<p>Unidirectional nucleation followed by seamless stitching has emerged as a promising strategy for the scalable epitaxial growth of single-crystalline monolayer transition metal dichalcogenides on sapphire substrates, which holds potential for post-silicon electronics. In contrast, here we present a different growth mechanism for single-crystalline MoS<sub>2</sub> on c-plane sapphire via metal-organic chemical vapor deposition (MOCVD). We show that the initial nucleation generates not only 0° and antiparallel 60° domains but also low-angle twisted domains, consistent with the coincidence site lattice framework. However, these rotationally misoriented domains are observed to deterministically self-align and merge into energetically preferred 0° domain during coalescence, yielding a continuous, unidirectional single-crystal. Additionally, by employing MoO<sub>2</sub>Cl<sub>2</sub> as a molybdenum precursor, we demonstrate that the growth of MoS<sub>2</sub> occurs in a self-limiting manner. This epitaxial strategy is substantiated by a carrier mobility of 66 cm<sup>2</sup>/Vs at room temperature and 749 cm<sup>2</sup>/Vs at low temperatures. Our approach offers a practical and reproducible scheme for MOCVD-based van der Waals epitaxy for 2D electronics.</p>

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Self-aligned and self-limiting van der Waals epitaxy of monolayer MoS2 for scalable 2D electronics

  • Yoshiki Sakuma,
  • Keisuke Atsumi,
  • Takanobu Hiroto,
  • Jun Nara,
  • Akihiro Ohtake,
  • Yuki Ono,
  • Takashi Matsumoto,
  • Yukihiro Muta,
  • Kai Takeda,
  • Emi Kano,
  • Toshiki Yasuno,
  • Xu Yang,
  • Nobuyuki Ikarashi,
  • Asato Suzuki,
  • Michio Ikezawa,
  • Shuhong Li,
  • Tomonori Nishimura,
  • Kaito Kanahashi,
  • Kosuke Nagashio

摘要

Unidirectional nucleation followed by seamless stitching has emerged as a promising strategy for the scalable epitaxial growth of single-crystalline monolayer transition metal dichalcogenides on sapphire substrates, which holds potential for post-silicon electronics. In contrast, here we present a different growth mechanism for single-crystalline MoS2 on c-plane sapphire via metal-organic chemical vapor deposition (MOCVD). We show that the initial nucleation generates not only 0° and antiparallel 60° domains but also low-angle twisted domains, consistent with the coincidence site lattice framework. However, these rotationally misoriented domains are observed to deterministically self-align and merge into energetically preferred 0° domain during coalescence, yielding a continuous, unidirectional single-crystal. Additionally, by employing MoO2Cl2 as a molybdenum precursor, we demonstrate that the growth of MoS2 occurs in a self-limiting manner. This epitaxial strategy is substantiated by a carrier mobility of 66 cm2/Vs at room temperature and 749 cm2/Vs at low temperatures. Our approach offers a practical and reproducible scheme for MOCVD-based van der Waals epitaxy for 2D electronics.