Sequential Spin State Transition and Intermetallic Charge Transfer in PbCoO3

Zhehong Liu, Yuki Sakai, Junye Yang, Wenmin Li, Ying Liu, Xubin Ye, Shijun Qin, Jinming Chen, Stefano Agrestini, Kai Chen, Sheng-chieh Liao, Shu-chih Haw, François Baudelet, Hirofumi Ishii, Takumi Nishikubo, Hayato Ishizaki, Tatsuru Yamamoto, Zhao Pan, Masayuki Fukuda, Kotaro OhashiKana Matsuno, Akihiko Machida, Tetsu Watanuki, Saori I. Kawaguchi, Angel M Arevalo-lopez, Changqing Jin, Zhiwei Hu, J. Paul Attfield, Masaki Azuma, Youwen Long

Research output: Contribution to journalArticlepeer-review

Abstract

Spin state transition and intermetallic charge transfer can essentially change material structural and physical properties with a fashion of excluding external chemical doping. However, these two effects have rarely been found to occur sequentially in a specific material. In this article, we show the unprecedented realization of these two phenomena in a perovskite oxide PbCoO3 ABO3 under high pressure. PbCoO3 possesses a peculiar A- and B-site ordered charge distribution Pb2+Pb4+3Co2+2Co3+2O12 with insulating behavior at ambient conditions. The high spin Co2+ gradually changes to low spin with increasing pressure up to about 15 GPa, leading to the anomalous increase of resistance magnitude. Between 15 GPa and 30 GPa, the intermetallic charge transfer occurs between Pb4+ and Co2+ cations. The accumulated charge-transfer effect triggers a metal-insulator transition as well as a first-order structural phase transition toward a Tetra.-I phase at the onset of ~20 GPa near room temperature. On further compression over 30 GPa, the charge transfer completes, giving rise to another first-order structural transformation toward a Tetra.-II phase and the reentrant electrical insulating behavior.
Original languageEnglish
JournalJournal of the American Chemical Society
Early online date21 Feb 2020
DOIs
Publication statusE-pub ahead of print - 21 Feb 2020

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