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Back-End-of-Line-Compatible Passivation of Sulfur Vacancies in MoS2 Transistors Using Electron-Withdrawing Benzenethiol

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    Back-End-of-Line-Compatible Passivation of Sulfur Vacancies in MoS2 Transistors Using Electron-Withdrawing Benzenethiol
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    • Haksoon Jung
      Haksoon Jung
      Department of Electrical Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-Gil, Eonyang-Eup, Ulju-Gun, Ulsan 44919, Republic of Korea
      Department of Chemical Engineering, Pohang University of Science and Technology (POSTECH), 77 Cheongam-Ro, Nam-Gu, Pohang 37673, Republic of Korea
      More by Haksoon Jung
      Orcidhttps://orcid.org/0000-0003-1567-692X
    • Mingyu Kim
      Mingyu Kim
      Department of Chemical Engineering, Pohang University of Science and Technology (POSTECH), 77 Cheongam-Ro, Nam-Gu, Pohang 37673, Republic of Korea
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    • Yongwoo Lee
      Yongwoo Lee
      Department of Electrical Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-Gil, Eonyang-Eup, Ulju-Gun, Ulsan 44919, Republic of Korea
      More by Yongwoo Lee
      Orcidhttps://orcid.org/0000-0002-9367-0235
    • Gi Beom Sim
      Gi Beom Sim
      Department of Energy Science, Sungkyunkwan University (SKKU), 2066 Seobu-Ro, Jangan-Gu, Suwon Gyeonggi-Do 16419, Republic of Korea
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    • Hyeonho Gu
      Hyeonho Gu
      Department of Electrical Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-Gil, Eonyang-Eup, Ulju-Gun, Ulsan 44919, Republic of Korea
      More by Hyeonho Gu
    • Sumin Hong
      Sumin Hong
      Graduate School of Semiconductor Materials and Devices Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-Gil, Eonyang-Eup, Ulju-Gun, Ulsan 44919, Republic of Korea
      More by Sumin Hong
    • Sanghyun Lee
      Sanghyun Lee
      Department of Electrical Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-Gil, Eonyang-Eup, Ulju-Gun, Ulsan 44919, Republic of Korea
      More by Sanghyun Lee
    • Jaehyun Lee
      Jaehyun Lee
      Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-Ro, Yuseong-Gu, Daejeon 34141, Republic of Korea
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    • Donghyeop Lee
      Donghyeop Lee
      Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-Ro, Yuseong-Gu, Daejeon 34141, Republic of Korea
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    • Taoyu Zou
      Taoyu Zou
      Department of Chemical Engineering, Pohang University of Science and Technology (POSTECH), 77 Cheongam-Ro, Nam-Gu, Pohang 37673, Republic of Korea
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      Orcidhttps://orcid.org/0000-0003-4477-051X
    • Kibum Kang
      Kibum Kang
      Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-Ro, Yuseong-Gu, Daejeon 34141, Republic of Korea
      More by Kibum Kang
      Orcidhttps://orcid.org/0000-0003-1674-1826
    • Chang Woo Myung
      Chang Woo Myung
      Department of Energy Science, Sungkyunkwan University (SKKU), 2066 Seobu-Ro, Jangan-Gu, Suwon Gyeonggi-Do 16419, Republic of Korea
      Center for 2D Quantum Heterostructures, Institute for Basic Science (IBS), 2066 Seobu-Ro, Jangan-Gu, Suwon, Gyeonggi-Do 16419, Republic of Korea
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      Orcidhttps://orcid.org/0000-0002-9480-6982
    • Yong-Young Noh*
      Yong-Young Noh
      Department of Chemical Engineering, Pohang University of Science and Technology (POSTECH), 77 Cheongam-Ro, Nam-Gu, Pohang 37673, Republic of Korea
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0001-7222-2401
    • Jimin Kwon*
      Jimin Kwon
      Department of Electrical Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-Gil, Eonyang-Eup, Ulju-Gun, Ulsan 44919, Republic of Korea
      Graduate School of Semiconductor Materials and Devices Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-Gil, Eonyang-Eup, Ulju-Gun, Ulsan 44919, Republic of Korea
      *Email: [email protected]
      More by Jimin Kwon
      Orcidhttps://orcid.org/0000-0002-5213-1323
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    ACS Nano

    Cite this: ACS Nano 2025, 19, 6, 6069–6078
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    https://doi.org/10.1021/acsnano.4c12927
    Published February 3, 2025
    Copyright © 2025 American Chemical Society
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    Abstract

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    Atomically thin two-dimensional semiconductor molybdenum disulfide (MoS2) is considered an ideal n-type channel material for field-effect transistors (FETs) due to its immunity to short-channel effects by dangling bond-free surface. However, sulfur atom dissociation or nonideal film deposition can easily lead to sulfur vacancies (SVs) in the MoS2 film. These crystal imperfections create defects in the electronic structure, thereby limiting the utility of this promising material. We introduce an electron-withdrawing benzenethiol (BT) to repair the vacancies with the exact missing atoms at 200°C─marking the lowest process temperature for complete SV repair. These thiol groups actively and selectively bond with the vacant sites due to their self-assembly nature. Notably, we found that the fluorination of BT weakens the S–C bond as the BT withdraws electrons from the sulfur side. This enables a low-temperature annealing process to detach the headgroups from the MoS2 surface. The atomic ratio of MoS2 was recovered from 1.68 to 1.98, leading to an ideal subthreshold swing of MoS2 FETs 62.5 mV·dec–1. The proposed SV repair process, repeatedly applicable between fabrication steps for its low process temperature, unveils the potential of the BEOL MoS2 FETs with a nearly ideal atomic ratio adhering to their thermal budget.

    Copyright © 2025 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/acsnano.4c12927.

    • UV–vis of electrochemical-exfoliated 2H-phase MoS2 solution; molecular geometric information for transition state calculation; XPS deconvolution with exponential fitting; XPS spectra of the as-exfoliated MoS2 after thermal annealing; Raman spectra of MoS2 with SV passivation and thermal annealing; AFM images of Al2O3 grown on MoS2; cycling test of ion-gated MoS2 FET; EIS analysis; electrical characteristics of MoS2 single flake transistor fabricated on 100 nm SiO2 substrate; electrical characterization of ML-MOCVD MoS2; DFT calculations; spectrum deconvolutions of XPS data, atomic ratio calculation method; optical microscope identification of MoS2 flake; I–V curves for raw data; and tables for fitting parameters of fitting XPS results and comparison on other studies (PDF)

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    1. Ziyang Shen, Rıdvan Küçükosman, Zhongdong Liang, Bao Yang, Ashwani K. Gupta. Effects of Atomic Layer Deposition-Alumina on Moisture Resistance Properties of Yttria-Stabilized Zirconia Thermal Barrier Coatings in Hydrogen Enriched Flame. Journal of Energy Resources Technology, Part A: Sustainable and Renewable Energy 2025, 1 (4) https://doi.org/10.1115/1.4068140
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    ACS Nano

    Cite this: ACS Nano 2025, 19, 6, 6069–6078
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.4c12927
    Published February 3, 2025
    Copyright © 2025 American Chemical Society
    Request reuse permissions

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