Topochemical Synthesis and Electronic Structure of High-Crystallinity Infinite-Layer Nickelates on an Orthorhombic Substrate

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Abstract
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, NdNiO2. This is achieved through the growth of a perovskite precursor phase (NdNiO3) of superior crystallinity on the NdGaO3 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 5d and Ni 3d orbitals. These findings unlock new pathways for preparing high-quality infinite-layer nickelates and provide new insights into the intrinsic features of these compounds.
Funding Information
  • Beijing University of Posts and Telecommunications (2023ZCJH1)
  • Research Grants Council, University Grants Committee (A-CityU102/23, C1018-22E, CityU 11300923, CityU 11309622, CityU 21301221)
  • State Key Laboratory of Information Photonics and Optical Communications (IPOC2021ZT05)
  • Schweizerischer Nationalfonds zur F?rderung der Wissenschaftlichen Forschung (200020_179155, 200020_207338)
  • Basic Energy Sciences (DE-SC0022216)
  • Basic and Applied Basic Research Foundation of Guangdong Province (2023A1515011352)
  • National Natural Science Foundation of China (12174325)

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