Ma Wei, Ma Lai-Peng, Kong Xiao, Yan Han, Liu Zhibo, Han Tiannan, Zhu Chao, Cheng Hui-Ming, Liu Zheng, Ding Feng, Ren Wencai
Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, People's Republic of China.
School of Materials Science and Engineering, University of Science and Technology of China, Shenyang 110016, People's Republic of China.
Proc Natl Acad Sci U S A. 2025 May 6;122(18):e2419968122. doi: 10.1073/pnas.2419968122. Epub 2025 Apr 29.
State-of-the-art synthesis strategies of two-dimensional (2D) materials have been designed following the nucleation-dominant pattern for structure control. However, this classical methodology fails to achieve the precise layer- and stacking-resolved growth of wafer-scale few-layer 2D materials due to its intrinsically low energy resolution. Here, we present an intelligent self-correcting method for the high-resolution growth of uniform few-layer graphene. We demonstrate the layer-resolved growth of wafer-scale bilayer and trilayer graphene (BLG and TLG) with selective Bernal stacking through spontaneous correction of the single-layer graphene film with disordered multilayer graphene islands. Theoretical calculations reveal that the self-correcting growth is driven by the stepwise energy minimization of the closed system and kinetically activated by forming a low-barrier pathway for the carbon detachment-diffusion-attachment. Such uniform Bernal-stacked BLG and TLG films show high quality with distinct quantum Hall effect being observed. Our work opens an avenue for developing an intelligent methodology to realize the precise synthesis of diverse 2D materials.
二维（2D）材料的先进合成策略是按照成核主导模式设计的，用于结构控制。然而，这种经典方法由于其固有的低能量分辨率，无法实现晶圆级少层2D材料的精确层分辨和堆叠分辨生长。在此，我们提出了一种用于均匀少层石墨烯高分辨率生长的智能自校正方法。我们通过用无序多层石墨烯岛对单层石墨烯薄膜进行自发校正，展示了具有选择性伯纳尔堆叠的晶圆级双层和三层石墨烯（BLG和TLG）的层分辨生长。理论计算表明，自校正生长是由封闭系统的逐步能量最小化驱动的，并通过形成碳脱离 - 扩散 - 附着的低势垒路径在动力学上被激活。这种均匀的伯纳尔堆叠BLG和TLG薄膜显示出高质量，观察到了明显的量子霍尔效应。我们的工作为开发一种智能方法以实现各种二维材料的精确合成开辟了一条途径。
