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Low Temperature Nanoscale Oxygen-Ion Intercalation into Epitaxial MoO2 Thin Films

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Department of Physics, Pusan National University, Busan, 46241, Korea
Pohang Accelerator Laboratory, Pohang University of Science and Technology, Pohang, 37673, Korea
Department of Naval Architecture and Ocean Engineering, Pusan National University, Busan, 46241, Korea
§ Conversion Materials Laboratory, Energy Materials and Process Research Division, Korea Institute of Energy Research, Daejeon, 34129, Korea
*(H.J.) E-mail: [email protected]
Cite this: J. Phys. Chem. C 2017, 121, 6, 3410–3415
Publication Date (Web):January 24, 2017
https://doi.org/10.1021/acs.jpcc.6b11959
Copyright © 2017 American Chemical Society

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    Abstract

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    In transition metal oxides (TMOs), lots of physical phenomena such as metal–insulator transitions (MIT), magnetism, and ferroelectricity are closely related to the amounts of oxygen contents. Thus, understanding surface oxidation process in TMOs and its effect are important for enhancing performances of modern electronic and electrochemical devices due to miniaturization of those devices. In this regard, MoO2+x (0 ≤ x ≤ 1) is an interesting TMO, which shows MIT driven by the change of its oxygen content, i.e. metallic MoO2 and insulating MoO3. Hence, understanding thermally driven oxygen intercalation into MoO2 is very important. In this work, we conducted in situ postannealing of as-grown epitaxial MoO2 thin films at different temperatures in oxidative condition to investigate the thermal effect on oxygen ion intercalation and resultant MIT in MoO2+x. Through the spectroscopic techniques such as spectroscopic ellipsometry and X-ray absorption spectroscopy, we observed that oxygen ions can intercalate into MoO2 and trigger a phase transition in nanoscale at surprisingly low-temperature as low as 250 °C. In addition, after oxygen annealing at 350 °C, we find that both hybridization and interband transition energy between O 2p and Mo 4d t2g are significantly shifted to low energy nearly 0.2 eV, which clearly supports that the electronic transition of MoO2+x is predominantly driven by change of oxygen contents.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpcc.6b11959.

    • X-ray diffraction patterns, optical conductivity of MoO3, O K-edge TFY spectra, reconstruction of TFY spectrum of the MoO2+x film annealed at 250 °C, and evidence of full oxidation in the 25-nm-thick MoO2 thin films (PDF)

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    Cited By

    This article is cited by 8 publications.

    1. Jongbeom Lee, Jinyoung Jeong, Hyowon Lee, Jaesoung Park, Jinman Jang, Haguk Jeong. Effects of Sintering Processes on Microstructure Evolution, Crystallite, and Grain Growth of MoO2 Powder. Crystals 2023, 13 (9) , 1311. https://doi.org/10.3390/cryst13091311
    2. Vipin Kumar, Rajneesh Kumar Mishra, Pushpendra Kumar, Le Gia Trung, Jin Seog Gwag. Strong anisotropic optical response in two-dimensional Mo-VIA and Mo-VIIA monolayer binary materials. Photonics and Nanostructures - Fundamentals and Applications 2023, 53 , 101114. https://doi.org/10.1016/j.photonics.2023.101114
    3. Youngkyoung Ha, Shinbuhm Lee. Stable Correlated 4d 2 SrMoO 3 Films Epitaxially Coated on Al 2 O 3 for Electromagnetic Shielding and Transparent Conductors. Advanced Materials Interfaces 2022, 9 (31) https://doi.org/10.1002/admi.202200893
    4. H. H. Afify, S. A. Hassan, Badawi Anis, A. Abouelsayed. Effect of UV light illumination in humid air on the optical and electronic properties of the orthorhombic α -MoO3 and monoclinic β -MoO3. Journal of Applied Physics 2022, 132 (7) https://doi.org/10.1063/5.0095295
    5. Hao Tan, Qianqian Ji, Chao Wang, Hengli Duan, Yuan Kong, Yao Wang, Sihua Feng, Liyang Lv, Fengchun Hu, Wenhua Zhang, Wangsheng Chu, Zhihu Sun, Wensheng Yan. Asymmetrical π back-donation of hetero-dicationic Mo4+-Mo6+ pairs for enhanced electrochemical nitrogen reduction. Nano Research 2022, 15 (4) , 3010-3016. https://doi.org/10.1007/s12274-021-3934-6
    6. Xiaochi Liu, Deshun Qu, Lu Wang, Ming Huang, Yahua Yuan, Peng Chen, Yuanyuan Qu, Jian Sun, Won Jong Yoo. Charge Density Depinning in Defective MoTe 2 Transistor by Oxygen Intercalation. Advanced Functional Materials 2020, 30 (50) https://doi.org/10.1002/adfm.202004880
    7. Hyeonjun Kong, Han Sol Kwon, Hyegyeong Kim, Gwang-Soo Jeen, Jaekwang Lee, Joonhyuk Lee, Yun Seok Heo, Jinhyung Cho, Hyoungjeen Jeen. Reductive-annealing-induced changes in Mo valence states on the surfaces of MoO3 single crystals and their high temperature transport. Current Applied Physics 2019, 19 (12) , 1379-1382. https://doi.org/10.1016/j.cap.2019.09.001
    8. Eunyoung Ahn, Taewon Min, Jaekwang Lee, Inwon Lee, Younghak Kim, Hyoungjeen Jeen. Role of surface oxidation for thickness-driven insulator-to-metal transition in epitaxial MoO2 films. Applied Surface Science 2018, 459 , 92-97. https://doi.org/10.1016/j.apsusc.2018.07.188

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