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Novel Approach to High κ (∼59) and Low EOT (∼3.8 Å) near the Morphotrophic Phase Boundary with AFE/FE (ZrO2/HZO) Bilayer Heterostructures and High-Pressure Annealing

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Download Hi-Res ImageDownload to MS-PowerPointCite This:ACS Appl. Mater. Interfaces 2022, 14, 38, 43463-43473
    Functional Inorganic Materials and Devices

    Novel Approach to High κ (∼59) and Low EOT (∼3.8 Å) near the Morphotrophic Phase Boundary with AFE/FE (ZrO2/HZO) Bilayer Heterostructures and High-Pressure Annealing
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    • Venkateswarlu Gaddam
      Venkateswarlu Gaddam
      School of Electrical Engineering, Korea Advanced Institute of Science & Technology, Daejeon 34141, Korea
      More by Venkateswarlu Gaddam
    • Giuk Kim
      Giuk Kim
      School of Electrical Engineering, Korea Advanced Institute of Science & Technology, Daejeon 34141, Korea
      More by Giuk Kim
    • Taeho Kim
      Taeho Kim
      School of Electrical Engineering, Korea Advanced Institute of Science & Technology, Daejeon 34141, Korea
      More by Taeho Kim
    • Minhyun Jung
      Minhyun Jung
      School of Electrical Engineering, Korea Advanced Institute of Science & Technology, Daejeon 34141, Korea
      More by Minhyun Jung
    • Chaeheon Kim
      Chaeheon Kim
      School of Electrical Engineering, Korea Advanced Institute of Science & Technology, Daejeon 34141, Korea
      More by Chaeheon Kim
    • Sanghun Jeon*
      Sanghun Jeon
      School of Electrical Engineering, Korea Advanced Institute of Science & Technology, Daejeon 34141, Korea
      *email: [email protected]
      More by Sanghun Jeon
      Orcidhttps://orcid.org/0000-0002-7995-6640
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2022, 14, 38, 43463–43473
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    https://doi.org/10.1021/acsami.2c08691
    Published September 15, 2022
    Copyright © 2022 American Chemical Society
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    Abstract

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    We present herewith a novel approach of equally thick AFE/FE (ZrO2/HZO) bilayer stack heterostructure films for achieving an equivalent oxide thickness (EOT) of 4.1 Å with a dielectric constant (κ) of 56 in complementary metal-oxide semiconductor (CMOS) compatible metal–ferroelectric–metal (MFM) capacitors using a high-pressure annealing (HPA) technique. The low EOT and high κ values were achieved by careful optimization of AFE/FE film thicknesses and HPA conditions near the morphotropic phase boundary (MPB) after field cycling effects. Stable leakage current density (J < 10–7 A/cm2 at ±0.8 V) was found at 3/3 nm bilayer stack films (κ = 56 and EOT = 4.1 Å) measured at room temperature. In comparison with previous work, our remarkable achievement stems from the interfacial coupling between FE and AFE films as well as a high-quality crystalline structure formed by HPA. Kinetically stabilized hafnia films result in a small grain size in bilayer films, leading to reducing the leakage current density. Further, a higher κ value of 59 and lower EOT of 3.4 Å were found at 333 K. However, stable leakage current density was found at 273 K with a high κ value of 53 and EOT of 3.85 Å with J < 10–7 A/cm2. This is the lowest recorded EOT employing hafnia and TiN electrodes that are compatible with CMOS, and it has important implications for future dynamic random access memory (DRAM) technology.

    Copyright © 2022 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.2c08691.

    • P–E curves for the various bilayer heterostructure films at different field cycles; C–E curves for the various bilayer heterostructure films at different field cycles; J–V curves for the bilayer devices annealed at HPA 400 and 500 °C; TEM images for thickness-dependent ZrO2 films; C–E curves for 20 bilayer capacitors and cumulative plots at various annealing temperatures (PDF)

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    Cited By

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    This article is cited by 5 publications.

    1. Hyojun Choi, Yong Hyeon Cho, Se Hyun Kim, Kun Yang, Min Hyuk Park. Hafnia-Based Ferroelectric Memory: Device Physics Strongly Correlated with Materials Chemistry. The Journal of Physical Chemistry Letters 2024, 15 (4) , 983-997. https://doi.org/10.1021/acs.jpclett.3c03363
    2. Geun Hyeong Park, Dong Hyun Lee, Hyojun Choi, Taegyu Kwon, Yong Hyeon Cho, Se Hyun Kim, Min Hyuk Park. Emerging Fluorite-Structured Antiferroelectrics and Their Semiconductor Applications. ACS Applied Electronic Materials 2023, 5 (2) , 642-663. https://doi.org/10.1021/acsaelm.2c01615
    3. Da Hee Hong, Jae Hoon Yoo, Won Ji Park, So Won Kim, Jong Hwan Kim, Sae Hoon Uhm, Hee Chul Lee. Characteristics of Hf0.5Zr0.5O2 Thin Films Prepared by Direct and Remote Plasma Atomic Layer Deposition for Application to Ferroelectric Memory. Nanomaterials 2023, 13 (5) , 900. https://doi.org/10.3390/nano13050900
    4. Seung Won Lee, Min Ji Jeong, Youkyoung Oh, Hyo-Bae Kim, Tae-Eon Park, Ji-Hoon Ahn. Enhanced dielectric and energy storage performances of Hf0.6Zr0.4O2 thin films by Al doping. Ceramics International 2023, 1 https://doi.org/10.1016/j.ceramint.2023.02.173
    5. Yeongseok Jeong, Venkateswarlu Gaddam, Youngin Goh, Hunbeom Shin, Sangho Lee, Giuk Kim, Sanghun Jeon. Oxygen Vacancy Control as a Strategy to Enhance Imprinting Effect in Hafnia Ferroelectric Devices. IEEE Transactions on Electron Devices 2023, 70 (1) , 354-359. https://doi.org/10.1109/TED.2022.3223886
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2022, 14, 38, 43463–43473
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.2c08691
    Published September 15, 2022
    Copyright © 2022 American Chemical Society
    Request reuse permissions

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