Changes of the magnetic interactions in TlCo2Se2 upon metal substitution

Various solid solutions TlCo_2−xMe_xSe₂ (Me=Fe, Ni and Cu) have been investigated by neutron powder diffraction, supplemented by magnetometry. The incommensurate spin-helix running along the c-axis in tetragonal TlCo₂Se₂ prevails for low concentrations of copper and iron but changes pitch. In the copper case, only cobalt carries a magnetic moment. On nickel substitution, however, collinear antiferromagnetic coupling between the ferromagnetic layers occurs. The magnetic moment distribution between the two transition metals in the solid solution TlCo_2−xNi_xSe₂ was tentatively probed with first principle calculations on fictive ordered TlCoNiSe₂, modelled by two types of superstructures. Also the ternary mother compounds, Pauli paramagnetic TlNi₂Se₂ and antiferromagnetic TlCo₂Se₂, were investigated with the same LMTO method.