Controllable growth and electronic phase transitions for metastable perovskite rare-earth nickelate films

Zhou Xuan-Chi; Jiao Yong-Jie

doi:10.7498/aps.73.20240584

Abstract

The multiple electronic phase transition achieved in the metastable perovskite (ReNiO₃, where Re denotes a lanthanide rare-earth element) by using critical temperature, hydrogenation, electrical field and interfacial strain has attracted considerable attention in condensed matter physics and materials science, making it promising applications in the critical temperature thermistor, artificial intelligence, energy conversion and weak electric field sensing. Nevertheless, the above abundant applications are still bottlenecked by the intrinsically thermodynamic metastability related to ReNiO₃. Herein, we synthesize the atomic-level flat ReNiO₃ film material with thermodynamic metastability using laser molecular beam epitaxy (LMBE) that exhibits excellent thermally-driven electronic phase transitions. Notably, the interfacial heterogeneous nucleation of ReNiO₃ film can be triggered by the template effect of (001)-oriented LaAlO₃ substrates, owing to the similar lattice constants between LaAlO₃ substrate and ReNiO₃ film. In addition, we elucidate the key role of in situ annealing under oxygen-enriched atmosphere in stabilizing the distorted perovskite structure related to ReNiO₃. Apart from the depositing process related to LMBE, the ReNiO₃ with heavy rare-earth composition exhibits a more distorted NiO₆ octahedron and a higher Gibbs free energy that is rather difficult to synthesize by using physical vacuum deposition. As a representative case, the in situ annealing-assisted LMBE process cannot be utilized to deposit the SmNiO₃ film, in which the impurity peaks related to Re₂O₃ and NiO are observed in its XRD spectra. With the assistance of X-ray photoelectron spectraoscopy and near-edge X-ray absorption fine structure, the valence state of nickel for ReNiO₃ is found to be +3, and the $t_{2{\mathrm{g}}}^6e_{\mathrm{g}}^1 $ configuration is observed. Considering the highly tunable electronic orbital configuration of ReNiO₃ related to the NiO₆ octahedron, co-occupying the A-site of perovskite structure with Nd and Sm elements regulates the transition temperature (T_MIT) for ReNiO₃ within a broad temperature range. Furthermore, we demonstrate the anisotropy in the electronic phase transitions for Nd_1–xSm_xNiO₃, in which case the T_MIT achieved in the Nd_1–xSm_xNiO₃/LaAlO₃ (111) heterostructure exceeds the one deposited on the (001)-oriented LaAlO₃ substrate. The presently observed anisotropy in the electrical transportation for Nd_1–xSm_xNiO₃ film material is related to the anisotropic in-plane NiO₆ octahedron configuration triggered by differently oriented LaAlO₃ substrates. The present work is expected to introduce a new degree of freedom to regulate the electronic phase transition, explore new electronic phase in ReNiO₃ material system, and pave the way for growing atomic-level flat ReNiO₃ film materials with expected electronic phase transitions.

Keywords:

Authors and contacts

1.
Key Laboratory of Magnetic Molecules and Magnetic Information Materials of Ministry of Education, School of Chemistry and Materials Science, Shanxi Normal University, Taiyuan 030031, China
2.
Collaborative Innovation Center for Shanxi Advanced Permanent Magnetic Materials and Technology, Research Institute of Materials Science, Shanxi Normal University, Taiyuan 030031, China

Corresponding author: Zhou Xuan-Chi, xuanchizhou@sxnu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 52401240, 12174237) and the Open Project of Tianjin Key Laboratory of Optoelectronic Detection Technology and System, China (Grant No. 2024LODTS102).

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References

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[3]	Vistoli L, Wang W B, Sander A, Zhu Q X, Casals B, Cichelero R, Barthélémy A, Fusil S, Herranz G, Valencia S, Abrudan R, Weschke E, Nakazawa K, Kohno H, Santamaria J, Wu W D, Garcia V, Bibes M 2019 Nat. Phys. 15 67 Google Scholar
[4]	周轩弛, 李海帆 2024 73 117102 Google Scholar Zhou X C, Li H F 2024 Acta Phys. Sin. 73 117102 Google Scholar
[5]	Zhou X C, Shang Y L, Gu Z J, Jiang G Z, Ozawa T, Mao W, Fukutani K, Matsuzaki H, Jiang Y, Chen N F, Chen J K 2024 Appl. Phys. Lett. 124 082103 Google Scholar
[6]	Li D F, Lee K, Wang B Y, Osada M, Crossley S, Lee H R, Cui Y C, Hikita Y, Hwang H Y 2019 Nature 572 624 Google Scholar
[7]	Bisogni V, Catalano S, Green R J, Gibert M, Scherwitzl R, Huang Y B, Strocov V N, Zubko P, Balandeh S, Triscone J M, Sawatzky G, Schmitt T 2016 Nat. Commun. 7 13017 Google Scholar
[8]	Domínguez C, Georgescu A B, Mundet B, Zhang Y J, Fowlie J, Mercy A, Waelchli A, Catalano S, Alexander D T L, Ghosez P, Georges A, Millis A J, Gibert M, Triscone J M 2020 Nat. Mater. 19 1182 Google Scholar
[9]	Song Q, Doyle S, Pan G A, El Baggari I, Segedin D F, Carrizales D C, Nordlander J, Tzschaschel C, Ehrets J R, Hasan Z, El-Sherif H, Krishna J, Hanson C, LaBollita H, Bostwick A, Jozwiak C, Rotenberg E, Xu S Y, Lanzara A, N'Diaye A T, Heikes C A, Liu Y H, Paik H, Brooks C M, Pamuk B, Heron J T, Shafer P, Ratcliff W D, Botana A S, Moreschini L, Mundy J A 2023 Nat. Phys. 19 522 Google Scholar
[10]	Zhang H T, Park T J, Islam A, Tran D S J, Manna S, Wang Q, Mondal S, Yu H M, Banik S, Cheng S B, Zhou H, Gamage S, Mahapatra S, Zhu Y M, Abate Y, Jiang N, Sankaranarayanan S, Sengupta A, Teuscher C, Ramanathan S 2022 Science 375 533 Google Scholar
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[15]	Zhao W Y, Ma Z W, Shi Y, Fu R J, Wang K, Sui Y M, Xiao G J, Zou B 2023 Cell Rep. Phys. Sci. 4 101663 Google Scholar
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[21]	Zhou Y, Guan X F, Zhou H, Ramadoss K, Adam S, Liu H J, Lee S, Shi J, Tsuchiya M, Fong D D, Ramanathan S 2016 Nature 534 231 Google Scholar
[22]	Yang Z, Ko C, Ramanathan S 2011 Annu. Rev. Mater. Res. 41 337 Google Scholar
[23]	Mattoni G, Zubko P, Maccherozzi F, van der Torren A J H, Boltje D B, Hadjimichael M, Manca N, Catalano S, Gibert M, Liu Y, Aarts J, Triscone J M, Dhesi S S, Caviglia A D 2016 Nat. Commun. 7 13141 Google Scholar
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[27]	Zhou X C, Jiao Y J, Li H F 2024 Appl. Phys. Lett. 125 032103 Google Scholar
[28]	Schiffer P, Ramirez A P, Bao W, Cheong S W 1995 Phys. Rev. Lett. 75 3336 Google Scholar
[29]	Catalano S, Gibert M, Fowlie J, Iñiguez J, Triscone J M, Kreisel J 2018 Rep. Prog. Phys. 81 046501 Google Scholar
[30]	Nikulin I V, Novojilov M A, Kaul A R, Mudretsova S N, Kondrashov S V 2004 Mater. Res. Bull. 39 775 Google Scholar
[31]	Escote M T, da Silva A M L, Matos J R, Jardim R F 2000 J. Solid State Chem. 151 298 Google Scholar
[32]	Chen X G, Zhang X, Koten M A, Chen H H, Xiao Z Y, Zhang L, Shield J E, Dowben P A, Hong X 2017 Adv. Mater. 29 1701385 Google Scholar
[33]	Hadjimichael M, Mundet B, Domínguez C, Waelchli A, De Luca G, Spring J, Jöhr S, Walker S M, Piamonteze C, Alexander D T L, Triscone J M, Gibert M 2023 Adv. Electron. Mater. 9 2201182 Google Scholar
[34]	Demazeau G, Marbeuf A, Pouchard M, Hagenmuller P 1971 J. Solid State Chem. 3 582 Google Scholar
[35]	Chen J K, Li Z A, Dong H L, Xu J N, Wang V, Feng Z J, Chen Z Q, Chen B, Chen N F, Mao H K 2020 Adv. Funct. Mater. 30 2000987 Google Scholar
[36]	Chen J K, Hu H Y, Wang J O, Yajima T, Ge B H, Ke X Y, Dong H L, Jiang Y, Chen N F 2019 Mater. Horiz. 6 788 Google Scholar
[37]	Chen J H, Chen J K, Ren Z Y, Zhao D D, Wang M X, Miao J, Xu X G, Jiang Y, Chen N F 2021 J. Rare Earths 39 174 Google Scholar
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Cited By

图 1 稀土镍酸盐(ReNiO₃)的电子相变特性　(a) ReNiO₃的晶体结构及 ReNiO₃绝缘相的电子结构和扭曲的NiO₆八面体; (b) ReNiO₃的T_MIT随其扭曲钙钛矿结构容忍因子的变化; (c) 温度为1100 K时ReNiO₃的吉布斯自由能(ΔG)随稀土离子半径的变化

Figure 1. Electronic phase transitions for rare-earth nickelates (ReNiO₃): (a) Crystal structure for ReNiO₃ and the electronic structure and distorted NiO₆ octahedron for the insulating phase of ReNiO₃; (b) transition temperature (T_MIT) for ReNiO₃ plotted as a function of the tolerance factor of distorted perovskite structure; (c) Gibbs free energy (ΔG) for ReNiO₃ plotted as a function of the ionic radius of Re elements at 1100 K.

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图 2 揭示高氧压原位退火在沉积ReNiO₃薄膜中的关键作用　(a) 未经原位退火、经原位退火及放置空气中4个月后NdNiO₃的X射线衍射图谱(XRD); (b) 经原位退火NdNiO₃薄膜的原子力显微镜(AFM)图; (c) 原位退火、放置于空气中4个月及未经原位退火NdNiO₃的阻温特性曲线(ρ-T曲线); (d) 原位退火及未经原位退火NdNiO₃的电阻温度系数与温度的变化关系图(TCR -T曲线), 插图为本工作制备的NdNiO₃薄膜的归一化特性曲线与文献[36]的对比图

Figure 2. Revealing the critical role of in situ annealing upon high oxygen pressure in depositing the ReNiO₃ film material: (a) X-ray diffraction for the as-deposited NdNiO₃ film before and after in-situ annealing and exposed to the air for 4 months; (b) image of atomic force microscope for NdNiO₃ film upon in-situ annealing; (c) resistance temperature characteristic curves (ρ-T tendency) of NdNiO₃ after in-situ annealing, 4 months in air, and without in-situ annealing; (d) temperature dependance of the temperature coefficient of resistance (TCR) for the NdNiO₃ film before and after in-situ annealing, while the normalized ρ-T tendency for as-deposited NdNiO₃ film as compared for the previously reported one were shown in the inset ^[36].

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图 3 所制备NdNiO₃薄膜的X射线光电子能谱(XPS)　(a) Ni-2p核心能级, (b) O-1s核心能级. 所制备NdNiO₃薄膜的同步辐射X射线近边吸收谱(NEXAFS)　(c) Ni-L边, (d) O-K边

Figure 3. X-ray photoelectron spectroscopy (XPS) for NdNiO₃ film: (a) Ni-2p core-level peak; (b) O-1s core-level peak. Near-edge X-ray absorption fine structure (NEXAFS) for NdNiO₃ film: (c) Ni-L edge, (d) O-K edge.

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图 4 Nd_1–xSm_xNiO₃薄膜的晶体结构和电子相变特性　(a) Nd_1–xSm_xNiO₃ (x = 0, 0.25, 0.5) 薄膜的XRD图谱, 插图为Nd_1–xSm_xNiO₃ (x = 0.75, 1) 薄膜的XRD图谱; (b) Nd_1–xSm_xNiO₃ (x = 0, 0.25, 0.5) 薄膜c轴晶格参数随A位Sm元素共占据比例的变化关系图; (c) Nd_1–xSm_xNiO₃ (x = 0, 0.25)薄膜的阻温特性曲线; (d) Nd_1–xSm_xNiO₃ (x = 0, 0.25) 薄膜的相变温度随A位Sm元素共占据比例的变化关系图, 插图为Nd_1–xSm_xNiO₃ (x = 0, 0.25, 0.5) 薄膜的TCR-T曲线

Figure 4. Crystal structure and electronic phase transition for Nd_1–xSm_xNiO₃ film material: (a) The XRD spectra for as-deposited Nd_1–xSm_xNiO₃ films (x = 0, 0.25, 0.5), while the XRD spectra for as-deposited Nd_1–xSm_xNiO₃ films (x = 0.75, 1) was shown in the inset; (b) the c-axis lattice constant for Nd_1–xSm_xNiO₃ (x = 0, 0.25, 0.5) films plotted as a function of Sm substituting concentration; (c) the ρ-T tendency for Nd_1–xSm_xNiO₃ films (x = 0, 0.25); (d) T_MIT for as-grown Nd_1–xSm_xNiO₃ (x = 0, 0.25) films plotted as a function of Sm substituting concentration; while the TCR-T tendency as achieved in the Nd_1–xSm_xNiO₃ (x = 0, 0.25, 0.5) film was shown in the inset.

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图 5 Nd_1–xSm_xNiO₃电输运特性的各向异性　(a) 不同取向NdNiO₃薄膜的XRD图谱; (b)不同取向 NdNiO₃的归一化阻温特性曲线; (c) NdNiO₃相变温度随晶体学取向的变化关系图, 插图中为NdNiO₃/LAO(111)异质结的AFM图; (d) 不同取向Nd_1–xSm_xNiO₃薄膜的归一化阻温特性曲线, 插图为其XRD图谱

Figure 5. Anisotropy in the electrical transport properties for Nd_1–xSm_xNiO₃: (a) XRD spectra for differently oriented NdNiO₃ films; (b) the normalized ρ-T tendency for differently oriented NdNiO₃ films; (c) T_MIT for NdNiO₃ films plotted as a function of crystallographic orientation, while the respective AFM spectra of NdNiO₃/LAO (111) heterostructure was shown in the inset; (d) the normalized ρ-T tendency for differently oriented Nd_1–xSm_xNiO₃ films, while the respective XRD spectra are shown in the inset.

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map

[1]	Ding X, Tam C C, Sui X L, Zhao Y, Xu M H, Choi J, Leng H Q, Zhang J, Wu M, Xiao H Y, Zu X T, Garcia-Fernandez M, Agrestini S, Wu X Q, Wang Q Y, Gao P, Li S A, Huang B, Zhou K J, Qiao L 2023 Nature 615 50 Google Scholar
[2]	Jeong J, Aetukuri N, Graf T, Schladt T D, Samant M G, Parkin S S 2013 Science 339 1402 Google Scholar
[3]	Vistoli L, Wang W B, Sander A, Zhu Q X, Casals B, Cichelero R, Barthélémy A, Fusil S, Herranz G, Valencia S, Abrudan R, Weschke E, Nakazawa K, Kohno H, Santamaria J, Wu W D, Garcia V, Bibes M 2019 Nat. Phys. 15 67 Google Scholar
[4]	周轩弛, 李海帆 2024 73 117102 Google Scholar Zhou X C, Li H F 2024 Acta Phys. Sin. 73 117102 Google Scholar
[5]	Zhou X C, Shang Y L, Gu Z J, Jiang G Z, Ozawa T, Mao W, Fukutani K, Matsuzaki H, Jiang Y, Chen N F, Chen J K 2024 Appl. Phys. Lett. 124 082103 Google Scholar
[6]	Li D F, Lee K, Wang B Y, Osada M, Crossley S, Lee H R, Cui Y C, Hikita Y, Hwang H Y 2019 Nature 572 624 Google Scholar
[7]	Bisogni V, Catalano S, Green R J, Gibert M, Scherwitzl R, Huang Y B, Strocov V N, Zubko P, Balandeh S, Triscone J M, Sawatzky G, Schmitt T 2016 Nat. Commun. 7 13017 Google Scholar
[8]	Domínguez C, Georgescu A B, Mundet B, Zhang Y J, Fowlie J, Mercy A, Waelchli A, Catalano S, Alexander D T L, Ghosez P, Georges A, Millis A J, Gibert M, Triscone J M 2020 Nat. Mater. 19 1182 Google Scholar
[9]	Song Q, Doyle S, Pan G A, El Baggari I, Segedin D F, Carrizales D C, Nordlander J, Tzschaschel C, Ehrets J R, Hasan Z, El-Sherif H, Krishna J, Hanson C, LaBollita H, Bostwick A, Jozwiak C, Rotenberg E, Xu S Y, Lanzara A, N'Diaye A T, Heikes C A, Liu Y H, Paik H, Brooks C M, Pamuk B, Heron J T, Shafer P, Ratcliff W D, Botana A S, Moreschini L, Mundy J A 2023 Nat. Phys. 19 522 Google Scholar
[10]	Zhang H T, Park T J, Islam A, Tran D S J, Manna S, Wang Q, Mondal S, Yu H M, Banik S, Cheng S B, Zhou H, Gamage S, Mahapatra S, Zhu Y M, Abate Y, Jiang N, Sankaranarayanan S, Sengupta A, Teuscher C, Ramanathan S 2022 Science 375 533 Google Scholar
[11]	Shi J, Zhou Y, Ramanathan S 2014 Nat. Commun. 5 4860 Google Scholar
[12]	Shi J, Ha S D, Zhou Y, Schoofs F, Ramanathan S 2013 Nat. Commun. 4 2676 Google Scholar
[13]	Scherwitzl R, Zubko P, Lezama I G, Ono S, Morpurgo A F, Catalan G, Triscone J M 2010 Adv. Mater. 22 5517 Google Scholar
[14]	Phillips P J, Rui X, Georgescu A B, Disa A S, Longo P, Okunishi E, Walker F, Ahn C H, Ismail-Beigi S, Klie R F 2017 Phys. Rev. B 95 205131 Google Scholar
[15]	Zhao W Y, Ma Z W, Shi Y, Fu R J, Wang K, Sui Y M, Xiao G J, Zou B 2023 Cell Rep. Phys. Sci. 4 101663 Google Scholar
[16]	Zhao D L, Cong M, Liu Z, Ma Z W, Wang K, Xiao G J, Zou B 2023 Cell Rep. Phys. Sci. 4 101445 Google Scholar
[17]	Shi Y, Zhao W Y, Ma Z W, Xiao G J, Zou B 2021 Chem. Sci. 12 14711 Google Scholar
[18]	Zhou X C, Li H F, Jiao Y J, Zhou G W, Ji H H, Jiang Y, Xu X H 2024 Adv. Funct. Mater. 34 2316536 Google Scholar
[19]	Zhang H T, Park T J, Zaluzhnyy I A, Wang Q, Wadekar S N, Manna S, Andrawis R, Sprau P O, Sun Y F, Zhang Z, Huang C Z, Zhou H, Zhang Z, Narayanan B, Srinivasan G, Hua N, Nazaretski E, Huang X J, Yan H F, Ge M Y, Chu Y S, Cherukara M J, Holt M V, Krishnamurthy M, Shpyrko O G, Sankaranarayanan S, Frano A, Roy K, Ramanathan S 2020 Nat. Commun. 11 2245 Google Scholar
[20]	Zhang Z, Schwanz D, Narayanan B, Kotiuga M, Dura J A, Cherukara M, Zhou H, Freeland J W, Li J R, Sutarto R, He F Z, Wu C Z, Zhu J X, Sun Y F, Ramadoss K, Nonnenmann S S, Yu N F, Comin R, Rabe K M, Sankaranarayanan S, Ramanathan S 2018 Nature 553 68 Google Scholar
[21]	Zhou Y, Guan X F, Zhou H, Ramadoss K, Adam S, Liu H J, Lee S, Shi J, Tsuchiya M, Fong D D, Ramanathan S 2016 Nature 534 231 Google Scholar
[22]	Yang Z, Ko C, Ramanathan S 2011 Annu. Rev. Mater. Res. 41 337 Google Scholar
[23]	Mattoni G, Zubko P, Maccherozzi F, van der Torren A J H, Boltje D B, Hadjimichael M, Manca N, Catalano S, Gibert M, Liu Y, Aarts J, Triscone J M, Dhesi S S, Caviglia A D 2016 Nat. Commun. 7 13141 Google Scholar
[24]	Zhou X C, Li H F, Meng F Q, Mao W, Wang J O, Jiang Y, Fukutani K, Wilde M, Fugetsu B, Sakata I, Chen N F, Chen J K 2022 J. Phys. Chem. Lett. 13 8078 Google Scholar
[25]	Zhou X C, Cui Y C, Shang Y L, Li H F, Wang J O, Meng Y, Xu X, Jiang Y, Chen N F, Chen J K 2023 J. Phys. Chem. C 127 2639 Google Scholar
[26]	Zhou X C, Li H F, Shang Y L, Meng F Q, Li Z A, Meng K K, Wu Y, Xu X G, Jiang Y, Chen N F, Chen J K 2023 Phys. Chem. Chem. Phys. 25 21908 Google Scholar
[27]	Zhou X C, Jiao Y J, Li H F 2024 Appl. Phys. Lett. 125 032103 Google Scholar
[28]	Schiffer P, Ramirez A P, Bao W, Cheong S W 1995 Phys. Rev. Lett. 75 3336 Google Scholar
[29]	Catalano S, Gibert M, Fowlie J, Iñiguez J, Triscone J M, Kreisel J 2018 Rep. Prog. Phys. 81 046501 Google Scholar
[30]	Nikulin I V, Novojilov M A, Kaul A R, Mudretsova S N, Kondrashov S V 2004 Mater. Res. Bull. 39 775 Google Scholar
[31]	Escote M T, da Silva A M L, Matos J R, Jardim R F 2000 J. Solid State Chem. 151 298 Google Scholar
[32]	Chen X G, Zhang X, Koten M A, Chen H H, Xiao Z Y, Zhang L, Shield J E, Dowben P A, Hong X 2017 Adv. Mater. 29 1701385 Google Scholar
[33]	Hadjimichael M, Mundet B, Domínguez C, Waelchli A, De Luca G, Spring J, Jöhr S, Walker S M, Piamonteze C, Alexander D T L, Triscone J M, Gibert M 2023 Adv. Electron. Mater. 9 2201182 Google Scholar
[34]	Demazeau G, Marbeuf A, Pouchard M, Hagenmuller P 1971 J. Solid State Chem. 3 582 Google Scholar
[35]	Chen J K, Li Z A, Dong H L, Xu J N, Wang V, Feng Z J, Chen Z Q, Chen B, Chen N F, Mao H K 2020 Adv. Funct. Mater. 30 2000987 Google Scholar
[36]	Chen J K, Hu H Y, Wang J O, Yajima T, Ge B H, Ke X Y, Dong H L, Jiang Y, Chen N F 2019 Mater. Horiz. 6 788 Google Scholar
[37]	Chen J H, Chen J K, Ren Z Y, Zhao D D, Wang M X, Miao J, Xu X G, Jiang Y, Chen N F 2021 J. Rare Earths 39 174 Google Scholar
[38]	Zhou X C, Wu Y, Yan F B, Zhang T Z, Ke X Y, Meng K K, Xu X G, Li Z P, Miao J, Chen J K, Jiang Y 2021 Ceram. Int. 47 25574 Google Scholar
[39]	Catalan G 2008 Phase Transit. 81 729 Google Scholar
[40]	Zhou X C, Mao W, Cui Y C, Zhang H, Liu Q, Nie K Q, Xu X G, Jiang Y, Chen N F, Chen J K 2023 Adv. Funct. Mater. 33 2303416 Google Scholar
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Vol. 73, Issue 19 - 2024-10-05

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