Topochemical Synthesis and Electronic Structure of High-Crystallinity Infinite-Layer Nickelates on an Orthorhombic Substrate
Superconductivity in infinite-layer nickelates has stirred much research interest, to which questions regarding the nature of superconductivity remain elusive. A critical leap forward to address these intricate questions is through the growth of high-crystallinity infinite-layer nickelates, including the "parent" phase. Here, we report the synthesis of a high-quality thin-film nickelate, NdNiO<sub>2</sub>. This is achieved through the growth of a perovskite precursor phase (NdNiO<sub>3</sub>) of superior crystallinity on the NdGaO<sub>3</sub> substrate by off-axis RF magnetron sputtering and a low-temperature topochemical reduction using NaH. We observe a nonlinear Hall effect at low temperatures in this "non-doped" phase. We further study the electronic properties using advanced X-ray scattering and first-principles calculations. We observe spectroscopic indications of the enhanced two-dimensionality and a reduced hybridization of Nd 5<i>d</i> and Ni 3<i>d</i> orbitals. These findings unlock new pathways for preparing high-quality infinite-layer nickelates and provide new insights into the intrinsic features of these compounds.
Authors
- Stefano Agrestini (ORCID: https://orcid.org/0000-0002-3625-880X)
- Yufeng Liang (ORCID: https://orcid.org/0000-0003-4402-4146)
- Rudra P. Bhatta
- Bernat Mundet (ORCID: https://orcid.org/0000-0003-0608-2070)
- Ke‐Jin Zhou (ORCID: https://orcid.org/0000-0001-9293-0595)
- Marios Hadjimichael (ORCID: https://orcid.org/0000-0001-6618-8075)
- Jean‐Marc Triscone (ORCID: https://orcid.org/0000-0002-9067-701X)
- Danfeng Li (ORCID: https://orcid.org/0000-0001-6894-6765)
- Mirian García‐Fernández (ORCID: https://orcid.org/0000-0002-6982-9066)
- Charles C. Tam (ORCID: https://orcid.org/0000-0002-5207-6512)
- Jaewon Choi (ORCID: https://orcid.org/0000-0003-4616-4345)
- Zhenping Wu (ORCID: https://orcid.org/0000-0003-2986-8068)
- Chunjing Jia (ORCID: https://orcid.org/0000-0001-7999-1932)
- Yue Yu (ORCID: https://orcid.org/0000-0003-0205-0995)
- Zhengang Dong
- Claribel Domínguez
Institutions
- University of Geneva (CH)
- Beijing University of Posts and Telecommunications (CN)
- Lawrence Berkeley National Laboratory (US)
- City University of Hong Kong (HK)
- Diamond Light Source (GB)
- University of Florida (US)
- University of Bristol (GB)
- University of Warwick (GB)
- Institut Català de Nanociència i Nanotecnologia (ES)
- City University of Hong Kong, Shenzhen Research Institute (CN)
- École Polytechnique Fédérale de Lausanne (CH)
Publication Details
- Journal
- Nano Letters
- Published
- 2025-01-09
- DOI
- https://doi.org/10.1021/acs.nanolett.4c06557
- Citations
- 6
- Primary Topic
- Magnetic and transport properties of perovskites and related materials
- Type
- article
- Field-Weighted Citation Impact
- 2.56
Funders
- National Science Foundation
- U.S. Department of Energy
- City University of Hong Kong
- Diamond Light Source
- Institut Català de Nanociència i Nanotecnologia
- University of Warwick
- University of Bristol
- Agence Nationale de la Recherche
- École Polytechnique Fédérale de Lausanne
- Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung
- National Natural Science Foundation of China
- Beijing University of Posts and Telecommunications
- Research Grants Council, University Grants Committee
- Université de Genève
- State Key Laboratory of Information Photonics and Optical Communications
- Office of Science
- Shenzhen Research Institute, City University of Hong Kong
- Fundamental Research Funds for the Central Universities
- Basic and Applied Basic Research Foundation of Guangdong Province
- Basic Energy Sciences
- Lawrence Berkeley National Laboratory