In this work we studied, by means of high-resolution neutron diffraction as a function of temperature, the La 1.4 Sr 0.8 Ca 0.8 Mn 2 O 7 bilayered manganite for two different annealing treatments. Out data allowed us to shown, for the first time, the absence of long-range magnetic order in this optimally doped bilayered manganite where the A-site of the structure is doped with equal proportions of different isovalent cations (Ca and Sr). The system, however, presents defined IM transitions which suggest 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.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.
IntroductionThere is an increasing interest in materials that show magnetoresistance, because of their use in magnetic information storage or as magnetic field sensors [1]. Most of the available theoretical and experimental work has, until now, been focused on the 3D perovskite structures, that is the n=∞ endmember of the A n+1 B n O 3n+1 Ruddlesden-Popper family, in which n 2D layers of BO 6 corner-sharing octahedra are joined along the stacking direction and separated by rock-salt AO layers.The optimally-doped n=2 members of this family (La 2-2x B 1+2x Mn 2 O 7 where B = Ca or Sr) behave analogously to the n=∞ manganites in the sense that they undergo an insulating-to metallic-like state (I-M) transition coupled to a ferromagnetic transition at temperatures around 120-140 K; besides, they present a large magnetoresistance in this temperature range [2]. However, the change in dimensionality and resulting pronounced cation dependence of the electronic properties can produce physical properties which contrast strongly with the perovskite systems [3][4][5][6].In the n=2 member La 2-2x Sr 1+2x Mn 2 O 7 an extremely rich variety of magnetic phases have been found as a function of the Sr-doping. One of the most interesting regions extends from x=0.3 to x=0.4 where ferromagnetic metals (FMM) are found. However, also within a so relatively narrow doping range several different kinds of arrangements of manganese ions spin occur. A common property is the presence of a 2D ferromagnetic ordering in each perovskite layer and between the MnO 2 layers even though with different spin directions as a function of x. At x=0.3, the magnetic moments of each MnO 2 layer couple ferromagnetically within a bilayer and antiferromagnetically, along the c-axis, between successive bilayers. At x≈0.32 the inter-bilayer coupling becomes FM but still directed along the c-axis.At x≥0.33 the magnetic moments direct along the ab-plane. The magnetic coupling between the constituents single MnO 2 layers changes from FM into canted-antiferromagnetic (AFM) beyond x~0.4 [7]. Also the magnetic coupling above the transition temperature (T C ) is rather interesting. As suggested by several gro...