Improved conduction and orbital polarization in ultrathin LaNiO3 sublayer by modulating octahedron rotation in LaNiO3/CaTiO3 superlattices

Wenxiao Shi, Jing Zhang, Bowen Yu, Jie Zheng, Mengqin Wang, Zhe Li, Jingying Zheng, Banggui Liu (), Yunzhong Chen, Fengxia Hu, Baogen Shen, Yuansha Chen () and Jirong Sun ()
Additional contact information
Wenxiao Shi: Chinese Academy of Sciences
Jing Zhang: Songshan Lake Materials Laboratory
Bowen Yu: Chinese Academy of Sciences
Jie Zheng: Chinese Academy of Sciences
Mengqin Wang: Chinese Academy of Sciences
Zhe Li: Chinese Academy of Sciences
Jingying Zheng: Fuzhou University
Banggui Liu: Chinese Academy of Sciences
Yunzhong Chen: Chinese Academy of Sciences
Fengxia Hu: Chinese Academy of Sciences
Baogen Shen: Chinese Academy of Sciences
Yuansha Chen: Chinese Academy of Sciences
Jirong Sun: Chinese Academy of Sciences

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Artificial oxide heterostructures have provided promising platforms for the exploration of emergent quantum phases with extraordinary properties. Here, we demonstrate an approach to stabilize a distinct oxygen octahedron rotation (OOR) characterized by $${a}^{-}{a}^{-}{c}^{+}$$ a − a − c + in the ultrathin LaNiO3 sublayers of the LaNiO3/CaTiO3 superlattices. Unlike the $${a}^{-}{a}^{-}{c}^{-}$$ a − a − c − OOR in the LaNiO3 bare film, the $${a}^{-}{a}^{-}{c}^{+}$$ a − a − c + OOR favors high conductivity, driving the LaNiO3 sublayer to a metallic state of ~100 K even when the layer thickness is as thin as 2 unit cells (u.c.). Simultaneously, strongly preferred occupation of $${d}_{{x}^{2}-{y}^{2}}$$ d x 2 − y 2 orbital is achieved in LaNiO3 sublayers. The largest change of occupancy is as high as 35%, observed in the 2 u.c.-thick LaNiO3 sublayers sandwiched between 4 u.c.-thick CaTiO3 sublayers. X-ray absorption spectra indicate that the $${a}^{-}{a}^{-}{c}^{+}$$ a − a − c + OOR pattern of LaNiO3 achieved in the LaNiO3/CaTiO3 heterostructures has significantly enhanced the Ni-3d/O-2p hybridization, stabilizing the metallic phase in ultrathin LaNiO3 sublayers. The present work demonstrates that modulating the mode of OOR through heteroepitaxial synthesis can modify the orbital-lattice correlations in correlated perovskite oxides, revealing hidden properties of the materials.

Date: 2024
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DOI: 10.1038/s41467-024-54311-0

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