Abstract: We report the synthesis of double perovskites La2Ni4/3−xCoxSb2/3O6 with x=0, 1/3, 2/3 and 1 by a solid state method. Rietveld refinements of X-ray and neutron powder diffraction data show that all samples crystallize in space group P21/n, with almost perfect occupation of the 2d octahedral site with the transition metals, while all Sb5+ are randomly distributed in a 2c octahedral site. The saturation magnetization in hysteresis loops indicates that the samples are ferrimagnetic throughout all the series. Virgin magnetization curves lie outside hysteresis loops at low temperatures and thermal evolution of Hm – defined as the inflection point of these curves – follows the de Almeida–Thouless dependence for x ≠ 0 . This spin glass like behavior below 30 K is also supported by thermal evolution of the coercivity, which follows an exponential law typical of magnetic clusters, not found in the pure Ni2+ perovskite, x=0 extreme.

Abstract: New double perovskites LaPbMSbO₆, where M²⁺ = Mn²⁺, Co²⁺, and Ni²⁺, were synthesized as polycrystals by an aqueous synthetic route at temperatures below 1000 ^°C. All samples are monoclinic, space group P2₁/n, as it is observed from Rietveld analysis of X-ray powder diffraction patterns. The distribution of M²⁺ and Sb⁵⁺ among the two octahedral sites have 3% of disorder for M²⁺ = Ni²⁺, whereas for M²⁺ = Mn²⁺ and Co²⁺ less disorder is found. The three samples have an antiferromagnetic transition, due to the antiferromagnetic coupling between M^{2 +} through super-superexchange paths M²⁺-O^2--Sb⁵⁺-O^2--M²⁺. Transition temperatures are low: 8, 10 and 17 K for Mn²⁺, Co²⁺, and Ni^{2 +} respectively, as a consequence of the relatively long distances between the magnetic ions M²⁺. Besides, for LaPbMnSbO₆ a small transition at 45 K was found, with ferrimagnetic characteristics, possibly as a consequence of a small disorder between Mn²⁺ and Sb⁵⁺. This disorder would give additional and shorter interaction paths: superexchange Mn²⁺-O^2--Mn²⁺.