics and phase transition in CrI${}_3$ single crystals
• Koopmans-compliant spectral functionals for extended systems
• Raman Spectrum of CrI${}_3$: an ab-initio study
• Electron correlation effects on exchange interactions and spin excitations in 2D van der Waals materials
• Ab initio electron-phonon interactions in correlated electron systems
• Assessing model-dielectric-dependent hybrid functionals on the antiferromagnetic transition-metal monoxides MnO, FeO, CoO, and NiO
• Accurate electronic properties and intercalation voltages of olivine-type Li-ion cathode materials from extended Hubbard functionals
• Pulay forces in density-functional theory with extended Hubbard functionals: From nonorthogonalized to orthogonalized manifolds
• Electric fields with ultrasoft pseudo-potentials: applications to benzene and anthracene
• Magnetic exchange interactions in monolayer CrI${}_3$ from many-body wavefunction calculations
• A Combined First Principles Study of the Structural, Magnetic, and Phonon Properties of Monolayer CrI${}_3$
• Inducing Magnetic Phase Transitions in Monolayer CrI${}_3$ via Lattice Deformations
• Excitons in Bulk and Layered Chromium Tri-Halides: From Frenkel to the Wannier-Mott Limit
• Frequency splitting of chiral phonons from broken time reversal symmetry in CrI${}_3$
• Observation of giant surface second harmonic generation coupled to nematic orders in the van der Waals antiferromagnet FePS${}_3$
• Electronic Structure of Chromium Trihalides beyond Density Functional Theory
• Electronic structure of pristine and Ni-substituted LaFeO${}_3$ from near edge x-ray absorption fine structure experiments and first-principles simulations
• 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)
• Role of non-locality in exchange-correlation for magnetic 2D van der Waals materials
• Importance of intersite Hubbard interactions in $\beta$-MnO${}_2$: A first-principles DFT+$U$+$V$ study
• Valence band electronic structure of the van der Waals ferromagnetic insulators: VI${}_3$ and CrI${}_3$
• koopmans: an open-source package for accurately and efficiently predicting spectral properties with Koopmans functionals
• Spin dynamics from time-dependent density functional perturbation theory
• Pivotal Role of Intersite Hubbard Interactions in Fe-doped $\alpha$-MnO${}_2$
• Dynamical correlations in single-layer CrI${}_3$
• Unraveling the effects of inter-site Hubbard interactions in spinel Li-ion cathode materials
• Prediction of topological phases in metastable ferromagnetic MPX${}_3$ monolayers
• Electronic correlation, magnetic structure and magnetotransport in few-layer CrI3
• 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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• Charge doping into spin minority states mediates doubling of $T_{\mathrm{C}}$ in ferromagnetic CrGeTe${}_3$
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