Multilayer graphene and its stacking order provide both fundamentally intriguing properties and technological engineering applications. Several approaches to control the stacking order have been demonstrated, but a method of precisely controlling the number of layers with desired stacking sequences is still lacking. Here, we propose an approach for controlling the layer thickness and crystallographic stacking sequence of multilayer graphene films at the wafer scale via Cu–Si alloy formation using direct chemical vapour deposition. C atoms are introduced by tuning the ultra-low-limit CH₄ concentration to form a SiC layer, reaching one to four graphene layers at the wafer scale after Si sublimation. The crystallographic structure of single-crystalline or uniformly oriented bilayer (AB), trilayer (ABA) and tetralayer (ABCA) graphene are determined via nano-angle-resolved photoemission spectroscopy, which agrees with theoretical calculations, Raman spectroscopy and transport measurements. The present study takes a step towards the layer-controlled growth of graphite and other two-dimensional materials.

多层石墨烯及其堆叠顺序从根本上提供了有趣的特性和技术工程应用。已经证明了几种控制堆叠顺序的方法，但是仍然缺少一种精确控制具有所需堆叠顺序的层数的方法。在这里，我们提出了一种使用直接化学气相沉积通过Cu-Si合金形成来控制晶圆级多层石墨烯薄膜的层厚度和晶体学堆叠顺序的方法。通过调节超低限CH ₄引入C原子升华形成硅层后，在硅片上达到晶片级的一到四个石墨烯层。单晶或均匀取向的双层（AB），三层（ABA）和四层（ABCA）石墨烯的晶体结构是通过纳米角分辨光发射光谱法确定的，这与理论计算，拉曼光谱和传输测量相吻合。本研究朝着石墨和其他二维材料的层控制生长迈出了一步。