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A series of bimagnetic heterostructured nanocrystals having an antiferromagnetic NiO core and a ferrimagnetic MnxNi1-xO and/or FiM Mn3O4 island nanophase overgrowth has been synthesized under varying aqueous solution pH conditions. The two-step self-assembly process employs a thermal decomposition method to synthesize NiO nanoparticles, followed by growth of the MnxNi1-xO and/or Mn3O4 nanophase over the NiO core using hydrothermal synthesis at pH values ranging from 2.4-7.0. The environmentally benign hydrothermal process involves pH c
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