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

Zhengang Dong; Marios Hadjimichael; Bernat Mundet; Jaewon Choi; Charles C. Tam; Mirian Garcia-Fernandez; Stefano Agrestini; Claribel Domínguez; Regan Bhatta; Yue Yu; Yufeng Liang; Zhenping Wu; Jean-Marc Triscone; Chunjing Jia; Ke-Jin Zhou; Danfeng Li

doi:10.1021/acs.nanolett.4c06557

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

Zhengang Dong
, Marios Hadjimichael
, Bernat Mundet
, Jaewon Choi
, Charles C. Tam
, Mirian Garcia-Fernandez
, Stefano Agrestini
, Claribel Domínguez
, Regan Bhatta
, Yue Yu
, Yufeng Liang
, Zhenping Wu^*
, Jean-Marc Triscone
, Chunjing Jia^*
, Ke-Jin Zhou^*
, Danfeng Li^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

9 Citations (Scopus)

26 Downloads (CityUHK Scholars)

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. © 2025 American Chemical Society.

Original language	English
Pages (from-to)	1233-1241
Journal	Nano Letters
Volume	25
Issue number	3
Online published	9 Jan 2025
DOIs	https://doi.org/10.1021/acs.nanolett.4c06557
Publication status	Published - 22 Jan 2025

Funding

We thank Harold Hwang, Kyuho Lee, and Zhihai Zhu for discussions. We acknowledge the funding support from the National Natural Science Foundation of China (Grant No. 12174325) and a Guangdong Basic and Applied Basic Research Grant (Grant No. 2023A1515011352). This research was partially supported by research grants from the Research Grants Council (RGC) of the Hong Kong Special Administrative Region, China, under Early Career Scheme, General Research Fund, and ANR-RGC Joint Researh Scheme (CityU 21301221, CityU 11309622, CityU 11300923, and A-CityU102/23). Part of the work utilized the equipment support through a Collaborative Research Equipment Grant from RGC (C1018-22E). The work was also supported by the Fund of State Key Laboratory of Information Photonics and Optical Communications (IPOC2021ZT05) and the Fundamental Research Funds for the Central Universities (BUPT, 2023ZCJH1). M.H., C.D., and J.-M.T. acknowledge the support by the Swiss National Science Foundation - division II (Grant Nos. 200020_179155 and 200020_207338). C.J. acknowledges the support by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award No. DE-SC0022216. We thank Diamond Light Source for providing beamtime under proposal ID MM32305. We also acknowledge access to the electron microscopy facilities at the Interdisciplinary Centre for Electron Microscopy (CIME), École Polytechnique Fédérale de Lausanne.

Research Keywords

electronic structure
infinite-layer nickelates
NaH
off-axis RF magnetron sputtering
orthorhombic substrates
topochemistry

Publisher's Copyright Statement

This full text is made available under CC-BY 4.0. https://creativecommons.org/licenses/by/4.0/

RGC Funding Information

RGC-funded

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10.1021/acs.nanolett.4c06557

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Dong, Z., Hadjimichael, M., Mundet, B., Choi, J., Tam, C. C., Garcia-Fernandez, M., Agrestini, S., Domínguez, C., Bhatta, R., Yu, Y., Liang, Y., Wu, Z., Triscone, J.-M., Jia, C., Zhou, K.-J., & Li, D. (2025). Topochemical Synthesis and Electronic Structure of High-Crystallinity Infinite-Layer Nickelates on an Orthorhombic Substrate. Nano Letters, 25(3), 1233-1241. https://doi.org/10.1021/acs.nanolett.4c06557

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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. {\textcopyright} 2025 American Chemical Society.",

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author = "Zhengang Dong and Marios Hadjimichael and Bernat Mundet and Jaewon Choi and Tam, \{Charles C.\} and Mirian Garcia-Fernandez and Stefano Agrestini and Claribel Dom{\'i}nguez and Regan Bhatta and Yue Yu and Yufeng Liang and Zhenping Wu and Jean-Marc Triscone and Chunjing Jia and Ke-Jin Zhou and Danfeng Li",

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Dong, Z, Hadjimichael, M, Mundet, B, Choi, J, Tam, CC, Garcia-Fernandez, M, Agrestini, S, Domínguez, C, Bhatta, R, Yu, Y, Liang, Y, Wu, Z, Triscone, J-M, Jia, C, Zhou, K-J & Li, D 2025, 'Topochemical Synthesis and Electronic Structure of High-Crystallinity Infinite-Layer Nickelates on an Orthorhombic Substrate', Nano Letters, vol. 25, no. 3, pp. 1233-1241. https://doi.org/10.1021/acs.nanolett.4c06557

TY - JOUR

T1 - Topochemical Synthesis and Electronic Structure of High-Crystallinity Infinite-Layer Nickelates on an Orthorhombic Substrate

AU - Dong, Zhengang

AU - Hadjimichael, Marios

AU - Mundet, Bernat

AU - Choi, Jaewon

AU - Tam, Charles C.

AU - Garcia-Fernandez, Mirian

AU - Agrestini, Stefano

AU - Domínguez, Claribel

AU - Bhatta, Regan

AU - Yu, Yue

AU - Liang, Yufeng

AU - Wu, Zhenping

AU - Triscone, Jean-Marc

AU - Jia, Chunjing

AU - Zhou, Ke-Jin

AU - Li, Danfeng

PY - 2025/1/22

Y1 - 2025/1/22

N2 - 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. © 2025 American Chemical Society.

AB - 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. © 2025 American Chemical Society.

KW - electronic structure

KW - infinite-layer nickelates

KW - NaH

KW - off-axis RF magnetron sputtering

KW - orthorhombic substrates

KW - topochemistry

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UR - https://www.scopus.com/pages/publications/85214872595#tab=impact

U2 - 10.1021/acs.nanolett.4c06557

DO - 10.1021/acs.nanolett.4c06557

M3 - RGC 21 - Publication in refereed journal

C2 - 39783860

SN - 1530-6984

VL - 25

SP - 1233

EP - 1241

JO - Nano Letters

JF - Nano Letters

IS - 3

ER -

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

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Funding

Research Keywords

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ANR: An atomic-level platform for probing intertwined orders in correlated quantum materials (ImagingQM)

GRF: Phase-Sensitive Measurements in Mesoscopic Nickelate Superconducting Junction Devices

CRF: Advanced Integrated In-Situ Laser Molecular Beam Epitaxy and Angle-Resolved Photoemission Spectroscopy Platform for Quantum Materials Research

Cite this

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

Abstract

Funding

Research Keywords

Publisher's Copyright Statement

RGC Funding Information

Access Output

Other Access Options

Permanent Link

Other Files and Links

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Projects

ANR: An atomic-level platform for probing intertwined orders in correlated quantum materials (ImagingQM)

GRF: Phase-Sensitive Measurements in Mesoscopic Nickelate Superconducting Junction Devices

CRF: Advanced Integrated In-Situ Laser Molecular Beam Epitaxy and Angle-Resolved Photoemission Spectroscopy Platform for Quantum Materials Research

Cite this