Abstract

The transport and magnetic properties of layered manganites, ${\mathrm{La}}_{2\ensuremath{-}2x}{\mathrm{Sr}}_{1+2x}{\mathrm{Mn}}_{2}{\mathrm{O}}_{7}$ $(x=0.35$ and 0.40), synthesized by solid-state reactions at various temperatures are reported. In contrast to the compounds with other doping levels, these compounds show metal-nonmetal transitions at 70--90 K in addition to the double-exchange-driven transitions at about 120 K. The lower-temperature transition is most pronounced when the synthesis temperature is low and gradually decreases in magnitude as the reaction temperature is increased. Temperature-dependent magnetic data show that there is no magnetic change corresponding to the transition at the lower temperatures, whereas the higher-temperature transition accompanies a ferromagnetic ordering, consistent with the double-exchange mechanism. Low-temperature (10 K) neutron diffraction data of selected samples show that these compounds order ferromagnetically with co-linear Mn spins that have tilting angles of about 70\ifmmode^\circ\else\textdegree\fi{} against the c axis in all samples, intermediate between the $x=0.30$ and 0.40 compounds in the literature, and that the different synthesis temperatures do not influence the magnetic structures of these compounds to a significant level. A mechanism that involves the spin orientation in the ferromagnetic state and the grain boundary effect is proposed to explain why the low-temperature transitions are observed only from samples with limited doping range and low synthesis temperatures.

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