Origin of a topotactic reduction effect for superconductivity in infinite-layer nickelates
Topotactic reduction utilizing metal hydrides as reagents has emerged as an effective approach to achieve exceptionally low oxidization states of metal ions and unconventional coordination networks. This method opens avenues to the development of entirely new functional materials, with one notable e...
| Main Authors: | , , , , , , , , , , , , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2024
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| Online Access: | https://hdl.handle.net/10356/181367 |
| _version_ | 1824456373704851456 |
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| author | Zeng, Shengwei Tang, Chi Sin Luo, Zhaoyang Chow, Lin Er Lim, Zhi Shiuh Prakash, Saurav Yang, Ping Diao, Caozheng Yu, Xiaojiang Xing, Zhenxiang Ji, Rong Yin, Xinmao Li, Changjian Wang, Renshaw Xiao He, Qian Breese, Mark B. H. Ariando, A. Liu, Huajun |
| author2 | School of Physical and Mathematical Sciences |
| author_facet | School of Physical and Mathematical Sciences Zeng, Shengwei Tang, Chi Sin Luo, Zhaoyang Chow, Lin Er Lim, Zhi Shiuh Prakash, Saurav Yang, Ping Diao, Caozheng Yu, Xiaojiang Xing, Zhenxiang Ji, Rong Yin, Xinmao Li, Changjian Wang, Renshaw Xiao He, Qian Breese, Mark B. H. Ariando, A. Liu, Huajun |
| author_sort | Zeng, Shengwei |
| collection | NTU |
| description | Topotactic reduction utilizing metal hydrides as reagents has emerged as an effective approach to achieve exceptionally low oxidization states of metal ions and unconventional coordination networks. This method opens avenues to the development of entirely new functional materials, with one notable example being the infinite-layer nickelate superconductors. However, the reduction effect on the atomic reconstruction and electronic structures-crucial for superconductivity-remains largely unresolved. We designed two sets of control Nd_{0.8}Sr_{0.2}NiO_{2} thin films and used secondary ion mass spectroscopy to highlight the absence of reduction-induced hydrogen intercalation. X-ray absorption spectroscopy revealed a significant linear dichroism with dominant Ni 3d_{x2-y2} orbitals on superconducting samples, indicating a Ni single-band nature of infinite-layer nickelates. Consistent with the superconducting T_{c}, the Ni 3d orbitals asymmetry manifests a domelike dependence on the reduction duration. Our results unveil the critical role of reduction in modulating the Ni-3d orbital polarization and its impact on the superconducting properties. |
| first_indexed | 2025-02-19T03:53:04Z |
| format | Journal Article |
| id | ntu-10356/181367 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2025-02-19T03:53:04Z |
| publishDate | 2024 |
| record_format | dspace |
| spelling | ntu-10356/1813672024-11-27T01:04:16Z Origin of a topotactic reduction effect for superconductivity in infinite-layer nickelates Zeng, Shengwei Tang, Chi Sin Luo, Zhaoyang Chow, Lin Er Lim, Zhi Shiuh Prakash, Saurav Yang, Ping Diao, Caozheng Yu, Xiaojiang Xing, Zhenxiang Ji, Rong Yin, Xinmao Li, Changjian Wang, Renshaw Xiao He, Qian Breese, Mark B. H. Ariando, A. Liu, Huajun School of Physical and Mathematical Sciences School of Electrical and Electronic Engineering Physics Metals ions Nickelates Topotactic reduction utilizing metal hydrides as reagents has emerged as an effective approach to achieve exceptionally low oxidization states of metal ions and unconventional coordination networks. This method opens avenues to the development of entirely new functional materials, with one notable example being the infinite-layer nickelate superconductors. However, the reduction effect on the atomic reconstruction and electronic structures-crucial for superconductivity-remains largely unresolved. We designed two sets of control Nd_{0.8}Sr_{0.2}NiO_{2} thin films and used secondary ion mass spectroscopy to highlight the absence of reduction-induced hydrogen intercalation. X-ray absorption spectroscopy revealed a significant linear dichroism with dominant Ni 3d_{x2-y2} orbitals on superconducting samples, indicating a Ni single-band nature of infinite-layer nickelates. Consistent with the superconducting T_{c}, the Ni 3d orbitals asymmetry manifests a domelike dependence on the reduction duration. Our results unveil the critical role of reduction in modulating the Ni-3d orbital polarization and its impact on the superconducting properties. Ministry of Education (MOE) S. W. Z., Z. S. L., and H. J. L. acknowledge the RIE2025 MTC Individual Research Grants (M22K2c0084), National Research Foundation Competitive Research Program (NRF-CRP28-2022- 0002), Career Development Fund (C210812020) and Central Research Fund from the Agency for Science, Technology and Research (A*STAR) for the funding support. The work at NUS and the authors are supported by the Ministry of Education (MOE), Singapore, under its Tier-2 Academic Research Fund (AcRF) (Grants No. MOE-T2EP50121-0018 and No. MOE T2EP50123- 0013), the National Research Foundation (NRF) of Singapore under its NRF-ISF joint program (Grant No. NRF2020-NRF-ISF004-3518), and the SUSTechNUS Joint Research Program. X. R. W. acknowledges support from Singapore Ministry of Education under its Academic Research Fund (AcRF) Tier 2 (Grant No. MOET2EP50120-0006) and Tier 1 (Grant No. RG82/23). X. M. Y. acknowledges financial support by National Natural Science Foundation of China (Grant No. 12374378). C. S. T acknowledges the support from the NUS Emerging Scientist Fellowship. The authors would like to acknowledge the Singapore Synchrotron Light Source for providing the facility necessary for conducting the research. The Laboratory is a National Research Infrastructure under the National Research Foundation, Singapore. Any opinions, findings, and conclusions or recommendations expressed in this material are those of the author(s) and do not reflect the views of National Research Foundation, Singapore. 2024-11-27T01:04:16Z 2024-11-27T01:04:16Z 2024 Journal Article Zeng, S., Tang, C. S., Luo, Z., Chow, L. E., Lim, Z. S., Prakash, S., Yang, P., Diao, C., Yu, X., Xing, Z., Ji, R., Yin, X., Li, C., Wang, R. X., He, Q., Breese, M. B. H., Ariando, A. & Liu, H. (2024). Origin of a topotactic reduction effect for superconductivity in infinite-layer nickelates. Physical Review Letters, 133(6), 066503-. https://dx.doi.org/10.1103/PhysRevLett.133.066503 0031-9007 https://hdl.handle.net/10356/181367 10.1103/PhysRevLett.133.066503 39178458 2-s2.0-85200910227 6 133 066503 en MOE-T2EP50120-0006 RG82/23 Physical Review Letters © 2024 American Physical Society. All rights reserved. |
| spellingShingle | Physics Metals ions Nickelates Zeng, Shengwei Tang, Chi Sin Luo, Zhaoyang Chow, Lin Er Lim, Zhi Shiuh Prakash, Saurav Yang, Ping Diao, Caozheng Yu, Xiaojiang Xing, Zhenxiang Ji, Rong Yin, Xinmao Li, Changjian Wang, Renshaw Xiao He, Qian Breese, Mark B. H. Ariando, A. Liu, Huajun Origin of a topotactic reduction effect for superconductivity in infinite-layer nickelates |
| title | Origin of a topotactic reduction effect for superconductivity in infinite-layer nickelates |
| title_full | Origin of a topotactic reduction effect for superconductivity in infinite-layer nickelates |
| title_fullStr | Origin of a topotactic reduction effect for superconductivity in infinite-layer nickelates |
| title_full_unstemmed | Origin of a topotactic reduction effect for superconductivity in infinite-layer nickelates |
| title_short | Origin of a topotactic reduction effect for superconductivity in infinite-layer nickelates |
| title_sort | origin of a topotactic reduction effect for superconductivity in infinite layer nickelates |
| topic | Physics Metals ions Nickelates |
| url | https://hdl.handle.net/10356/181367 |
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