Double MITs and magnetoresistance: an intrinsic feature of Ru substituted La0.67Ca0.33MnO3

In this paper, we examine the possible influence of extrinsic factors on the electrical and magnetotransport of La0.67Ca0.33Mn1-xRuxO3 (x≤0.10). Ru substitution results in double metal-insulator transitions (MITs) at TMI1 and TMI2, both exhibiting magnetoresistance (MR). No additional magnetic signal corresponding to a second low-temperature maximum (LTM) at TMI2 could be observed, either in ac susceptibility (χ') or in specific heat (Cp). Typical grain sizes of ∼18 000-20 000 nm, as estimated from the scanning electron microscope (SEM) micrographs, are not so small as to warrant an LTM. The absence of additional peaks in the high statistics powder x-ray diffraction (XRD), a linear systematic increase of the unit cell parameters, close matching of the transition temperatures in resistivity, χ' and Cp and their linear systematic decrease with x, and an homogeneous distribution of Mn, Ru and O at arbitrarily selected regions within and across the grains exclude chemical inhomogeneity in the samples. The insensitivity of grain boundary MR at 5 K to Ru composition indicates that the grain boundary is not altered to result in an LTM. Oxygen stoichiometry of all the compounds is close to the nominal value of 3. These results not only exclude the extrinsic factors, but also establish that double MITs, both exhibiting MR, are intrinsic to Ru substituted La0.67Ca0.33MnO3