LAUSR

Abstract The magnetic structures and magnetic phase transitions in intermetallic layered La 1 - x Tb x Mn 2 Si 2 compounds (the ThCr2Si2-type structure) are investigated using the first-principles method and XPS measurements. The experimentally observed transition from ferromagnetic (FM) to antiferromagnetic (AFM) ordering of Mn sublattice with increase of terbium concentration is successfully reproduced in calculations for collinear magnetic moments model. The FM → AFM change of interplane magnetic ordering at small x is irrelevant to the number of f-electrons of the rare-earth ion. In contrast it was shown to be related to the Mn-Mn in-plane distance. Calculated Tb critical concentration for this transition x ≈ 0.14 corresponds to the Mn-Mn in-plane distance 0.289 nm, very close to the experimentally observed transition distance 0.287 nm. The crystal cell compression due to substitution increases an overlap between Mn d xz , yz and the rare-earth ion d orbitals. Resulting hybridized states manifest themselves as an additional peak in the density of states. We suggest that a corresponding interlayer Mn-R-Mn superexchange interaction stabilizes AFM magnetic ordering in these compounds with Tb doping level x > 0.2 . The results of DFT calculations are in agreement with X-ray photoemission spectra for La 1 - x Tb x Mn 2 Si 2 .