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Charge Disproportionation and Complex Magnetism in a PbMnO3 Perovskite Synthesized under High Pressure
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-11-24 , DOI: 10.1021/acs.chemmater.0c02706
Xiang Li, Zhiwei Hu, Yujin Cho, Xinyu Li, Hao Sun, Longzheng Cong, Hong-Ji Lin, Sheng-Chieh Liao, Chien-Te Chen, Anna Efimenko, Christoph J. Sahle, Youwen Long, Changqing Jin, Michael C. Downer, John B. Goodenough, Jianshi Zhou

Because of the possible crossover of Pb and 3d transition-metal (TM) redox levels, a charge transfer between Pb and TM leads to a continuous evolution from Pb2+Ti4+O3 to Pb4+Ni2+O3 in the perovskite family of PbTMO3 as verified by several reports. However, very little information is known about PbMnO3 in the PbTMO3 series. The perovskite PbMnO3 is the most difficult one to synthesize, although its geometric tolerance factor is close to 1. Here, we report a careful study of PbMnO3 synthesized under 15 GPa by a structural refinement and high-precision X-ray absorption spectroscopy (XAS) as well as a variety of measurements of physical properties. We can rationalize the physical properties of PbMnO3 based on a local bonding model and the valence states of Pb and Mn from XAS. Moreover, the complete study of PbMnO3 allows us to construct a more consistent picture of the valence evolution and the charge disproportionation for the entire family of PbTMO3 perovskites.

中文翻译:

高压合成的PbMnO 3钙钛矿中的电荷歧化和复磁性

因为Pb和3d过渡金属(T的可能的交叉的中号)的氧化还原水平,铅和T之间的电荷转移中号导致一个连续的演化选自Pb 2+的Ti 4+ ø 3对Pb 4+的Ni 2+ ö 3 PbT M O 3的钙钛矿家族中的一些元素,已得到一些报道的证实。然而,关于PbT M O 3系列的PbMnO 3的信息知之甚少。钙钛矿型PbMnO 3是最难合成的,尽管其几何公差系数接近1。在这里,我们报道了对PbMnO的仔细研究。在15 GPa下通过结构改进和高精度X射线吸收光谱(XAS)以及各种物理性能测量合成了3种。我们可以基于局部键合模型以及XAS中Pb和Mn的价态来合理化PbMnO 3的物理性质。此外,对PbMnO 3的完整研究使我们能够为整个PbT M O 3钙钛矿家族的化合价演化和电荷歧化建立更一致的图景。
更新日期:2021-01-12
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