Magnetic exchange interactions in monolayer CrI${}_3$ from many-body wavefunction calculations

Abstract

The marked interplay between the crystalline, electronic, and magnetic structure of atomically thin magnets has been regarded as the key feature for designing next-generation magneto-optoelectronic devices. In this respect, a detailed understanding of the microscopic interactions underlying the magnetic responses of these crystals is of primary importance. Here, we combine model Hamiltonians with multi-reference configuration interaction wavefunctions to accurately determine the strength of the spin couplings in the prototypical single-layer magnet CrI${}_3$. Our calculations identify the (ferromagnetic) Heisenberg exchange interaction $J=-1.44$ meV as the dominant term, being the inter-site magnetic anisotropies substantially {weaker}. We also find that single-layer CrI${}_3$ features an out-of-plane easy axis ensuing from a single-ion anisotropy $A=-0.10$ meV, and predict $g$-tensor in-plane components $g_{xx}=g_{yy}=1.90$ and out-of-plane component $g_{zz}=1.92$. In addition, we assess the performance of a dozen widely used density functionals against our accurate correlated wavefunctions {calculations} and available experimental data, thereby establishing reference results for future first-principles investigations. Overall, our findings offer a firm theoretical ground to experimental observations.

References in corpus (38)

• Electric Field Effect in Atomically Thin Carbon Films
• The electronic properties of graphene
• Atomically thin MoS2: A new direct-gap semiconductor
• Restoring the density-gradient expansion for exchange in solids and surfaces
• Generalized gradient approximation for solids and their surfaces
• Two Dimensional Atomic Crystals
• Van der Waals heterostructures
• Magic-angle graphene superlattices: a new platform for unconventional superconductivity
• 2D materials and van der Waals heterostructures
• Layer-dependent Ferromagnetism in a van der Waals Crystal down to the Monolayer Limit
• Correlated Insulator Behaviour at Half-Filling in Magic Angle Graphene Superlattices
• Quantum Spin Hall Effect and Topological Field Effect Transistor in Two-Dimensional Transition Metal Dichalcogenides
• Two-dimensional materials from high-throughput computational exfoliation of experimentally known compounds
• Epitaxial Growth of Two-Dimensional Stanene
• Magnetic 2D materials and heterostructures
• Magnetism in Graphene Induced by Single-Atom Defects
• 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
• Spin-half paramagnetism in graphene induced by point defects
• Realization of Quantum Spin Hall State in Monolayer 1T'-WTe2
• On the origin of magnetic anisotropy in two dimensional CrI${}_3$
• Very Large Tunneling Magnetoresistance in Layered Magnetic Semiconductor CrI${}_3$
• Switching 2D Magnetic States via Pressure Tuning of Layer Stacking
• Pressure-controlled interlayer magnetism in atomically thin CrI3
• Atomically Thin Boron Nitride: Unique Properties and Applications
• CDW, Superconductivity and Anomalous Metallic Behavior in 2D Transition Metal Dichalcogenides
• Probing magnetism in 2D materials at the nanoscale with single spin microscopy
• Interplay between Kitaev interaction and single ion anisotropy in ferromagnetic CrI${}_3$ and CrGeTe${}_3$ monolayers
• Spin-orbit excitation energies, anisotropic exchange, and magnetic phases of honeycomb RuCl3
• Kitaev interactions between j=1/2 moments in honeycomb Na2IrO3 are large and ferromagnetic: insights from ab initio quantum chemistry calculations
• Calculating critical temperatures for ferromagnetic order in two-dimensional materials
• High throughput computational screening for 2D ferromagnetic materials: the critical role of anisotropy and local correlations
• Highly-Oriented Atomically Thin Ambipolar MoSe${}_2$ Grown by Molecular Beam Epitaxy
• Magnetic state of pyrochlore Cd2Os2O7 emerging from strong competition of ligand distortions and longer-range crystalline anisotropy
• Point defects in the 1$T^{\prime }$ and 2$H$ phases of single-layer MoS${}_2$: A comparative first-principles study
• Strong effect of hydrogen order on magnetic Kitaev interactions in H${}_3$LiIr${}_2$O${}_6$

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• Magnetic Anisotropy in Spin-3/2 with Heavy Ligand in Honeycomb Mott Insulators: Application to CrI${}_3$
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• Unified Treatment of Magnons and Excitons in Monolayer CrI${}_3$ from Many-Body Perturbation Theory
• Magnetoelectric Response of Antiferromagnetic Van der Waals Bilayers
• Theory of magnetism in the van der Waals magnet CrI3
• Systematic DFT+U and Quantum Monte Carlo benchmark of magnetic two-dimensional (2D) CrX${}_3$ (X = I, Br, Cl, F)
• Magnon-phonon interactions enhance the gap at the Dirac point in the spin-wave spectra of CrI${}_3$ two-dimensional magnets
• Exotic Magnetic and Electronic Properties of Layered CrI3 Single Crystals Under High Pressure
• Control of magnetic states and spin interactions in bilayer CrCl${}_3$ with strain and electric fields: an ab initio study
• On-site and inter-site Hubbard corrections in magnetic monolayers: The case of FePS${}_3$ and CrI${}_3$
• Altermagnetism in Two Dimensional Ca${}_2$RuO${}_4$ Perovskite
• Monolayer C${}_{60}$ networks: A first-principles perspective
• First-principles study of the gap in the spin excitation spectrum of the CrI${}_3$ honeycomb ferromagnet
• Beyond the random phase approximation for calculating Curie temperatures in ferromagnets: application to Fe, Ni, Co and monolayer CrI3
• Electronic excitations and spin interactions in chromium trihalides from embedded many-body wavefunctions
• DMRG and Monte Carlo studies of ${\text{CrI}}_3$ magnetic phases and the phase transition