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Polycrystalline Sr2Fe1−xAlxMoO6 compounds with x=0, 0.05, 0.10, 0.15, and 0.30 were fabricated and their low-field magnetoresistance (LFMR) performance studied. The LFMR was greatly enhanced as x increased from nil to 0.15, and its origin was found to be intragranular spin-dependent scattering. The replacement of Fe by Al weakened the antiferromagnetic exchange in the antiphase boundary arising from the antisite defect and acted as a barrier for electron transport along the Mo–O–Fe–O–Mo–O–Fe chain in the ferromagnetic segregation and weakened the ferromagnetic exchange. When the external magnetic field was applied, the spin in the antiphase boundary appeared to align more easily to the external field after Al doping and the transport of the electron was easier due to the weakening of the double exchange barrier.

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