Realization of Intrinsic Colossal Magnetoresistance in Pb(Pb1/3Hg2/3)3Mn4O12: An A Site-Ordered Quadruple Perovskite
Jie Zhang1,2, Xubin Ye1, Xiao Wang1
1Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China.
Abstract:
Colossal magnetoresistance (CMR) effects have been extensively studied in ABO3 perovskite manganites where the Mn3+-O-Mn4+ double-exchange mechanism plays a pivotal role. However, A-site-ordered AA'3B4O12-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(Pb1/3Hg2/3)3Mn4O12 (PPHMO) characterized by an unusually increased Mn-O-Mn bond angle of up to 153°. This compound crystallizes into a cubic Im3̅ structure with the charge distribution Pb2+(Pb1/33.5+Hg2/32+)3Mn43.63+O12. A ferromagnetic phase transition is observed at the Curie temperature TC ≈ 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 TC. 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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