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Ordering of cations in different structural types occurs when there is a significant difference in the oxidation states and ionic radii of the ions involved. Herein we report an unusual ordering of isovalent cations Fe3+ and Al3+ in the polar rhombohedral R3 double perovskite structure of Bi2FeAlO6 synthesized at high‐pressure (6 GPa) and high‐temperature (1000 °C). This ordered structure is derived...
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