Electron microscopy study of interface structure in infinite-layer nickelate-based superconducting thin films

LI Boyu; HU Kejun; LIN Renju; HAN Kun; HUANG Zhen; GE Binghui; SONG Dongsheng

doi:10.7498/aps.74.20250171

Abstract

The discovery of superconductivity in infinite-layer nickelate Nd_0.8Sr_0.2NiO₂ has established another type of unconventional superconductors, whose structure and electron pairing mechanism are similar to those of cuprate superconductors. Unlike in cuprate superconductors, superconductivity in infinite-layer nickelates has only been observed in thin film samples, where heterointerface structures, elemental doping, and the infinite-layer configuration are critical for epitaxial systems. Therefore, the film-substrate interfacial effects require exploration for understanding superconductivity. However, comparative studies on the interfacial structures between superconducting and non-superconducting Nd_0.8Sr_0.2NiO_x nickelate thin films have not been reported in the literature so far.This work focuses on Nd_0.8Sr_0.2NiO₃/SrTiO₃ and Nd_0.8Sr_0.2NiO₂/SrTiO₃, and the phase distribution and interfacial structural changes in superconducting and non-superconducting nickelate thin films are characterized in detail by using scanning transmission electron microscopy (STEM). Further analysis of the corresponding atomic high-angle annular dark filed (HAADF), integrated differential phase contrast (iDPC) and energy dispersive X-ray spectroscopy (EDS) maps reveals the phenomena such as elements mixing, atomic steps, and changes in lattice parameters at the interfaces. These results also show that in the Nd_0.8Sr_0.2NiO₂ film, the first 1−2 unit cells near the interface are not fully reduced to the superconducting infinite-layer structure. Such findings contribute to alleviating the strong polarity discontinuity at the sharp interface.This study also emphasizes the atomic reconstruction and the modulation effect at the interface between the substrate and the film, thus enriching the understanding of the structural properties of the Nd_0.8Sr_0.2NiO_x films, and providing crucial experimental evidence for understanding the interfacial structure of infinite-layer nickelates.

Keywords:

Authors and contacts

Information Materials and Intelligent Sensing Laboratory of Anhui Province, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, Institutes of Physical Science and Information Technology, Anhui University, Hefei 230601, China

Corresponding author: HAN Kun, hankun@ahu.edu.cn ; SONG Dongsheng, dsong@ahu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 52173215, 52473226).

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References

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图 1 (a), (b) Nd_0.8Sr_0.2NiO₃/SrTiO₃原子模型图及对应的HAADF图像; (c), (d) Nd_0.8Sr_0.2NiO₂/SrTiO₃原子模型图及对应的HAADF图像; (e) Nd_0.8Sr_0.2NiO₂/SrTiO₃, Nd_0.8Sr_0.2NiO₃/SrTiO₃的电阻率随温度的变化; (f), (g) Nd_0.8Sr_0.2NiO₂/SrTiO₃, Nd_0.8Sr_0.2NiO₃/SrTiO₃的几何相位图, 黄框标记的为RP相区域

Figure 1. (a), (b) Atomic structure model and HAADF image of the Nd_0.8Sr_0.2NiO₃/SrTiO₃; (c), (d) the atomic structure model and HAADF image of the Nd_0.8Sr_0.2NiO₂/SrTiO₃; (e) the temperature-dependent resistivity profile of Nd_0.8Sr_0.2NiO₂/SrTiO₃ and Nd_0.8Sr_0.2NiO₃/SrTiO₃; (f), (g) the geometric phase analysis of Nd_0.8Sr_0.2NiO₂/SrTiO₃ and Nd_0.8Sr_0.2NiO₃/SrTiO₃, the RP phase regions marked by yellow boxes.

DownLoad: Full-Size Img PowerPoint

图 2 (a) Nd_0.8Sr_0.2NiO₃/STO界面[100]取向的HAADF图像及相应的EDS分布图; (b) 图(a)对应的EDS积分强度分析图; (c) Nd_0.8Sr_0.2NiO₂/STO界面[100]取向HAADF图像及相应的EDS分布图; (d) 图(c)对应的EDS积分强度分析图

Figure 2. (a) HAADF image at [100] orientation of the Nd_0.8Sr_0.2NiO₃/STO interface and corresponding EDS mapping images; (b) the EDS integrated line intensity analysis corresponding to panel (a); (c) the HAADF image at [100] orientation of the Nd_0.8Sr_0.2NiO₂/STO interface and corresponding EDS mapping images; (d) the EDS intensity analysis corresponding to panel (c).

DownLoad: Full-Size Img PowerPoint

图 3 (a) Nd_0.8Sr_0.2NiO₃/SrTiO₃沿[100]方向HAADF和iDPC图像; (b) Nd_0.8Sr_0.2NiO₂/SrTiO₃沿[100]方向HAADF和iDPC图像; (c) Nd_0.8Sr_0.2NiO₂/SrTiO₃界面处原子台阶HAADF图像; (d) Nd_0.8Sr_0.2NiO₂/SrTiO₃界面处面内a和面外c晶格常数在空间上的变化; (e) 1, 2, 3三个区域对应的放大iDPC图和原子模型图

Figure 3. (a) HAADF and iDPC images in the direction of [100] of the Nd_0.8Sr_0.2NiO₃/SrTiO₃; (b) HAADF and iDPC images in the direction of [100] of the Nd_0.8Sr_0.2NiO₂/SrTiO₃; (c) HAADF image of atomic steps appear at the Nd_0.8Sr_0.2NiO₂/SrTiO₃ interface; (d) spatial variation of the in-plane (a) and out-of-plane (c) lattice parameters across the Nd_0.8Sr_0.2NiO₂/SrTiO₃; (e) the magnified iDPC images and structure model corresponding to regions 1, 2 and 3.

DownLoad: Full-Size Img PowerPoint

图 4 (a), (c) Nd_0.8Sr_0.2NiO₃/SrTiO₃, Nd_0.8Sr_0.2NiO₂/SrTiO₃薄膜沿[100]带轴的HAADF图像; (b), (d) Nd_0.8Sr_0.2NiO₃/SrTiO₃, Nd_0.8Sr_0.2NiO₂/SrTiO₃沿面内和面外方向的晶格常数随位置的变化

Figure 4. (a), (c) HAADF images of the Nd_0.8Sr_0.2NiO₃/SrTiO₃ and Nd_0.8Sr_0.2NiO₂/SrTiO₃ films along the [100] axis; (b), (d) variation of the lattice constants along the in-plane and out-of-plane directions as a function of position for Nd_0.8Sr_0.2NiO₃/SrTiO₃ and Nd_0.8Sr_0.2NiO₂/SrTiO₃ films.

DownLoad: Full-Size Img PowerPoint

[1]	Gu Q Q, Li Y Y, Wan S Y, Li H Z, Guo W, Yang H, Li Q, Zhu X Y, Pan X Q, Nie Y F, Wen H H 2020 Nat. Commun. 11 6027 Google Scholar
[2]	Hepting M, Li D, Jia C J, Lu H, Paris E, Tseng Y, Feng X, Osada M, Been E, Hikita Y, Chuang Y D, Hussain Z, Zhou K J, Nag A, Garcia Fernandez M, Rossi M, Huang H Y, Huang D J, Shen Z X, Schmitt T, Hwang H Y, Moritz B, Zaanen J, Devereaux T P, Lee W S 2020 Nat. Mater. 19 381 Google Scholar
[3]	Goodge B H, Geisler B, Lee K, Osada M, Wang B Y, Li D F, Hwang H Y, Pentcheva R, Kourkoutis L F 2023 Nat. Mater. 22 466 Google Scholar
[4]	Anisimov V I, Bukhvalov D, Rice T M 1999 Phys. Rev. B 59 7901 Google Scholar
[5]	Crespin M, Levitz P, Gatineau L 1983 J. Chem. Soc., Faraday Trans. 79 1181 Google Scholar
[6]	Hayward M A, Green M A, Rosseinsky M J, Sloan J 1999 J. Am. Chem. Soc. 121 8843 Google Scholar
[7]	Li D F, Lee K, Wang B Y, Osada M, Crossley S, Lee H R, Cui Y, Hikita Y, Hwang H Y 2019 Nature 572 624 Google Scholar
[8]	Li D F, Wang B Y, Lee K, Harvey S P, Osada M, Goodge B H, Kourkoutis L F, Hwang H Y 2020 Phys. Rev. Lett. 125 027001 Google Scholar
[9]	Puphal P, Wu Y M, Fürsich K, Lee H, Pakdaman M, Bruin J A N, Nuss J, Suyolcu Y E, van Aken P A, Keimer B, Isobe M, Hepting M 2021 Sci. Adv. 7 eabl8091 Google Scholar
[10]	Li Q, He C P, Si J, Zhu X Y, Zhang Y, Wen H H 2020 Commun. Mater. 1 16 Google Scholar
[11]	Wang B X, Zheng H, Krivyakina E, Chmaissem O, Lopes P P, Lynn J W, Gallington L C, Ren Y, Rosenkranz S, Mitchell J F 2020 Phys. Rev. Mater. 4 084409 Google Scholar
[12]	Lee Y, Wei X, Yu Y J, Bhatt L, Lee K, Goodge B H, Harvey S P, Wang B Y, Muller D A, Kourkoutis L F, Lee W S, Raghu S, Hwang H Y 2025 Nat. Synth. DOI: 10.1038/s44160-024-00714-2
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[14]	Ko E K, Yu Y J, Liu Y D, Bhatt L, Li J R, Thampy V, Kuo C T, Wang B Y, Lee Y, Lee K, Lee J, Goodge B H, Muller D A, Hwang H Y 2025 Nature 638 935 Google Scholar
[15]	Zhou G D, Lü W, Wang H, Nie Z H, Chen Y Q, Li Y Y, Huang H L, Chen W Q, Sun Y J, Xue Q K 2025 Nature 640 641 Google Scholar
[16]	Bernardini F, Olevano V, Blase X, Cano A 2020 J. Phys. Mater. 3 035003 Google Scholar
[17]	Geisler B, Pentcheva R 2020 Phys. Rev. B 102 020502 Google Scholar
[18]	Lee K, Goodge B H, Li D F, Osada M, Wang B Y, Cui Y, Kourkoutis L F, Hwang H Y 2020 APL Mater. 8 041107 Google Scholar
[19]	Tokuda Y, Kobayashi S, Ohnishi T, Mizoguchi T, Shibata N, Ikuhara Y, Yamamoto T 2011 Appl. Phys. Lett. 99 033110 Google Scholar
[20]	Bak J, Bae H B, Kim J, Oh J, Chung S Y 2017 Nano Lett. 17 3126 Google Scholar
[21]	Goodge B H, Li D F, Lee K, Osada M, Wang B Y, Sawatzky G A, Hwang H Y, Kourkoutis L F 2021 Proc. Natl. Acad. Sci. U.S.A. 118 e2007683118 Google Scholar
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