Orbital and magnetic ordering in single-layer FePS3: A DFT+U study

Abstract

Among the numerous 2D system that can be prepared via exfoliation, iron phosphorus trisulfide (FePS3) attracts a lot of attention recently due to its broad-range photoresponse, its unusual Ising-type magnetic order and possible applications in spintronic nano-devices. Despite various experimental and theoretical-computational reports, there are still uncertainties in identifying its magnetic ground state. In this paper, we investigate the structural and magnetic properties of single-layer FePS3 by using Density Functional Theory. Our findings show that orbital ordering leads to a variation in distance between pairs of iron atoms by 0.14 Angstrom. These lattice distortions, albeit small, trigger different (ferromagnetic and antiferromagnetic) exchange couplings so that the ground state consists of ferromagnetically aligned zigzag chains along the long Fe-Fe bonds which couple antiferromagnetically along the shorter Fe-Fe bonds. Within the DFT+U framework, we parameterize a spin Hamiltonian including Heisenberg, single-ion anisotropy, Dzyaloshinskii-Moriya and biquadratic interactions. Using U=2.22eV gives a consistent description of both the electronic band gap and the Neel temperature in 2D FePS3.

10 pages, 8 figures

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• Theory of orbital magnetoelectric response
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• Spin-lattice couplings in two-dimensional CrI${}_3$ from first-principles study
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Cited by in corpus (10)

• Magnetic Anisotropy in Two-dimensional van der Waals Magnetic Materials and Their Heterostructures: Importance, Mechanisms, and Opportunities
• Giant spin Nernst effect in a two-dimensional antiferromagnet due to magnetoelastic coupling-induced gaps and interband transitions between magnon-like bands
• Molecular intercalation in the van der Waals antiferromagnets FePS3 and NiPS3
• On-site and inter-site Hubbard corrections in magnetic monolayers: The case of FePS${}_3$ and CrI${}_3$
• Identifying band structure changes of FePS3 across the antiferromagnetic phase transition
• Understanding the Ising zigzag antiferromagnetism of FePS3 and FePSe3 monolayers
• Effect of biquadratic magnetic exchange interaction in the 2D antiferromagnets MPS_3 (M = Mn, Fe, Co, Ni)
• Orbital magnetization in two-dimensional materials from high-throughput computational screening
• Magnetodielectric Properties in Two Dimensional Magnetic Insulators
• Giant orbital magnetization in two-dimensional materials