Magnetic phase diagram of Ca-substituted EuFe2As2

The simultaneous presence of a Fe-related spin-density wave and antiferromagnetic order of Eu$^{2+}$ moments ranks EuFe$_2$As$_2$ among the most interesting parent compounds of iron-based pnictide superconductors. Here we explore the consequences of the dilution of Eu$^{2+}$ magnetic lattice through on-site Ca substitution. By employing macro- and microscopic techniques, including electrical transport and magnetometry, as well as muon-spin spectroscopy, we study the evolution of Eu magnetic order in both the weak and strong dilution regimes, achieved for Ca concentration $x(\mathrm{Ca}) = 0.12$ and 0.43, respectively. We demonstrate the localized (mostly RKKY) character of the Eu antiferromagnetism, in contrast with the largely itinerant nature of Fe magnetic interactions. Our results suggest a weak coupling between the Fe and Eu magnetic sublattices and a rapid decrease of the Eu magnetic interaction strength upon Ca substitution. The latter is confirmed both by the depression of the ordering temperature of the Eu$^{2+}$ moments, $T_\mathrm{N}$, and the decrease of magnetic volume fraction with increasing $x(\mathrm{Ca})$. We establish that, similarly to the EuFe$_2$As$_2$ parent compound, the investigated Ca-doped compounds have a twinned structure and undergo a permanent detwinning upon appllying an external magnetic field.