Hole-doping-assisted epitaxial growth of wafer-scale rhombohedral-stacked bilayer transition-metal dichalcogenides single crystals

Hang Sun, Zhu Du, Yanan Peng, Xiaohui Li, Qiang Wan, Ling Huang, Luying Song, Ziyi Han, Ruihan Xu, Yinuo Li, Yuhang Li, Yulin Jiang, Xiaoxu Zhao, Nan Xu, Lei Liao, Congxin Xia (), Jianping Shi () and Jun He ()
Additional contact information
Hang Sun: Wuhan University
Zhu Du: Wuhan University
Yanan Peng: Wuhan University
Xiaohui Li: Wuhan University
Qiang Wan: Wuhan University
Ling Huang: Wuhan University
Luying Song: Wuhan University
Ziyi Han: Peking University
Ruihan Xu: Wuhan University
Yinuo Li: Wuhan University
Yuhang Li: Wuhan University
Yulin Jiang: Wuhan University
Xiaoxu Zhao: Peking University
Nan Xu: Wuhan University
Lei Liao: Hunan University
Congxin Xia: Henan Normal University
Jianping Shi: Wuhan University
Jun He: Wuhan University

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract Bilayer rhombohedral-stacked transition-metal dichalcogenides (3R-TMDCs) combining high carrier mobility, good electrostatic control, and exotic switchable polarization are emerging as promising semiconducting channels for beyond-silicon electronics. However, despite great efforts, the growth of wafer-scale bilayer 3R-TMDCs single crystals remains difficult due to challenges in the synergistic control of phase structure and grain orientation. Here we design a hole-doping-assisted strategy to synthesize a series of two-inch bilayer 3R-TMDCs single crystals on c-plane sapphire. The introduction of hole dopants (e.g. Hf, V, Nb, Ta) not only increases the interlayer coupling to break the formation energy degeneracy of bilayer 3R-stacked and hexagonal-stacked TMDCs, but also promotes the parallel steps formation on sapphire surfaces to induce the unidirectionally aligned bilayer grain nucleation. The fabricated ferroelectric semiconductor field-effect transistors based on bilayer Hf-MoS2 demonstrate high endurance (more than 105 cycles) and long retention time (exceeding one year) due to the restriction of interlayer charge defect migration/aggregation caused by sliding ferroelectricity. This work proposes a promising strategy for synthesizing wafer-scale ferroelectric semiconductor single crystals, which could promote the further exploration of logic-in-memory chips.

Date: 2025
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DOI: 10.1038/s41467-025-65427-2

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