Single crystals of intermetallic phases RCrxGa3−yGey (R = Tb, Dy; x = 0.19–0.23, y = 0–0.4) and R4Cr1−xGa12−yGey (R = Tb, Dy; x = 0–0.13, y = 3–4) were grown from Ga flux ensuring the absence of magnetic impurities. The X-ray diffraction experiments revealed that the compounds belong to the family of filled AuCu3-type gallides. The compounds are formed upon the insertion of Cr atoms into E6 octahedral voids (E = Ga/Ge), which can occur in either disordered (RCrxGa3-yGey) or ordered (R4Cr1-xGa12-yGey) fashion. The unique feature of the obtained compounds is the strong correlation between the level of Ge doping and the Cr concentration in the phases, which allows one to control both the structural and magnetic ordering. At low Ge concentration, the cubic RCrxGa3-yGey phases form, which then experience tetragonal distortion upon the increase in the Ge content, and the cubic R4Cr1-xGa12-yGey 2×2×2 superstructures are formed at even higher Ge concentrations. The X-ray diffraction analysis also showed a presence of structural defects in the phases, which are caused by different size of empty E6 and filled CrE6 octahedra. Magnetic measurements of the single crystals of the cubic phases reveal antiferromagnetic ordering of the rare earth sublattice with the Neel temperatures decreasing upon Ge doping from 22 K for RCrxGa3 to 10 K for R4Cr1−xGa12−yGey. The Ge doping causes gradual decrease in the strength of antiferromagnetic R-R interactions ultimately leading to noncollinear magnetic structure in the superstructure R4Cr1−xGa12−yGey phases.
Read full abstract