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Ion Migration Studies in Exfoliated 2D Molybdenum Oxide via Ionic Liquid Gating for Neuromorphic Device Applications

  • Cheng Zhang
    Cheng Zhang
    Department of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    More by Cheng Zhang
  • Pushpa R. Pudasaini
    Pushpa R. Pudasaini
    Department of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Akinola D. Oyedele
    Akinola D. Oyedele
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    Bredesen Center for Interdisciplinary Research and Graduate Education, University of Tennessee, Knoxville, Tennessee 37996, United States
  • Anton V. Ievlev
    Anton V. Ievlev
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Liubin Xu
    Liubin Xu
    Department of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States
    More by Liubin Xu
  • Amanda V. Haglund
    Amanda V. Haglund
    Department of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States
  • Joo Hyon Noh
    Joo Hyon Noh
    Department of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States
    More by Joo Hyon Noh
  • Anthony T. Wong
    Anthony T. Wong
    Department of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States
  • Kai Xiao
    Kai Xiao
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    More by Kai Xiao
  • Thomas Z. Ward
    Thomas Z. Ward
    Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • David G. Mandrus
    David G. Mandrus
    Department of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States
    Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • Haixuan Xu
    Haixuan Xu
    Department of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States
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  • Olga S. Ovchinnikova
    Olga S. Ovchinnikova
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
  • , and 
  • Philip D. Rack*
    Philip D. Rack
    Department of Materials Science and Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States
    Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    *E-mail [email protected] (P.D.R.).
Cite this: ACS Appl. Mater. Interfaces 2018, 10, 26, 22623–22631
Publication Date (Web):June 11, 2018
https://doi.org/10.1021/acsami.8b05577
Copyright © 2018 American Chemical Society

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Supporting Info (1)»

Abstract

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The formation of an electric double layer in ionic liquid (IL) can electrostatically induce charge carriers and/or intercalate ions in and out of the lattice which can trigger a large change of the electronic, optical, and magnetic properties of materials and even modify the crystal structure. We present a systematic study of ionic liquid gating of exfoliated 2D molybdenum trioxide (MoO3) devices and correlate the resultant electrical properties to the electrochemical doping via ion migration during the IL biasing process. A nearly 9 orders of magnitude modulation of the MoO3 conductivity is obtained for the two types of ionic liquids that are investigated. In addition, notably rapid on/off switching was realized through a lithium-containing ionic liquid whereas much slower modulation was induced via oxygen extraction/intercalation. Time of flight–secondary ion mass spectrometry confirms the Li intercalation. Density functional theory (DFT) calculations have been carried out to examine the underlying metallization mechanism. Results of short-pulse tests show the potential of these MoO3 devices as neuromorphic computing elements due to their synaptic plasticity.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsami.8b05577.

  • Supplementary figures and the corresponding descriptions, including microscopic images, Raman spectra results, XRD results, and additional ToF-SIMS and DFT analysis (PDF)

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Cited By

This article is cited by 12 publications.

  1. Masahito Morita, Satoshi Toyoda, Hisao Kiuchi, Takeshi Abe, Kazuhiro Kumagai, Takahiro Saida, Katsutoshi Fukuda. Chromogenic Amorphous MoO3–x Nanosheets and Their Nanostructured Films for Smart Window Applications. ACS Applied Nano Materials 2021, 4 (9) , 8781-8788. https://doi.org/10.1021/acsanm.1c01428
  2. Cheng Zhang, Wei Zhao, Sheng Bi, Christopher M. Rouleau, Jason D. Fowlkes, Walker L. Boldman, Genda Gu, Qiang Li, Guang Feng, Philip D. Rack. Low-Temperature Charging Dynamics of the Ionic Liquid and Its Gating Effect on FeSe0.5Te0.5 Superconducting Films. ACS Applied Materials & Interfaces 2019, 11 (19) , 17979-17986. https://doi.org/10.1021/acsami.9b02373
  3. Mohit Kumar, Sohail Abbas, Joondong Kim. All-Oxide-Based Highly Transparent Photonic Synapse for Neuromorphic Computing. ACS Applied Materials & Interfaces 2018, 10 (40) , 34370-34376. https://doi.org/10.1021/acsami.8b10870
  4. Xiao Liu, Shijie Huang, Kun Wang, Yue Wang, Lei Yin, Deren Yang, Xiaodong Pi. An Array of Light‐Stimulated Two‐Terminal Synaptic Devices with the Modulation of Electric Polarity. Advanced Functional Materials 2023, 33 (9) , 2211394. https://doi.org/10.1002/adfm.202211394
  5. Noushin Raeisi Kheirabadi, Alessandro Chiolerio, Konrad Szaciłowski, Andrew Adamatzky. Neuromorphic Liquids, Colloids, and Gels: A Review. ChemPhysChem 2023, 24 (1) https://doi.org/10.1002/cphc.202200390
  6. Jing‐Kai Qin, Bing‐Xuan Zhu, Cong Wang, Cheng‐Yi Zhu, Ruo‐Yao Sun, Liang Zhen, Yang Chai, Cheng‐Yan Xu. Heterosynaptic Plasticity Achieved by Highly Anisotropic Ionic Migration in Layered Li x MoO 3 for Neuromorphic Application. Advanced Electronic Materials 2022, 12 , 2200721. https://doi.org/10.1002/aelm.202200721
  7. Zirui Zhang, Dongliang Yang, Huihan Li, Ce Li, Zhongrui Wang, Linfeng Sun, Heejun Yang. 2D materials and van der Waals heterojunctions for neuromorphic computing. Neuromorphic Computing and Engineering 2022, https://doi.org/10.1088/2634-4386/ac8a6a
  8. Jingu Kang, Young‐Woo Jang, Sang Hee Moon, Youngjin Kang, Jaehyun Kim, Yong‐Hoon Kim, Sung Kyu Park. Symmetrically Ion‐Gated In‐Plane Metal‐Oxide Transistors for Highly Sensitive and Low‐Voltage Driven Bioelectronics. Advanced Science 2022, 9 (13) , 2103275. https://doi.org/10.1002/advs.202103275
  9. Xiaoxia Wang, Fanfan Du, Yingmei Zhang, Jie Yang, Xiaoli Li, Xiaohong Xu. Manipulating the optical and electronic properties of MoO 3 films through electric-field-induced ion migration. Journal of Materials Chemistry C 2021, 10 (1) , 135-141. https://doi.org/10.1039/D1TC04659D
  10. Xin Shan, Fang Wang, Kai Hu, Jun-Qing Wei, Xin Lin, Xuan-Yu Zhao, Bao-Zeng Zhou, Kai-Liang Zhang. Recent advances in synthesis and memory computing of large-area <i>α</i>-MoO<sub>3</sub>. Acta Physica Sinica 2021, 70 (9) , 098103. https://doi.org/10.7498/aps.70.20201813
  11. Shilei Dai, Yiwei Zhao, Yan Wang, Junyao Zhang, Lu Fang, Shu Jin, Yinlin Shao, Jia Huang. Recent Advances in Transistor‐Based Artificial Synapses. Advanced Functional Materials 2019, 29 (42) , 1903700. https://doi.org/10.1002/adfm.201903700
  12. Walker L. Boldman, Cheng Zhang, Thomas Z. Ward, Dayrl P. Briggs, Bernadeta R. Srijanto, Philip Brisk, Philip D. Rack. Programmable Electrofluidics for Ionic Liquid Based Neuromorphic Platform. Micromachines 2019, 10 (7) , 478. https://doi.org/10.3390/mi10070478

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