On the Topotactic Phase Transition Achieving Superconducting Infinite‐Layer Nickelates

Topotactic reduction is critical to a wealth of phase transitions of current interest, including synthesis of the superconducting nickelate Nd<sub>0.8</sub>Sr<sub>0.2</sub>NiO<sub>2</sub>, reduced from the initial Nd<sub>0.8</sub>Sr<sub>0.2</sub>NiO<sub>3</sub>/SrTiO<sub>3</sub> heterostructure. Due to the highly sensitive and often damaging nature of the topotactic reduction, however, only a handful of research groups have been able to reproduce the superconductivity results. A series of in situ synchrotron-based investigations reveal that this is due to the necessary formation of an initial, ultrathin layer at the Nd<sub>0.8</sub>Sr<sub>0.2</sub>NiO<sub>3</sub> surface that helps to mediate the introduction of hydrogen into the film such that apical oxygens are first removed from the Nd<sub>0.8</sub>Sr<sub>0.2</sub>NiO<sub>3</sub> / SrTiO<sub>3</sub> (001) interface and delivered into the reducing environment. This allows the square-planar / perovskite interface to stabilize and propagate from the bottom to the top of the film without the formation of interphase defects. Importantly, neither geometric rotations in the square planar structure nor significant incorporation of hydrogen within the films is detected, obviating its need for superconductivity. These findings unveil the structural basis underlying the transformation pathway and provide important guidance on achieving the superconducting phase in reduced nickelate systems.

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Publication Details

Journal
Advanced Materials
Published
2024-09-01
DOI
https://doi.org/10.1002/adma.202402484
Citations
5
Primary Topic
Magnetic and transport properties of perovskites and related materials
Type
article
Field-Weighted Citation Impact
0.59

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article

On the Topotactic Phase Transition Achieving Superconducting Infinite‐Layer Nickelates

Daniel Phelan, Hui Cao, Bruce A. Buchholz, Zihua Zhu et al.
5 citations
Advanced Materials
Magnetic and transport properties of perovskites and related materials
0.59
article

On the Topotactic Phase Transition Achieving Superconducting Infinite‐Layer Nickelates

Daniel Phelan, Hui Cao, Bruce A. Buchholz, Zihua Zhu, Hua Zhou, Yingge Du, Binod Paudel, J. S. Jiang, Dillon D. Fong, Evguenia Karapetrova, Chengjun Sun, Krishna Prasad Koirala, Yan Li, Hong Zheng, Brandon Fisher, Shelly D. Kelly, Anand Bhattacharya, Xi Yan, Huanhua Wang, Zhan Zhang, Changjiang Liu, J. F. Mitchell, K. V. L. V. Narayanachari
article en
5 citations

Abstract

Topotactic reduction is critical to a wealth of phase transitions of current interest, including synthesis of the superconducting nickelate Nd<sub>0.8</sub>Sr<sub>0.2</sub>NiO<sub>2</sub>, reduced from the initial Nd<sub>0.8</sub>Sr<sub>0.2</sub>NiO<sub>3</sub>/SrTiO<sub>3</sub> heterostructure. Due to the highly sensitive and often damaging nature of the topotactic reduction, however, only a handful of research groups have been able to reproduce the superconductivity results. A series of in situ synchrotron-based investigations reveal that this is due to the necessary formation of an initial, ultrathin layer at the Nd<sub>0.8</sub>Sr<sub>0.2</sub>NiO<sub>3</sub> surface that helps to mediate the introduction of hydrogen into the film such that apical oxygens are first removed from the Nd<sub>0.8</sub>Sr<sub>0.2</sub>NiO<sub>3</sub> / SrTiO<sub>3</sub> (001) interface and delivered into the reducing environment. This allows the square-planar / perovskite interface to stabilize and propagate from the bottom to the top of the film without the formation of interphase defects. Importantly, neither geometric rotations in the square planar structure nor significant incorporation of hydrogen within the films is detected, obviating its need for superconductivity. These findings unveil the structural basis underlying the transformation pathway and provide important guidance on achieving the superconducting phase in reduced nickelate systems.

Advanced MaterialsVol. 36(40)
Northwestern University (US), Argonne National Laboratory (US), Pacific Northwest National Laboratory (US), Chinese Academy of Sciences (CN), Environmental Molecular Sciences Laboratory (US), Institute of High Energy Physics (CN), University of Chinese Academy of Sciences (CN)
National Science Foundation, U.S. Department of Energy, Battelle, Northwestern University, University of Chicago, State University of New York, National Natural Science Foundation of China, Chinese Academy of Sciences, Office of Science, University at Buffalo, Materials Research Science and Engineering Center, Harvard University, Division of Materials Research, Division of Electrical, Communications and Cyber Systems, Basic Energy Sciences, Biological and Environmental Research, Argonne National Laboratory, Division of Materials Sciences and Engineering
Openalex Percentile: Top 40%
Magnetic and transport properties of perovskites and related materials
0.59
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