We investigate the electronic and magnetic structures of two-dimensional transition metal trichalcogenide CrSiTe 3 and CrGeTe 3 materials by carrying out first-principles calculations. The single-layer CrSiTe 3 and CrGeTe 3 are found to be a ferromagnetic insulator, where the presence of the strong d pσ -hybridization of Cr e g -Te p plays a crucial role for the ferromagnetic coupling between Cr ions. We observe that the bandgaps and the interlayer magnetic order vary notably depending on the magnitude of on-site Coulomb interaction U for Cr d electrons. The bandgaps are formed between the Cr e g conduction bands and the Te p valence bands for both CrSiTe 3 and CrGeTe 3 in the majority-spin channel. The dominant Te p antibonding character in the valence bands just below the Fermi level is related to the decrease of the bandgap for the increase of U. We elucidate the energy band diagram, which may serve to understand the electronic and magnetic properties of the ABX 3 -type transition metal trichalcogenides in general.

In order to investigate the electronic properties of the semiconducting van der Waals ferromagnet Cr 2 Ge 2 Te 6 (CGT), where ferromagnetic layers are bonded through van der Waals forces, we have performed angle-resolved photoemission spectroscopy (ARPES) measurements and density-functional-theory (DFT+U) calculations. The valence-band maximum at the Γ point is located ~ 0.2 eV below the Fermi level, consistent with the semiconducting property of CGT. Comparison of the experimental density of states with the DFT calculation has suggested that Coulomb interaction between the Cr 3d electrons U eff ~ 1.1 eV. The DFT+U calculation indicates that magnetic coupling between Cr atoms within the layer is ferromagnetic if Coulomb U eff is smaller than 3.0 eV and that the inter-layer coupling is ferromagnetic below U eff ~ 1.0 eV. We therefore conclude that, for U eff deduced by the experiment, the intra-layer Cr-Cr coupling is ferromagnetic and the inter-layer coupling is near the boundary between ferromagnetic and antiferromagnetic, which means experimentally deduced U eff is consistent with theoretical ferromagnetic condition.

Based on first-principles density-functional theory (DFT) calculations, we report that the transition-metal bis-dithiolene, M3C12S12 (M = Mn and Fe), complexes can be a two-dimensional (2D) ferromagnetic insulator with nontrivial Chern number. Among various synthetic pathways leading to metal bis-dithiolenes, the simplest choice of ligand, Benzene-hexathiol, connecting metal cations to form a Kagome lattice is studied following the experimental report of time-reversal symmetric isostructural compound Ni3C12S12. We show sulfur and carbon-based ligands play the key role in making the complexes topologically nontrivial. An unusual topological quantum phase transition induced by the on-site Coulomb interaction brings a nearly flat band with a nonzero Chern number as the highest occupied band. With this analysis we explain the electronic structure of the class M3C12S12 and predict the existence of nearly flat band with nonzero Chern number and it can be a fractional Chern insulator candidate with carrier doping.

Kagome metal-organic frameworks (MOFs) are considered a new class of materials that can host two-dimensional (2D) magnetism and correlated electron phenomena such as superconductivity and quantum anomalous Hall effect. Despite...

We report Chern insulating phases emerging from a single layer of layered chalcogenide CrSiTe3, a transition metal trichacogenides (TMTC) material, in the presence of charge doping. Due to strong hybridization with Te p orbitals, the spin-orbit coupling effect opens a finite band gap, leading to a nontrivial topology of the Cr eg conduction band manifold with higher Chern numbers. Our calculations show that quantum anomalous Hall effects can be realized by adding one electron in a formula unit cell of Cr2Si2Te6, equivalent to electron doping by 2.36 × 1014 cm−2 carrier density. Furthermore, the doping-induced anomalous Hall conductivity can be controlled by an external magnetic field via spin-orientation-dependent tuning of the spin-orbit coupling. In addition, we find distinct quantum anomalous Hall phases employing tight-binding model analysis, suggesting that CrSiTe3 can be a fascinating platform to realize Chern insulating systems with higher Chern numbers.