Colossal magnetoresistance (CMR) effects have been extensively studied in ABO perovskite manganites where the Mn-O-Mn double-exchange mechanism plays a pivotal role. However, A-site-ordered AA'BO-type quadruple perovskite oxides exhibit significantly suppressed double exchange due to their extremely small B-O-B bond angles (≈140°), hindering the realization of intrinsic CMR effects. Here, we report the design and synthesis of a novel quadruple perovskite oxide Pb(PbHg)MnO (PPHMO) characterized by an unusually increased Mn-O-Mn bond angle of up to 153°. This compound crystallizes into a cubic 3̅ structure with the charge distribution Pb(PbHg)MnO. A ferromagnetic phase transition is observed at the Curie temperature ≈ 120 K, accompanied by an insulator-to-metal transition. Furthermore, applying magnetic fields significantly reduces the resistivity, resulting in intrinsic CMR effects with an absolute MR value of 650% at 8 T, increasing to 2250% at 16 T near . The large intrinsic MR is thereby realized unprecedentedly in an A-site-ordered quadruple perovskite oxide. Related origins for the intrinsic CMR effects presented in the current PPHMO are discussed in detail.
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