Gas-phase Synthesis of Semiconducting Single-walled Carbon Nanotubes for Advanced Electronics

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School of Science | Doctoral thesis (article-based) | Defence date: 2025-01-17
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Date

2024

Department

Teknillisen fysiikan laitos
Department of Applied Physics

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Mcode

Degree programme

Language

en

Pages

78 + app. 48

Series

Aalto University publication series DOCTORAL THESES, 282/2024

Abstract

The advancement of electronics towards portable, high-performance, and flexible technologies faces significant challenges as device sizes continue to shrink. This has driven the exploration of advanced nanomaterials, with single-walled carbon nanotubes (SWCNTs), standing out due to their unique one-dimensional structure and exceptional properties, including superior conductivity, transparency, flexibility, and stability. However, scalable and controllable synthesis of SWCNT remains a critical challenge for their large-scale integration into nanoelectronics.  This dissertation focuses on the synthesis of semiconducting SWCNTs (s-SWCNTs) and their application in electronics, with the prime goal of achieving high-purity s-SWCNTs and effectively integrating them into electronic devices. The study employs a floating catalyst chemical vapor deposition (FCCVD) method to enable continuous large-scale synthesis. By optimizing growth parameters, such as temperature, gas composition, feeding rate, and carbon sources, we achieved a controllable synthesis of s-SWCNTs with a purity as high as 94%, one of the highest purities attained through direct synthesis. Water and carbon dioxide are believed to act as oxidizing agents, selectively etching metallic SWCNTs and enhancing the yield of s-SWCNTs. The resulting nanotubes have a mean diameter of approximately 1 nm and a mean length of 6.38 μm, significantly longer than those produced via solution-sorting methods. Furthermore, these synthesized s-SWCNTs demonstrated a mean mobility of 376 cm2V-1s-1 and an on-off ratio of up to 8.33×106 in individual-SWCNT field effect transistors (FETs). The carrier mobility in the optimal FETs approaches the theoretical limit for 1 nm SWCNT on a SiO2 substrate at room temperature.  Importantly, this dissertation introduces a novel, lithography-free fabrication technique for creating flexible, wafer-scale, all-CNT device arrays, addressing common issues of contamination and damage that typically arise during traditional wet processing. The resulting wafer-scale all-CNT photodetector arrays exhibit excellent uniformity, wearability, environmental stability, and notable broadband photoresponse. These photodetectors achieve a high responsivity of 44 A/W, significantly outperforming similar CNT photodetectors fabricated using photolithography and solution sorting, even with purities of up to 99% s-SWCNT. Furthermore, the dry transfer manufacturing process was employed to fabricate transparent flexible electrodes, successfully transferring SWCNT film onto MoS₂, thereby optimizing the photodetectors' light absorption and carrier separation, leading to improved responsivity. 

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Supervising professor

Kauppinen, Esko, Prof., Aalto University, Department of Applied Physics, Finland

Thesis advisor

Zhang, Qiang, Dr., Aalto University, Department of Applied Physics, Finland

Keywords

gas-phase synthesis, semiconducting single-walled carbon nanotubes, ethanol, isopropanol, transistor, wearable electronics, all-carbon nanotube devices, photodetector

Other note

Parts

  • [Publication 1]: Er-Xiong Ding†, Peng Liu†, Abu Taher Khan†, Qiang Zhang, Nan Wei, Hua Jiang, Esko I. Kauppinen. Towards the synthesis of semiconducting singlewalled carbon nanotubes by floating-catalyst chemical vapor deposition: Challenges of reproducibility. Carbon 195 (2022): 92-100.
    Full text in Acris/Aaltodoc: https://urn.fi/URN:NBN:fi:aalto-202205043004
    DOI: 10.1016/j.carbon.2022.04.020 View at publisher
  • [Publication 2]: Peng Liu, Abu Taher Khan, Er-Xiong Ding, Qiang Zhang, Zhenyu Xu, Xueyin Bai, Nan Wei, Ying Tian, Diao Li, Hua Jiang, Harri Lipsanen, Zhipei Sun, Esko I. Kauppinen. Direct synthesis of semiconducting single-walled carbon nanotubes toward high-performance electronics. Advanced Electronic Materials 9 (2023): 2300196.
    Full text in Acris/Aaltodoc: https://urn.fi/URN:NBN:fi:aalto-202308014565
    DOI: 10.1002/aelm.202300196 View at publisher
  • [Publication 3]: Peng Liu, Er-Xiong Ding, Zhenyu Xu, Xiaoqi Cui, Mingde Du, Weijun Zeng, Anastasios Karakassides, Jin Zhang, Qiang Zhang, Faisal Ahmed, Hua Jiang, Pertti Hakonen, Harri Lipsanen, Zhipei Sun, Esko I. Kauppinen. Waferscale fabrication of wearable all-carbon nanotube photodetector arrays. ACS Nano 18 (2024):18900-18909.
    Full text in Acris/Aaltodoc: https://urn.fi/URN:NBN:fi:aalto-202408065177
    DOI: 10.1021/acsnano.4c01087 View at publisher
  • [Publication 4]: Er-Xiong Ding, Peng Liu, Hoon Hahn Yoon, Faisal Ahmed, Mingde Du, Abde Mayeen Shafi, Naveed Mehmood, Esko I. Kauppinen, Zhipei Sun, Harri Lipsanen. Highly sensitive MoS2 photodetectors enabled with a dry-transferred transparent carbon nanotube electrode. ACS Applied Materials & Interfaces 15 (2023): 4216-4225.
    Full text in Acris/Aaltodoc: https://urn.fi/URN:NBN:fi:aalto-202302011875
    DOI: 10.1021/acsami.2c19917 View at publisher

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https://urn.fi/URN:ISBN:978-952-64-2208-4

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[diss] Perustieteiden korkeakoulu / SCI