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随着芯片尺寸不断缩小, 短沟道效应、热效应日趋显著. 开发全新的量子材料体系以实现高性能芯片器件应用已成为当前科技发展的迫切需求. 二维材料作为一类重要的量子材料, 其天然具备原子层厚度和平面结构, 能够有效克服短沟道效应并兼容当代微纳加工工艺, 非常有望应用于新一代高性能器件方向. 与硅基芯片发展类似, 二维材料芯片级器件应用必须基于高质量、大尺寸的二维单晶材料制造. 然而, 由于二维材料的表界面特性, 现有体单晶制备技术不能完全适用于单原子层结构的二维单晶制造. 因此, 亟需发展新的制备策略以实现大尺寸、高质量的二维单晶原子制造. 有鉴于此, 本文重点综述表界面调控二维单晶大尺寸制备技术发展现状, 总结梳理了米级二维单晶原子制造过程中的3个关键调控方向, 即单畴生长调控、单晶衬底制备和多畴取向控制. 最后, 系统展望了大尺寸二维单晶在未来规模化芯片器件方向的潜在应用前景.With the shrinkage of the chip feature size, the short-channel effect becomes more and more predominate. The development of new quantum materials for high-performance devices has become imperative for the current technological development. Two-dimensional (2D) materials, due to their excellent physical and chemical properties, are thought to be the promising candidate of quantum materials for achieving the high-end electronic and optoelectronic devices. Like the development of silicon-based chips, the wafer-scale device applications of 2D materials must be based on the fabrication of high-quality, large-size 2D single crystals. However, the existing manufacturing techniques of the well-studied bulk single crystals cannot be fully applied to the fabrication of 2D single crystals due to the interfacial characteristics of 2D materials. So far, single crystals of metre-sized graphene, decimetre-sized hBN and wafer-sized TMDCs have been successfully prepared by chemical vapor deposition, but the sizes of other 2D single crystals are still very limited and not in the same league as conventional semiconductor materials. Therefore, it is urgent to develop an effective preparation strategy for the manufacture of various 2D single crystals. In this review, we mainly overview the fabrication techniques for the meter-scale growth of 2D single crystals, and propose three key modulation aspects in the atomic-scale manufacture, i.e. the growth modulation of 2D single nucleus, the preparation of single-crystal substrates, and the alignment control of 2D single-crystal domains, in order to provide a universal method of fabricating the large-size 2D single crystals. Finally, the prospect of chip devices based on these high-quality large-size novel 2D single crystals is discussed, thereby paving the way for the future industrial applications of electronics and optoelectronics.
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图 1 大尺寸二维单晶制备3个关键调控方向
Fig. 1. Schematic illustration of three key aspects for the growth of large-size 2D single crystals.
图 2 二维材料单畴生长调控 (a)氧辅助铜箔上石墨烯晶畴生长的光学图像[47]; (b)石墨烯晶畴生长速率dr/dt与1/T的对数曲线[47]; (c)控制单个晶畴形核并长大示意图; (d)局域氧元素供应方法的实验设计示意图[84]; (e)局域氟元素供应反应能量曲线[56]; (f)同位素标记局域氟辅助石墨烯晶畴生长速率结果[56]; (g)金箔上WSe2晶畴快速生长光学结果[93]
Fig. 2. Growth modulation of 2D single nucleus: (a) Optical image of centimeter-scale graphene domains on oxygen-rich Cu exposed to O2[47]; (b) logarithmic plots of graphene domain growth rate dr/dt versus 1/T[47]; (c) schematic illustration of controlling single nucleus growth; (d) schematic illustration of the experimental design of local-oxygen-feeding method[84]; (e) the corresponding energy profile of carbon species with the assistance of local fluorine[56]; (f) isotope-labelled Raman mapping of the 2D band for graphene domain grown by local fluorine supply[56]; (g) optical image of single-crystal monolayer WSe2 domain grown on an Au foil[93]
图 3 单晶衬底制备 (a) 2 in蓝宝石衬底上沉积Cu(111)薄膜[96]; (b) Cu(111)表面原子力显微镜图像[96]; (c)温度梯度驱动单晶Cu(111)箔片实验设计图[55]; (d)退火获得的5 cm×50 cm大尺寸单晶Cu(111)箔[55]; (e)氧化层界面驱动A4纸尺寸高指数Cu(hkl)制备[100]; (f)高指数单晶铜箔电子背散射衍射反极图[101]
Fig. 3. Preparation of single-crystal substrate: (a) A photograph of 2 in Cu(111) film on sapphire[96]; (b) atomic force microscopic image of Cu(111) film with noncontact mode[96]; (c) schematic illustration of experimental design for the continuous production of single-crystal Cu(111) foil with a hot temperature zone at the central area of the furnace tube[55]; (d) the obtained 5 cm×50 cm single-crystal Cu(111) foil[55]; (e) the preparation of high-index Cu(hkl) with typical size of 35 cm×21 cm driven by oxide layer[100]; (f) electron backscatter diffraction inverse pole figure maps of the as-prepared high-index single-crystal Cu foils[101].
图 4 二维单晶多畴取向控制 (a) Cu(111)上单晶石墨烯晶畴取向排列[55]; (b) Cu(110)表面
$\left\langle {211} \right\rangle $ 方向原子台阶只倾向与hBN的N原子进行结合[58]; (c) Cu(110)衬底上hBN晶畴单一取向排列[58]; (d)在蓝宝石衬底上单层MoS2晶畴拼接的高分辨透射电子显微镜图像[109]; (e) Au(111)衬底上台阶诱导MoS2形核以及外延取向控制示意图[108]; (f) WS2晶畴沿Al2O3$\langle {1 \bar{1}01} \rangle$ 台阶方向形核生长的原子力显微镜结果[60]; (g) 2 in蓝宝石衬底上满覆盖单层WS2照片[60]Fig. 4. Alignment control of 2D single-crystal domains: (a) Optical image of unidirectionally aligned graphene domains grown on Cu(111)[55]; (b) Cu
$\left\langle {211} \right\rangle $ atomic steps tend to connect with the N atom of hBN[58]; (c) scanning electron microscopic image of as-grown aligned hBN domains on the Cu(110) substrate[58]; (d) high-resolution transmission electron microscopic image of the stitched domain boundary in monolayer MoS2 on sapphire substrate[109]; (e) schematic illustration of MoS2 nucleation and epitaxial growth process on Au(111) substrate[108]; (f) WS2 domain grown along the Al2O3$\langle {1 \bar{1}01} \rangle$ steps[60]; (g) photograph of the full-coverage WS2 monolayer on a 2 in sapphire substrate[60]. -
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