Realization of Intrinsic Colossal Magnetoresistance in Pb(Pb1/3Hg2/3)3Mn4O12: An A Site-Ordered Quadruple Perovskite Oxide

IF 14.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of the American Chemical Society Pub Date : 2025-03-08 DOI:10.1021/jacs.5c00186

Jie Zhang, Xubin Ye, Xiao Wang, Zhao Pan, Maocai Pi, Shuai Tang, Cheng Dong, Chien-Te Chen, Jin-Ming Chen, Chang-Yang Kuo, Zhiwei Hu, Xi Shen, Xiaohui Yu, Yao Shen, Richeng Yu, Youwen Long

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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(Pb_1/3Hg_2/3)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⁺(Pb_1/3^3.5+Hg_2/3²⁺)₃Mn₄^3.63+O₁₂. A ferromagnetic phase transition is observed at the Curie temperature T_C ≈ 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 T_C. 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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A位有序四重钙钛矿氧化物Pb(Pb1/3Hg2/3)3Mn4O12的本禀巨磁阻的实现

巨磁电阻（CMR）效应在ABO3钙钛矿锰矿中得到了广泛的研究，其中Mn3+ -O-Mn4 +双交换机制起着关键作用。然而，a位有序的AA ' 3b4o12型四重钙钛矿氧化物由于其极小的B-O-B键角（≈140°）而表现出明显的抑制双交换，阻碍了本构CMR效应的实现。在这里，我们报道了一种新型的四重钙钛矿氧化物Pb(Pb1/3Hg2/3)3Mn4O12 （PPHMO）的设计和合成，其特征是异常增加的Mn-O-Mn键角高达153°。该化合物结晶成立方Im3′s结构，其电荷分布为Pb2+(Pb1/33.5+Hg2/32+)3Mn43.63+O12。在居里温度TC≈120k处观察到铁磁相变，并伴有绝缘体到金属的转变。此外，施加磁场可显著降低电阻率，产生本征CMR效应，在8 T时绝对MR值为650%，在TC附近16 T时增加到2250%。因此，在a位有序的四重钙钛矿氧化物中实现了前所未有的大内禀磁共振。详细讨论了当前PPHMO中出现的本征CMR效应的相关来源。

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来源期刊

Journal of the American Chemical Society 化学-化学综合

CiteScore

24.40

自引率

6.00%

发文量

2398

审稿时长

1.6 months

期刊介绍： The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.