Chen Jikun, Mao Wei, Gao Lei, Yan Fengbo, Yajima Takeaki, Chen Nuofu, Chen Zhizhong, Dong Hongliang, Ge Binghui, Zhang Peng, Cao Xingzhong, Wilde Markus, Jiang Yong, Terai Takayuki, Shi Jian
Beijing Advanced Innovation Center for Materials Genome Engineering, School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing, 100083, China.
School of Engineering, The University of Tokyo, 2-11-16 Yayoi, Bunkyo-ku, Tokyo, 113-0032, Japan.
Adv Mater. 2020 Feb;32(6):e1905060. doi: 10.1002/adma.201905060. Epub 2019 Dec 19.
The discovery of hydrogen-induced electron localization and highly insulating states in d-band electron correlated perovskites has opened a new paradigm for exploring novel electronic phases of condensed matters and applications in emerging field-controlled electronic devices (e.g., Mottronics). Although a significant understanding of doping-tuned transport properties of single crystalline correlated materials exists, it has remained unclear how doping-controlled transport properties behave in the presence of planar defects. The discovery of an unexpected high-concentration doping effect in defective regions is reported for correlated nickelates. It enables electronic conductance by tuning the Fermi-level in Mott-Hubbard band and shaping the lower Hubbard band state into a partially filled configuration. Interface engineering and grain boundary designs are performed for H SmNiO /SrRuO heterostructures, and a Mottronic device is achieved. The interfacial aggregation of hydrogen is controlled and quantified to establish its correlation with the electrical transport properties. The chemical bonding between the incorporated hydrogen with defective SmNiO is further analyzed by the positron annihilation spectroscopy. The present work unveils new materials physics in correlated materials and suggests novel doping strategies for developing Mottronic and iontronic devices via hydrogen-doping-controlled orbital occupancy in perovskite heterostructures.
在d带电子相关钙钛矿中发现氢诱导的电子局域化和高绝缘态,为探索凝聚态物质的新型电子相以及在新兴场控电子器件(如Mottronics)中的应用开辟了新的范式。尽管对单晶相关材料的掺杂调控输运性质已有重要认识,但在存在平面缺陷的情况下,掺杂控制的输运性质如何表现仍不清楚。本文报道了在相关镍酸盐的缺陷区域发现意外的高浓度掺杂效应。它通过调节莫特-哈伯德带中的费米能级并将较低的哈伯德带态塑造成部分填充构型来实现电子电导。对H SmNiO /SrRuO异质结构进行了界面工程和晶界设计,并实现了一个Mottronic器件。对氢的界面聚集进行了控制和量化,以建立其与电输运性质的相关性。通过正电子湮没光谱进一步分析了掺入的氢与缺陷SmNiO之间的化学键。本工作揭示了相关材料中的新材料物理,并提出了通过钙钛矿异质结构中氢掺杂控制的轨道占据来开发Mottronic和离子电子器件的新型掺杂策略。