Absence of Long-Range Magnetic Order in the La_1.4Sr_0.8Ca_0.8Mn₂O₇ Bilayered Manganite

This paper presents the results of a high-resolution neutron diffraction and magnetometry investigation on the optimally doped (x = 0.3) La_1.4Sr_0.8Ca_0.8Mn₂O₇ bilayered manganite. In particular, two samples with different oxygen contents have been studied to put in prominence the role of the Mn average valence states at fixed cation concentration. The results show, for the first time, the absence of long-range magnetic order in this optimally doped manganite when the A-site of the structure is doped with equal proportions of isovalent Ca and Sr. This holds for both samples, which present different lattice effects with T, thus suggesting the primary role of cation disorder as the source of the lack of long-range order. The presence, for both samples, of defined insulating- to metallic-like transitions suggests that the transport properties are not linked to the evolution of long-range order and that two-dimensional spin ordering in the layers of the perovskite blocks may be sufficient to “assist” the hole hopping. A possible reason for the suppression of magnetic order induced by the Ca doping is a size effect coupled to the cation size mismatch between the Sr and Ca ions.