Milimeter-level MoS2 monolayers and WS2-MoS2 heterojunctions grown on molten glass by pre-chemical vapor deposition

Fei Xiang; Zhang Xiu-Mei; Fu Quan-Gui; Cai Zheng-Yang; Nan Hai-Yan; Gu Xiao-Feng; Xiao Shao-Qing

doi:10.7498/aps.71.20211735

Abstract

Molybdenum disulfide (MoS₂), as a kind of two-dimensional(2D) material with novel physical properties and excellent electrical performances, has great potential applications in electronic devices. Efficient and controllable growth of large-size single crystal MoS₂ is a major difficulty that must be overcome towards scalable production. Chemical vapor deposition (CVD) is considered as the most promising means for industrial production of 2D materials. Here in this work, the high-quality and millimeter-level single crystal MoS₂monolayer grows on molten glass by the pre-chemical vapor deposition, in which MoO₃ film deposited on the molten glass is used as Mo precursor instead of MoO₃ powder. In addition, by introducing WO₃ powder into such a CVD system, MoS₂-WS₂ lateral heterojunctions can also be obtained. Raman and PL measurements indicate that the as-grown MoS₂ monolayer samples possess high quality. The Back-gate FETs are fabricated on SiO₂/Si substrates by using transferring elelctrode methods to investigate the electrical properties of the as-grown MoS₂ crystals. At room temperature and atmosphere pressure, the on-off ratio can reach 10⁵ and the carrier mobility can arrive at 4.53 cm²/(V·s). The low-cost and high-quality large-size material growth method pave the way for the scalable production of such a 2D material based electronic devices.

Keywords:

Authors and contacts

1.
Internet of Things Application Technology Engineering Research Center, Ministry of Education, Department of Electronic Engineering, Jiangnan University, Wuxi 214122, China
2.
Department of Optoelectronic Information Science and Engineering, School of Science , Jiangnan University, Wuxi 214122, China

Corresponding author: Xiao Shao-Qing, xiaosq@jiangnan.edu.cn

Funds: Project supported by the National Nature Science Foundation (Grant Nos. 62074070, 62104084, 11704159), the Natural Science Foundation of Jiangsu Province, China (Grant No. BK20170167), and the Fundamental Research Funds for the Central Universities of China (Grant No. JUSRP221015) .

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References

[1]	Hynek D J, Singhania R M, Xu S, Davis B, Wang L, Yarali M, Pondick J V, Woods J M, Strandwitz N C, Cha J J 2021 ACS Nano 15 410 Google Scholar
[2]	Susarla S, Kutana A, Hachtel J A, Kochat V, Apte A, Vajtai R, Idrobo J C, Yakobson B I, Tiwary C S, Ajayan P M 2017 Advan. Mater. 29 1702457 Google Scholar
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[4]	Cheng P, Tang C, Ahmed S, Qiao J, Zeng L, Tsang Y 2020 Nanotechnology 32 055201
[5]	Wu Y, Lin Y M, Bol A A, Jenkins K A, Xia F, Farmer D B, Zhu Y, Avouris P 2011 Nature 472 74 Google Scholar
[6]	Sarkar D, Xie X, Liu W, Cao W, Kang J, Gong Y, Kraemer S, Ajayan P M, Banerjee K 2015 Nature 526 91 Google Scholar
[7]	Jia S, Jin Z, Zhang J, Yuan J, Chen W, Feng W, Hu P, Ajayan P M, Lou J 2020 Small 16 2002263 Google Scholar
[8]	Akinwande D, Petrone N, Hone J 2014 Nat. Commun. 5 5678 Google Scholar
[9]	Chang H Y, Yang S, Lee J, Tao L, Hwang W S, Jena D, Lu N, Akinwande D 2013 ACS Nano 7 5446 Google Scholar
[10]	Lee G H, Yu Y J, Cui X, Petrone N, Lee C H, Choi M S, Lee D Y, Lee C, Yoo W J, Watanabe K, Taniguchi T, Nuckolls C, Kim P, Hone J 2013 ACS Nano 7 7931 Google Scholar
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[14]	王铄, 王文辉, 吕俊鹏, 倪振华 2021 物理学报 70 026802 Wang S, Wang W H, Lv J P, Ni Z H 2021 Acta Phys. Sin. 70 026802
[15]	Yang P, Zou X, Zhang Z, Hong M, Shi J, Chen S, Shu J, Zhao L, Jiang S, Zhou X, Huan Y, Xie C, Gao P, Chen Q, Zhang Q, Liu Z, Zhang Y 2018 Nat. Commun. 9 979 Google Scholar
[16]	Zhang Z, Xu X, Song J, Gao Q, Li S, Hu Q, Li X, Wu Y 2018 Appl. Phys. Lett. 113 202103 Google Scholar
[17]	Chen J, Zhao X, Tan S J R, Xu H, Wu B, Liu B, Fu D, Fu W, Geng D, Liu Y, Liu W, Tang W, Li L, Zhou W, Sum T C, Loh K P 2017 J. Am. Chem. Soc. 139 1073 Google Scholar
[18]	Tang L, Tan J, Nong H, Liu B, Cheng H M 2021 Acc. Mater. Res. 2 36 Google Scholar
[19]	Wan X, Miao X, Yao J, Wang S, Shao F, Xiao S, Zhan R, Chen K, Zeng X, Gu X, Xu J 2021 Advan. Mater. 33 2100260 Google Scholar
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[25]	Yang P, Zhang S, Pan S, Tang B, Liang Y, Zhao X, Zhang Z, Shi J, Huan Y, Shi Y, Pennycook S J, Ren Z, Zhang G, Chen Q, Zou X, Liu Z, Zhang Y 2020 ACS Nano 14 5036 Google Scholar
[26]	Withanage S S, Khondaker S I 2019 MRS Advan. 4 587 Google Scholar

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图 1 (a)生长MoS₂的实验装置示意图; (b)生长WS₂-MoS₂的实验装置示意图

Figure 1. Schematic illustrations of the experimental set-up for (a) MoS₂ and (b) MoS₂-WS₂ heterostructure.

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图 2 (a)熔融玻璃衬底上CVD过程的示意图; (b)尺寸500 μm的MoS₂的光镜图; (c)毫米级的MoS₂的光镜图

Figure 2. (a) Schematic illustration of CVD reaction process of the as-grown MoS₂ films on the soda-lime glass; (b) optical images of MoS₂ with size of 500 μm, (c) optical images of MoS₂ with size of 1 mm.

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图 3 转移至硅衬底上的MoS₂及相应的拉曼荧光表征 (a)(b)转移后的MoS₂光镜图; (c)(d)为(b)中样品的拉曼与荧光表征; (e)所生长MoS₂的AFM图像; (f)生长MoS₂的HRTEM, 内插图为相应的SAED

Figure 3. MoS₂ films transfered onto the Si/SiO₂ substrates and its Raman spectrum: (a) (b) Optical images of transfered MoS₂; (c) (d)single-point Raman and PL spectrum of the as-grown MoS₂films in (b); (e) AFM image of as-grown MoS₂; (f) HRTEM of as-grown MoS₂, the inset image is the SAED pattern of as-grown MoS₂.

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图 4 所生长MoS₂薄膜的拉曼与荧光 mapping测试(a) MoS₂薄膜光镜图; (b)图(a)中蓝框区域拉曼峰$ \rm E^1_{\rm 2g} $的mapping图像; (c)拉曼峰A_1g的mapping图像; (d)荧光峰1.85 eV处的mapping图像

Figure 4. Raman mapping test of as-grown MoS₂ film: (a) Optical image of a selected MoS₂ films; (b) Raman intensity mapping of $ \rm E^1_{\rm 2g} $ peak (blue area in Fig. (a)); (c) Raman intensity mapping of A_1g (blue area in Fig. (a)) ; (d) PL intensity mapping of PL peak at 1.85 eV (blue area in Fig. (a)).

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图 5 (a) MoS₂场效应管的3D模型以及真实器件的光镜图; (b) MoS₂场效应管的输出曲线; (c) MoS₂场效应管的线性转移曲线; (d) MoS₂场效应管的指数转移曲线

Figure 5. (a) Schematic of MoS₂ FET and a typical optical image of the devices; (b) output curves (I_ds-V_ds) of a typical MoS₂ FET device; (c) liner transfer curves of a typical MoS₂ FET device; (d) semilog transfer curves of a typical MoS₂ FET device.

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图 6 (a)熔融玻璃上生长的WS₂-MoS₂异质结的光镜图; (b) WS₂-MoS₂相应区域的拉曼表征; (c)异质结对应于350 cm^–1处的拉曼强度mapping; (d)异质结对应于403 cm^–1处的拉曼强度mapping

Figure 6. (a) Optical image of the as-grown WS₂-MoS₂ heterostructures on soda-lime glass; (b) single-point Raman spectra of the as-grown WS₂-MoS₂ heterostructures, (c) Raman intensity mapping of the heterostructure region at 350 cm^–1; (d) Raman intensity mapping of the heterostructure region at 403 cm^–1.

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表 1 不同CVD法生长的MoS₂的各项性能对比

Table 1. MoS₂ FET performance of different kinds of CVD.

生长方法	温度	生长衬底	单晶尺寸	迁移率	开关比
生长方法	℃	生长衬底	μm	(cm²·V^–1·s^–1)	开关比
预沉积CVD^本文	1100	钠钙玻璃	1000	4.5	10⁵
普通CVD^[16]	800	钠钙玻璃	50	24	10⁸
预沉积CVD^[26]	750	蓝宝石	25	—	—
MOCVD^[22]	320	氧化硅	120	68	>10⁵

DownLoad: CSV

[1]	Hynek D J, Singhania R M, Xu S, Davis B, Wang L, Yarali M, Pondick J V, Woods J M, Strandwitz N C, Cha J J 2021 ACS Nano 15 410 Google Scholar
[2]	Susarla S, Kutana A, Hachtel J A, Kochat V, Apte A, Vajtai R, Idrobo J C, Yakobson B I, Tiwary C S, Ajayan P M 2017 Advan. Mater. 29 1702457 Google Scholar
[3]	Huo N, Yang Y, Li J 2017 J. Semicond. 38 031002 Google Scholar
[4]	Cheng P, Tang C, Ahmed S, Qiao J, Zeng L, Tsang Y 2020 Nanotechnology 32 055201
[5]	Wu Y, Lin Y M, Bol A A, Jenkins K A, Xia F, Farmer D B, Zhu Y, Avouris P 2011 Nature 472 74 Google Scholar
[6]	Sarkar D, Xie X, Liu W, Cao W, Kang J, Gong Y, Kraemer S, Ajayan P M, Banerjee K 2015 Nature 526 91 Google Scholar
[7]	Jia S, Jin Z, Zhang J, Yuan J, Chen W, Feng W, Hu P, Ajayan P M, Lou J 2020 Small 16 2002263 Google Scholar
[8]	Akinwande D, Petrone N, Hone J 2014 Nat. Commun. 5 5678 Google Scholar
[9]	Chang H Y, Yang S, Lee J, Tao L, Hwang W S, Jena D, Lu N, Akinwande D 2013 ACS Nano 7 5446 Google Scholar
[10]	Lee G H, Yu Y J, Cui X, Petrone N, Lee C H, Choi M S, Lee D Y, Lee C, Yoo W J, Watanabe K, Taniguchi T, Nuckolls C, Kim P, Hone J 2013 ACS Nano 7 7931 Google Scholar
[11]	Das S, Gulotty R, Sumant A V, Roelofs A 2014 Nano Lett. 14 2861 Google Scholar
[12]	Xiao X, Chen M, Zhang J, Zhang T, Zhang L, Jin Y, Wang J, Jiang K, Fan S, Li Q 2019 ACS Appl. Mater. Inter. 11 11612 Google Scholar
[13]	董艳芳, 何大伟, 王永生, 许海腾, 巩哲 2016 物理学报 65 128101 Google Scholar Dong Y F, He D W, Wang Y S, Xu H T, Gong Z 2016 Acta Phys. Sin. 65 128101 Google Scholar
[14]	王铄, 王文辉, 吕俊鹏, 倪振华 2021 物理学报 70 026802 Wang S, Wang W H, Lv J P, Ni Z H 2021 Acta Phys. Sin. 70 026802
[15]	Yang P, Zou X, Zhang Z, Hong M, Shi J, Chen S, Shu J, Zhao L, Jiang S, Zhou X, Huan Y, Xie C, Gao P, Chen Q, Zhang Q, Liu Z, Zhang Y 2018 Nat. Commun. 9 979 Google Scholar
[16]	Zhang Z, Xu X, Song J, Gao Q, Li S, Hu Q, Li X, Wu Y 2018 Appl. Phys. Lett. 113 202103 Google Scholar
[17]	Chen J, Zhao X, Tan S J R, Xu H, Wu B, Liu B, Fu D, Fu W, Geng D, Liu Y, Liu W, Tang W, Li L, Zhou W, Sum T C, Loh K P 2017 J. Am. Chem. Soc. 139 1073 Google Scholar
[18]	Tang L, Tan J, Nong H, Liu B, Cheng H M 2021 Acc. Mater. Res. 2 36 Google Scholar
[19]	Wan X, Miao X, Yao J, Wang S, Shao F, Xiao S, Zhan R, Chen K, Zeng X, Gu X, Xu J 2021 Advan. Mater. 33 2100260 Google Scholar
[20]	Zhang X, Nan H, Xiao S, Wan X, Gu X, Du A, Ni Z, Ostrikov K 2019 Nat. Commun. 10 598 Google Scholar
[21]	Wang Z, Xie Y, Wang H, Wu R, Nan T, Zhan Y, Sun J, Jiang T, Zhao Y, Lei Y, Yang M, Wang W, Zhu Q, Ma X, Hao Y 2017 Nanotechnology 28 325602 Google Scholar
[22]	Park J H, Lu A Y, Shen P C, Shin B G, Wang H, Mao N, Xu R, Jung S J, Ham D, Kern K, Han Y, Kong J 2021 Small Methods 5 2000720 Google Scholar
[23]	王璐, 高俊峰, 丁峰 2014 化学学报 72 345 Google Scholar Wang L, Gao J F, Ding F 2014 Acta Chim. Sin. 72 345 Google Scholar
[24]	Wang J, Cai X, Shi R, Wu Z, Wang W, Long G, Tang Y, Cai N, Ouyang W, Geng P, Chandrashekar B N, Amini A, Wang N, Cheng C 2018 ACS Nano 12 635 Google Scholar
[25]	Yang P, Zhang S, Pan S, Tang B, Liang Y, Zhao X, Zhang Z, Shi J, Huan Y, Shi Y, Pennycook S J, Ren Z, Zhang G, Chen Q, Zou X, Liu Z, Zhang Y 2020 ACS Nano 14 5036 Google Scholar
[26]	Withanage S S, Khondaker S I 2019 MRS Advan. 4 587 Google Scholar

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Milimeter-level MoS₂monolayers and WS₂-MoS₂ heterojunctions grown on molten glass by pre-chemical vapor deposition

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Corresponding author: Xiao Shao-Qing, xiaosq@jiangnan.edu.cn

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