Complex magnetic order in the Nd(Tb)Fe3(BO3)4 multiferroic revealed by single-crystal neutron diffraction

Magnetic structure of the substituted multiferroics-ferroborates ${\mathrm{Nd}}_0.9{\mathrm{Tb}}_0.1{\mathrm{Fe}}₃{({\mathrm{BO}}₃)}₄$ and ${\mathrm{Nd}}_0.8{\mathrm{Tb}}_0.2{\mathrm{Fe}}₃{({\mathrm{BO}}₃)}₄$ were determined in the framework of a self-consistent refinement of the single crystal neutron diffraction data. The small substitution of Nd for Tb leads to the reorientation of the main antiferromagnetic vector L from the basal plane towards the hexagonal axis. The reorientation takes place via an angular structure for which L does not coincide with the principal crystallographic directions and evolves with temperature due to competing magnetic anisotropies of Fe, Nd, and Tb subsystems. Our refinement at 2 K reveals the existence of distortions in the collinear antiferromagnetic Fe spin arrangement suggested before in other ferroborates. Therefore, besides the main antiferromagnetic vector L, the magnetic structure involves additional fine symmetrized combinations of spin components allowed by symmetry. They coexist with certain L components and could originate from the antisymmetric Dzyaloshinsky-Moriya Fe-Fe exchange interactions. At higher temperatures, the magnetic structure is described by the simple collinear model, where the L vector is deviated from the hexagonal plane.