Magnetic order in double-layer manganites (La(1-z)Pr(z))1.2Sr1.8Mn2O7: intrinsic properties and role of the intergrowths

We report on an investigation of the double-layer manganite series (La(1-z)Pr(z))1.2Sr1.8Mn2O7 (0 <= z <= 1), carried out on single crystals by means of both macroscopic magnetometry and local probes of magnetism (muSR, 55Mn NMR). Muons and NMR demonstrate an antiferromagnetically ordered ground state at non-ferromagnetic compositions (z >= 0.6), while more moderate Pr substitutions (0.2 <= z <= 0.4) induce a spin reorientation transition within the ferromagnetic phase. A large magnetic susceptibility is detected at {Tc,TN} < T < 250K at all compositions. From 55Mn NMR spectroscopy, such a response is unambiguously assigned to the intergrowth of a ferromagnetic pseudocubic phase (La(1-z)Pr(z))(1-x)Sr(x)MnO3, with an overall volume fraction estimated as 0.5-0.7% from magnetometry. Evidence is provided for the coupling of the magnetic moments of these inclusions with the magnetic moments of the surrounding (La(1-z)Pr(z))1.2Sr1.8Mn2O7 phase, as in the case of finely dispersed impurities. We argue that the ubiquitous intergrowth phase may play a role in the marked first-order character of the magnetic transition and the metamagnetic properties above Tc reported for double-layer manganites.