Observation of novel charge ordering and spin reorientation in perovskite oxide PbFeO3

• Published in: Nature communications Vol. 12; no. 1; p. 1917
• Main Authors: Ye, Xubin, Zhao, Jianfa, Das, Hena, Sheptyakov, Denis, Yang, Junye, Sakai, Yuki, Hojo, Hajime, Liu, Zhehong, Zhou, Long, Cao, Lipeng, Nishikubo, Takumi, Wakazaki, Shogo, Dong, Cheng, Wang, Xiao, Hu, Zhiwei, Lin, Hong-Ji, Chen, Chien-Te, Sahle, Christoph, Efiminko, Anna, Cao, Huibo, Calder, Stuart, Mibu, Ko, Kenzelmann, Michel, Tjeng, Liu Hao, Yu, Runze, Azuma, Masaki, Jin, Changqing, Long, Youwen
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 26.03.2021; Nature Publishing Group; Nature Portfolio
• Subjects: 639/301/119/1002; 639/301/119/997; Antiferromagnetism; Charge distribution; CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; Critical temperature; Energy balance; Ferromagnetism; Heavy metals; Humanities and Social Sciences; Iron; Iron constituents; Lead; magnetic properties and materials; multidisciplinary; Oxidation; Perovskites; Physical properties; Physics; Science; Science (multidisciplinary); structure of solids and liquids; Transition metals; Unit cell; TRANSITION; DIFFRACTION; STATES; MAGNETIC-PROPERTIES; CRYSTAL-STRUCTURE; STABILITY
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-021-22064-9

Pb M O 3 ( M  = 3 d transition metals) family shows systematic variations in charge distribution and intriguing physical properties due to its delicate energy balance between Pb 6 s and transition metal 3 d orbitals. However, the detailed structure and physical properties of PbFeO 3 remain unclear. Herein, we reveal that PbFeO 3 crystallizes into an unusual 2 a p  × 6 a p  × 2 a p orthorhombic perovskite super unit cell with space group Cmcm . The distinctive crystal construction and valence distribution of Pb 2+ 0.5 Pb 4+ 0.5 FeO 3 lead to a long range charge ordering of the -A-B-B- type of the layers with two different oxidation states of Pb (Pb 2+ and Pb 4+ ) in them. A weak ferromagnetic transition with canted antiferromagnetic spins along the a -axis is found to occur at 600 K. In addition, decreasing the temperature causes a spin reorientation transition towards a collinear antiferromagnetic structure with spin moments along the b -axis near 418 K. Our theoretical investigations reveal that the peculiar charge ordering of Pb generates two Fe 3+ magnetic sublattices with competing anisotropic energies, giving rise to the spin reorientation at such a high critical temperature. PbFeO 3 is part of a family of lead based perovskites with many intriguing properties; however, difficulties in synthesis have hampered investigation. Here, the authors present a detailed study of the structure of PbFeO 3 observing unique charge ordering and spin orientation among the constituent ions.