Abstract
The synthesis of La1+xBa2−xMn2O6 (0.2 ≤ x ≤ 0.4) under reducing conditions is reported. Neutron powder diffraction studies indicate an A-site ordered, oxygen deficient bilayer Ruddlesden–Popper structure. La3+ ions preferentially occupy oxygen vacant layers within the perovskite bilayers, leading to a structure analogous to the cuprate superconductor La1.85Ba0.15CaCu2O6+γ, with “MnO2” layers constructed from corner-linked square pyramidal MnO5 units. Magnetic measurements suggest that no long range magnetic order exists in this mixed Mn2+/Mn3+ system. Significantly, the low temperature oxidation of this phase leads to the synthesis of La1+xBa2−xMn2O6.95, which constitutes the first isolation of a complete barium analogue of La1+xSr2−xMn2O7, the important low field colossal magnetoresistive material. Neutron diffraction data confirm the retention of A-site order and a change in Jahn–Teller distortion. Low temperature neutron data and magnetic susceptibility suggest canted A-type antiferromagnetic order.
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