Realization of Intrinsic Colossal Magnetoresistance in Pb(Pb<sub>1/3</sub>Hg<sub>2/3</sub>)<sub>3</sub>Mn<sub>4</sub>O<sub>12</sub>: An A Site-Ordered Quadruple Perovskite Oxide
Colossal magnetoresistance (CMR) effects have been extensively studied in ABO<sub>3</sub> perovskite manganites where the Mn<sup>3+</sup>-O-Mn<sup>4+</sup> double-exchange mechanism plays a pivotal role. However, A-site-ordered AA'<sub>3</sub>B<sub>4</sub>O<sub>12</sub>-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(Pb<sub>1/3</sub>Hg<sub>2/3</sub>)<sub>3</sub>Mn<sub>4</sub>O<sub>12</sub> (PPHMO) characterized by an unusually increased Mn-O-Mn bond angle of up to 153°. This compound crystallizes into a cubic <i>Im</i>3̅ structure with the charge distribution Pb<sup>2+</sup>(Pb<sub>1/3</sub><sup>3.5+</sup>Hg<sub>2/3</sub><sup>2+</sup>)<sub>3</sub>Mn<sub>4</sub><sup>3.63+</sup>O<sub>12</sub>. A ferromagnetic phase transition is observed at the Curie temperature <i>T</i><sub>C</sub> ≈ 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 <i>T</i><sub>C</sub>. 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.
Authors
- Zhiwei Hu (ORCID: https://orcid.org/0000-0003-0324-2227)
- Youwen Long (ORCID: https://orcid.org/0000-0002-8587-7818)
- Xubin Ye (ORCID: https://orcid.org/0000-0002-5739-8318)
- Chien‐Te Chen (ORCID: https://orcid.org/0000-0002-1881-2600)
- Dong Cheng (ORCID: https://orcid.org/0000-0002-2891-8759)
- Xiaohui Yu (ORCID: https://orcid.org/0000-0001-8880-2304)
- Maocai Pi
- Jie Zhang (ORCID: https://orcid.org/0009-0006-9055-2969)
- Zhao Pan (ORCID: https://orcid.org/0000-0002-8693-2508)
- Yao Shen (ORCID: https://orcid.org/0000-0003-4697-4719)
- Xiao Wang (ORCID: https://orcid.org/0000-0001-8139-4192)
- Xi Shen (ORCID: https://orcid.org/0009-0006-0403-703X)
- Jin‐Ming Chen (ORCID: https://orcid.org/0000-0001-5727-8562)
- Richeng Yu
- Chang‐Yang Kuo
- Shuai Tang (ORCID: https://orcid.org/0000-0003-2822-5060)
Institutions
- National Yang Ming Chiao Tung University (TW)
- Chinese Academy of Sciences (CN)
- National Synchrotron Radiation Research Center (TW)
- Max Planck Institute for Chemical Physics of Solids (DE)
- Songshan Lake Materials Laboratory (CN)
- FZU ‒ Institute of Physics of the Academy of Sciences of the Czech Republic (CZ)
- Institute of Physics (CN)
- National Laboratory for Superconductivity (CN)
- University of Chinese Academy of Sciences (CN)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2025-03-08
- DOI
- https://doi.org/10.1021/jacs.5c00186
- Citations
- 6
- Primary Topic
- Magnetic and transport properties of perovskites and related materials
- Type
- article
- Field-Weighted Citation Impact
- 2.56
Funders
- National Natural Science Foundation of China
- China Postdoctoral Science Foundation
- National Key Research and Development Program of China