Hund's physics and the magnetic ground state of CrOX (X = Cl, Br)

Abstract

To understand the magnetic property of layered van der Waals materials CrOX (X = Cl, Br), we performed the detailed first-principles calculations for both bulk and monolayer. We found that the charge-only density functional theory combined with the explicit on-site interaction terms (so-called cDFT$+U$) well reproduces the experimental magnetic ground state of bulk CrOX, which is not the case for the use of spin-dependent density functional (so-called sDFT$+U$). Unlike some of the previous studies, our results show that CrOX monolayers are antiferromagnetic as in the bulk. It is also consistent with our magnetic force linear response calculation of exchange couplings $J_{\mathrm{ex}}$. The result of orbital-decomposed $J_{\mathrm{ex}}$ calculations shows that the Cr $t_{\text{2g}}$-$t_{\text{2g}}$ component mainly contributes to the antiferromagnetic order in both bulk and monolayer. Our result and analysis show that taking the correct Hund's physics into account is of key importance to construct the magnetic phase diagram and to describe the electronic structure.

References in corpus (25)

• Layer-dependent Ferromagnetism in a van der Waals Crystal down to the Monolayer Limit
• Discovery of intrinsic ferromagnetism in 2D van der Waals crystals
• Gate-tunable Room-temperature Ferromagnetism in Two-dimensional Fe${}_3$GeTe${}_2$
• Electronic Structure Calculations with Dynamical Mean-Field Theory: A Spectral Density Functional Approach
• Two-dimensional materials from high-throughput computational exfoliation of experimentally known compounds
• Wannier90 as a community code: new features and applications
• Magnetic 2D materials and heterostructures
• Electrical Control of 2D Magnetism in Bilayer CrI3
• Giant Tunneling Magnetoresistance in Spin-Filter van der Waals Heterostructures
• Controlling magnetism in 2D CrI3 by electrostatic doping
• Probing magnetism in 2D van der Waals crystalline insulators via electron tunneling
• Electric-field switching of two-dimensional van der Waals magnets
• van der Waals forces in density functional theory: The vdW-DF method
• Frequency-dependent local interactions and low-energy effective models from electronic structure calculations
• Effective Coulomb interaction in transition metals from constrained random-phase approximation
• Room temperature 2D ferromagnetism in few-layered 1$T$-CrTe${}_2$
• Viewpoint: Opportunities and challenges of two-dimensional magnetic van der Waals materials: magnetic graphene?
• Microscopic understanding of magnetic interactions in bilayer CrI${}_3$
• A family of high-temperature ferromagnetic monolayers with locked spin-dichroism-mobility anisotropy: MnNX and CrCX (X=Cl, Br, I; C=S, Se, Te)
• Direct theoretical evidence for weaker correlations in electron-doped and Hg-based hole-doped cuprates
• The effect of double counting, spin density, and Hund interaction in the different DFT+$U$ functionals
• Super-Exchange Theory for Polyvalent Anion Magnets
• Reliability and applicability of magnetic force linear response theory: Numerical parameters, predictability, and orbital resolution
• Spin-density functional theories and their $+U$ and $+J$ extensions: a comparative study of transition metals and transition metal oxides
• Charge density functional plus $U$ theory of LaMnO${}_3$: Phase diagram, electronic structure, and magnetic interaction

Cited by in corpus (6)

• Multi-state data storage in a two-dimensional stripy antiferromagnet implemented by magnetoelectric effect
• Superexchange Interaction in Insulating EuZn${}_2$P${}_2$
• Lattice Distortions and Magnetic Interactions in Single-Layer VOCl
• Chemical vapor deposition growth of continuous monolayer antiferromagnetic CrOCl films
• Many-body electronic structure, self-doped double-exchange, and Hund metallicity in 1T-CrTe2 bulk and monolayer
• Two-Dimensional Magnetic Materials from Ferromagnetism to Altermagnetism: Fabrication, Symmetry, Evidence, and Device Readiness