Chemical vapor deposition growth of large-areas two dimensional materials: Approaches and mechanisms

Wang Shuo; Wang Wen-Hui; Lü Jun-Peng; Ni Zhen-Hua

doi:10.7498/aps.70.20201398

Abstract

Two-dimensional (2D) layered materials have attracted increasing attention in recent years because of their abundant material categories and superior physical/chemical properties. In order to satisfy the requirements for highly integrated devices in the post-Moore era, substantial efforts have been devoted to producing atomically thin 2D materials with large lateral dimensions and high crystalline quality. The controllable synthesis is the precondition of the implementation of large mass producing 2D material in industry. Chemical vapor deposition (CVD) is a powerful method widely used in the synthesis of 2D materials and their hybrid structures. However, it is still challengeable to flexibly and easily grow any 2D materials into large area. Therefore, a systematic understanding of the requirements for controllable growth of different 2D materials are desired. In this review article, we provide a comprehensive discussion on the influencing factors, material transport, nucleation and growth rate in the CVD growth process. Finally, the strategies to further improve the size and quality of 2D materials are prospected.

Keywords:

Authors and contacts

School of Physics, Southeast University, Nanjing 211189, China

Corresponding author: Lü Jun-Peng, phyljp@seu.edu.cn ; Ni Zhen-Hua, zhni@seu.edu.cn

Funds: Project supported by the National Basic Research Program of China (Grant Nos. 2017YFA0205700, 2019YFA0308000) and the National Natural Science Foundation of China (Grant Nos. 61774034, 91963130)

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Cited By

图 1 CVD过程中影响二维材料产物的参数及因素^[21]

Figure 1. The affecting parameters and factors during CVD growth of two-dimensional materials^[21].

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图 2 传统CVD的反应过程示意图^[35]

Figure 2. Schematic illustration of the reaction processes in a typical CVD reactor^[35].

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图 3 (a) OIAG法生长MoX₂的方案示意图; (b) OIAG中OI的工作机制示意图; (c)−(f)不同OI剂量(c) 4 mg, (d) 5 mg, (e) 6 mg, (f) 7 mg 下MoS₂的光镜图像^[39]; (g) 使用多条路径制备MoS₂薄膜的方案示意图; (h) 蓝宝石衬底上生长的晶圆级MoS₂图像^[40]

Figure 3. Schematic illustration of (a) the growth of MoX₂ by OIAG and (b) the working mechanism of OI in the progress of OIAG; (c)−(f) optical images of MoS₂ with different concentrations: (c) 4 mg, (d) 5 mg, (e) 6 mg, (f) 7 mg^[39]; (g) schematic illustration of the modified CVD system for MoS₂ growth; (h) photograph of MoS₂ film grown on sapphire substrates^[40].

DownLoad: Full-Size Img PowerPoint

图 4 合成厘米级WTe₂的CVD装置图示^[42]

Figure 4. Schematic illustration of the growth of WTe₂ film with centimeter-scale by three-zone chemical vapor depo-sition^[42].

DownLoad: Full-Size Img PowerPoint

图 5 (a), (b) 抛光前后的铜箔的扫描电子显微镜(scanning electron microscope, SEM)图像^[53]; (c) 在钨衬底上平坦液体Cu表面制备石墨烯的示意图; (d) SEM下六方石墨烯畴在液体Cu表面的“自组装样”行为^[54]; (e) 合成MoSe₂薄膜的CVD装置图示; (f) 光镜下MoSe₂薄膜的图像; (g) MoSe₂薄膜的扫描隧道显微镜(scanning tunneling microscope, STM)图像^[55]

Figure 5. SEM images of Cu foil (a) before- and (b) after-polishing^[53]; (c) schematic illustration of the synthesis of graphene on the liquid Cu surface; (d) SEM image of “self-assembling sample behavior” of hexagonal graphene domains on liquid Cu surface^[54]; (e) schematic demonstration of the growth of the WTe₂ film by CVD; (f) optical image of MoSe₂ film; (g) STM image of MoSe₂ film^[55].

DownLoad: Full-Size Img PowerPoint

图 6 (a) 石墨烯在不同温度下在Ni(111)表面和台阶处的成核率与$ \Delta \mu $的函数关系; (b) 不同温度下R_E/R_T比率与$ \Delta \mu $的函数关系^[48] (R_T, 平台上石墨烯的成核率; R_E, 台阶表面的成核率); (c) 晶体生长曲线, 吉布斯自由能变化和团簇所含原子数n的关系^[57]

Figure 6. (a) Nucleation rates of graphene growth on a Ni(111) terrace and near a step edge as a function of$ \Delta \mu $; (b) R_E/R_T ratio as the function of $ \Delta \mu $^[48] (R_T, nucleation rate of graphene on the terrace; R_E, nucleation rate of graphene on the step edge); (c) crystal growth curve: Gibbs free energy as a function of the cluster size, n^[57].

DownLoad: Full-Size Img PowerPoint

图 7 (a)铜片氧化前后对比图^[58]; 不同退火时间下的石墨烯光学图片 (b) 50 min; (c) 90 min; 不同CH₄和H₂比例下长出的石墨烯光学图片 (d) 2 sccm: 60 sccm; (e) 1 sccm: 80 sccm; (f) 1 sccm: 100 sccm; (g) 0.5 sccm: 80 sccm; 不同生长时间下石墨烯的形貌图 (h) 100 min; (i) 200 min; (j) 420 min; (k) 500 min; (l) 660 min^[59]

Figure 7. (a) Comparison diagram of Cu foil with/without oxidation^[58]; optical images of graphene for different annealing time: (b) 50 min; (c) 90 min; optical images of graphene for different proportion of CH₄ and H₂: (d) 2 sccm:60 sccm; (e) 1 sccm:80 sccm; (f) 1 sccm∶100 sccm; (g) 0.5 sccm∶80.0 sccm; optical images of graphene for different growth time: (h) 100 min; (i) 200 min; (j) 420 min; (k) 500 min; (l) 660 min^[59].

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图 8 (a)—(d) 不同生长时间下WS₂的光学图像　(a) 3 min; (b) 5 min; (c) 8 min; (d) 15 min; (e) WS₂平均尺寸和生长时间的关系曲线^[60]

Figure 8. Optical images of WS₂ for different time: (a) 3 min; (b) 5 min; (c) 8 min; (d) 15 min; (e) plot of average flake size versus growth durations^[60].

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图 9 (a), (b) 位于石墨烯边缘的Ni原子的STM图像^[61]; (c) 未经氧处理的石墨烯边缘示意图; (d) 对H附着的能量进行的密度泛函理论计算(density functional theory, DFT)^[62]; (e) 氧处理的石墨烯边缘示意图; (f) 局部供氧法示意图; (g) 氧未参与反应的CH₄分解过程; (h) 反应能量分布示意图; (i) 氧参与反应的CH₄分解过程^[63]

Figure 9. (a), (b) STM images of the Ni adatoms at the graphene edges^[61]; (c)−(e) schematic illustration of graphene edges (e) with and (c) without oxygen and (d) the corresponding DFT calculations of the energies for H attachment^[62]; (f) schematic illustration of the growth of WTe₂ film by local-oxygen-feeding method; (g)−(i) the energy profiles of the reaction of CH₄ decomposition (i) with and (g) without oxygen supply on Cu surface and (h) the corresponding DFT calculations of the energy dispersion^[63].

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图 10 (a) 单层MoS₂的光学图像; (b), (c) 引入Na元素和未引入Na元素的DFT对比实验^[64]; (d) 使用盐辅助法合成的几种TMDs薄膜的光学图像^[65]

Figure 10. (a) Optical image of monolayer MoS₂ film; (b), (c) DFT calculations for the growth of MoS₂ (b) without and (c) with Na^[64]; (d) schematic illustration of the salt-assisted reaction process and optical images of TMDs films^[65].

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map

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