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以单层二硫化钼(MoS2)为代表的过渡金属硫族化合物半导体材料具有良好的光学、电学性质, 近十年来引起了人们广泛的研究兴趣. 合成高质量单层MoS2薄膜是科学研究及工业应用的基础. 最近科研人员提出了盐辅助化学气相沉积生长单层薄膜的方法, 大大提高了单层MoS2薄膜的生长速度及晶体质量. 本文基于此方法, 提出利用氯化钠(NaCl)的双辅助方法, 成功制备了高质量的单层MoS2薄膜. 光致发光(PL)谱显示其发光强度比无NaCl辅助生长的样品有了明显的提高. 本文提出的NaCl双辅助生长方法为二维材料的大规模生长提供了思路.In recent years, transition metal dichalcogenides materials represented by monolayer molybdenum disulfide (MoS2) have aroused great interest due to their excellent optical and electrical properties. The synthesis method of high-quality monolayer MoS2 film is a key problem for scientific research and industrial application. Recently, researchers have proposed a salt-assisted chemical vapor deposition method for growing the monolayer films, which greatly promotes the growth rate and quality of monolayer film. By using this method, we design a growth source of semi-enclosed quartz boat, and successfully obtain high-quality monolayer MoS2 films by using the double auxiliary action of sodium chloride (NaCl). Scanning electron microscopy shows the excellent film formation, and the photoluminescence spectra show that the luminescence intensity is significantly higher than that of the sample grown without NaCl. The NaCl double-assisted growth method proposed in this study can reduce the growth temperature of MoS2, shorten the growth time, and improve the optical properties of the films. Besides, the operation is simple and the cost is low, which provides an idea for growing the large-scale two-dimensional materials.
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Keywords:
- MoS2 /
- chemical vapor deposition /
- NaCl dual-assist strategy /
- monolayer film growth
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图 1 (a) 生长装置示意图; (b) 盛放Mo源的半封闭式石英舟; (c) 温度变化趋势图
Fig. 1. (a) Schematic illustrations of the experimental set-up; (b) semi-enclosed quartz boat for Mo source; (c) temperature program for the growth
图 2 不同生长时间下的MoS2光学显微镜图像 (a) 10 min; (b) 15 min, 内插图为单个MoS2的AFM图; (c) 20 min
Fig. 2. Optical microscope images of MoS2 at different growth times: (a) 10 min; (b) 15 min, the inside image is AFM diagram of single MoS2; (c) 20 min
图 3 Mo源中加入不同NaCl量的光学显微镜图像 (a) 0 mg; (b) 5 mg; (c) 10 mg, 内插图为单个MoS2的AFM图; (d) 15 mg
Fig. 3. Optical microscope images of Mo source with different amounts of NaCl: (a) 0 mg; (b) 5 mg; (c) 10 mg, the inside image is an AFM diagram of single MoS2; (d) 15 mg
图 4 衬底上添加不同浓度NaCl的光学显微镜图像 (a) 0.1 mmol/L; (b) 0.3 mmol/L, 内插图为单个MoS2的AFM图; (c) 0.5 mmol/L
Fig. 4. Optical microscope images of different concentrations of NaCl: (a) 0.1 mmol/L; (b) 0.3 mmol/L, the inside image is an AFM diagram of single MoS2; (c) 0.5 mmol/L.
图 5 (a)—(c) 不同浓度的NaCl搭配下的光学显微镜图像 (a) 10 mg + 0.1 mmol/L; (b) 10 mg + 0.3 mmol/L, 内插图为MoS2边界的AFM图; (c) 10 mg + 0.5 mmol/L. (d) 10 mg + 0.3 mmol/L条件下生长的MoS2在Si衬底的照片以及左中右三块区域的大范围SEM图像
Fig. 5. (a)–(c) Optical microscope images with different concentrations of NaCl: (a) 10 mg + 0.1 mmol/L; (b) 10 mg + 0.3 mmol/L, the inside image is an AFM diagram of MoS2 boundary; (c) 10 mg + 0.5 mmol/L. (d) Photographs of MoS2 grown under the condition of 10 mg + 0.3 mmol/L and large range SEM images corresponding to the three regions of left, middle and right
图 8 (a) 4种在不同位置添加NaCl生长的单层MoS2的PL光谱; (b) 4种样品的归一化PL光谱
Fig. 8. (a) PL spectra of four monolayer MoS2 grown at different locations with NaCl addition; (b) normalized PL spectra of four samples
图 6 在不同位置添加NaCl生长的MoS2的拉曼图
Fig. 6. Raman spectra of MoS2 growing at different locations of NaCl
图 7 掺入NaCl和未掺入NaCl条件下合成单层MoS2的XPS表征, 其中(a)—(c)分别是(a) Mo 3d, (b) S 2p和(c) Na 1s的XPS图; (d) XPS全谱
Fig. 7. XPS characterizations of monolayer MoS2 synthesized with NaCl and without NaCl. The XPS spectra of two MoS2 samples: (a) Mo 3d; (b) S 2p; (c) Na 1s. (d) The full spectrum of XPS
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[1] Novoselov K S, Geim A K, Morozov S V, Jiang D, Zhang Y, DUbonos S V, Grigorieva I V, Firsov A A 2004 Science 306 666
Google Scholar
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Google Scholar
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Google Scholar
[4] Wu T, Zhang X, Yuan Q, Xue J, Lu G, Liu Z, Wang H, Wang H, Ding F, Yu Q, Xie X, Jiang M 2016 Nat. Mater. 15 43
Google Scholar
[5] 徐依全, 王聪 2020 69 184216
Google Scholar
Xu Y Q, Wang C 2020 Acta Phys. Sin. 69 184216
Google Scholar
[6] Mak K F, Lee C, Hone J, Shan J, Heinz T F 2010 Phys. Rev. Lett. 105 136805
Google Scholar
[7] Yu Z, Ong Z Y, Li S, Xu J B, Zhang G, Zhang Y W, Shi Y, Wang X 2017 Adv. Funct. Mater. 27 1604093
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[9] Lembke D, Kis A 2012 ACS Nano 6 10070
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[10] Zhang W, Huang J K, Chen C H, Chang Y H, Cheng Y J, Li L J 2013 Adv. Mater. 25 3456
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Fan Z R, Kong Y Y, Li Y H, Li Z, Jia T T 2019 J. Synth. Cryst. 48 1190
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[13] Fu D, Zhao X, Zhang Y Y, Li L, Xu H, Jang A R, Yoon S I, Song P, Poh S M, Ren T, Ding Z, Fu W, Shin T J, Shin H S, Pantelides S T, Zhou W, Loh K P 2017 J. Am. Chem. Soc. 139 9392
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[15] Wang S, Rong Y, Fan Y, Pacios M, Bhaskaran H, He K, Warner J H 2014 Chem. Mater. 26 6371
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Wei X X, Cheng Y, Huo D, Zhang Y H, Wang J Z, Hu Y, Shi Y 2014 Acta Phys. Sin. 63 217802
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Google Scholar
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Google Scholar
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