First-principles calculations of tetragonal FeX (X=S, Se, Te): Magnetism, hyperfine-interaction, and bonding

• Published in: Journal of magnetism and magnetic materials 2017-11, Vol.441 (C), p.769-775
• Main Authors: Koteski, V., Ivanovski, V.N., Umićević, A., Belošević-Čavor, J., Toprek, D., Mahnke, H.-E.
• Format: Article
• Language: English
• Subjects: Charge density; Charge transfer; Chemical bonds; Crystallography; Density functional theory; Ferromagnetism; Interaction parameters; Iron; Local density approximation; Magnetic properties; Magnetism; Mathematical analysis; Mössbauer effect; Optimization; Plane waves; Quadrupoles; Superconductors
• ISSN: 0304-8853; 1873-4766
• DOI: 10.1016/j.jmmm.2017.06.092

[Display omitted] •Ab initio calculations of the structure and magnetism in tetragonal Feit X (X=S, Se,Te).•The collinear AFM structure best reproduces the measured Mössbauer parameters.•The Fe magnetic moments, fields, and EFGs critically depend on the X atom position.•The bonds in this system are determined to be of closed-shell type. Magnetic ground states, local crystallographic environment of Fe, and hyperfine interaction parameters in tetragonal FeX (X=S, Se, Te) are investigated by means of density functional theory (DFT) calculations using augmented plane waves plus local orbitals (APW+lo) method. We use several different magnetic configurations to evaluate the magnetic and electronic properties of this system, as well as the hyperfine interaction parameters at Fe lattice site. The results obtained for the ground state collinear anti-ferromagnetic arrangement relatively well reproduce the quadrupole splitting and isomer shifts from the available Mössbauer measurements. The Bader’s atoms in molecule charge density analysis indicates bonding of closed-shell type and a sizable charge transfer from Fe to X. The system properties are sensitive to the structural optimization of the position of the chalcogen atom with respect to the iron plane.