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

作者：Hang Sun, Du Zhu, Yanan Peng, Xiaohui Li, Qiang Wan, Ling Huang, Luying Song, Ziyi Han, Rui‐Hua Xu, Yinuo Li, Yuhang Li, Yulin Jiang, Xiaoxu Zhao, Nan Xu, Lei Liao, Congxin Xia, Jianping Shi, Jun He · 发表于：Nature Communications · 年份：2025 · DOI：10.1038/s41467-025-65427-2 · 被引用次数：6 · 研究领域：2D Materials and Applications、Ferroelectric and Negative Capacitance Devices、Advanced Sensor and Energy Harvesting Materials

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. 2D rhombohedral-stacked transition metal dichalcogenides (3R-TMDs) combine high carrier mobility and ferroelectric...