硒化温度对MoSe<sub>2</sub>薄膜结构和光学带隙的影响

吴诗漫; 陶思敏; 吉爱闯; 管绍杭; 肖剑荣

doi:10.7498/aps.73.20240611

摘要

使用射频磁控溅射技术制备了钼(Mo)膜, 再利用硒化退火方式生成二硒化钼(MoSe₂)薄膜. 对MoSe₂薄膜的表面形貌、晶体结构和光学带隙进行了表征和分析. 结果显示, MoSe₂薄膜的晶体结构与硒化温度(T_s)密切相关, 随着硒化温度的升高, 薄膜的平均晶粒尺寸先略减小后增大, 且(002)晶面取向优先生长. MoSe₂薄膜对短波长光(600 nm左右)具有较低的吸收率. 随着硒化温度升高, MoSe₂的直接带隙波发生蓝移, 光学带隙随之减小. 研究表明, 通过改变硒化温度可以有效调控MoSe₂结构和光学带隙, 为MoSe₂薄膜在光学器件应用方面提供更多可能.

关键词:

Abstract

In recent years, MoSe₂, as a kind of transition metal dichalcogenide, has aroused widespread research interest due to its special crystal structure with different electrical and optical properties. The band gap of molybdenum diselenide can be manipulated by different layers, strain engineering, doping, or the formation of heterostructures, which makes it potential advantages in optoelectronic devices and photovoltaic applications. In this work, we investigate the influence of selenization temperature on the structures and optical properties of the MoSe₂ films. Molybdenum (Mo) thin films are prepared by RF magnetron sputtering, and then MoSe₂ thin films are generated by selenization annealing. The surface morphology, crystal structure, and optical bandgap for each of the MoSe₂ thin films are characterized and analyzed by using scanning electron microscopy, X-ray diffraction, and ultraviolet visible spectroscopy, respectively. The results show that the crystal structures of the MoSe₂ thin films are closely related to the selenization temperature (T_s): with the increase of selenization temperature, the average grain size in the thin film decreases slightly and then increases rapidly from 24.82 nm to 55.76 nm. Meanwhile, the (002) crystal plane of MoSe₂ also exhibits preferential growth with temperature increasing. Each MoSe₂ thin film has a low absorption rate for short-wavelength light (around 600 nm). With the increase of selenization temperature, the bandgap waves of the MoSe₂ thin films are blue-shifted, and the optical bandgaps decrease, which is attributed to the fact that different selenization temperatures cause the lattice size of MoSe₂ to change, thereby affecting the spatial expansion of its electronic wave function. In addition, the structure and optical bandgap of MoSe₂ can be effectively controlled by changing the selenization temperature, which provides more possibilities for the applications of the MoSe₂ thin films in optical devices.

Keywords:

作者及机构信息

桂林理工大学物理与电子信息工程学院, 桂林　541004

通信作者: 肖剑荣, xjr@glut.edu.cn

基金项目: 国家自然科学基金(批准号: 12064006)资助的课题.

Authors and contacts

School of Physics and Electronic Information Engineering, Guilin University of Technology, Guilin 541004, China

Corresponding author: Xiao Jian-Rong, xjr@glut.edu.cn

文章全文 : translate this paragraph

参考文献

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施引文献

图 1 (a) MoSe₂薄膜的XRD图谱; (b) MoSe₂薄膜主要的衍射峰为(002), (100), (110)时不同硒化温度下的织构系数; (c) MoSe₂薄膜平均晶粒尺寸随硒化温度的变化曲线和微应变值

Fig. 1. (a) XRD pattern of MoSe₂ thin film; (b) texture coefficient at different selenization temperatures when the main diffraction peaks of MoSe₂ thin film are (002), (100), and (110); (c) variation curve and microstrain value of the average grain size of MoSe₂ thin film with selenization temperature.

下载: 全尺寸图片幻灯片

图 2 当硒化温度不同时, MoSe₂薄膜的SEM图像(a)—(d)及典型横截面图像(e)—(h)　(a), (e) 750 ℃; (b), (f) 800 ℃; (c), (g) 850 ℃; (d), (h) 900 ℃. (i)不同温度的MoSe₂薄膜的Se, Mo元素原子占比图

Fig. 2. SEM images (a)–(d) and typical cross-sectional images (e)–(h) of MoSe₂ thin films at different selenization temperatures: (a), (e) 750 ℃; (b), (f) 800 ℃; (c), (g) 850 ℃; (d), (h) 900 ℃. (i) Atomic proportion of Se and Mo elements in MoSe₂ thin films at different temperatures.

下载: 全尺寸图片幻灯片

图 3 MoSe₂薄膜的50 nm (a)和5 nm (b)分辨透射电子显微镜图片; MoSe₂薄膜(002) (c)和(100) (d)面的选取电子衍射图样; (e)衍射环

Fig. 3. 50 nm (a) and 5 nm (b) resolution TEM images of MoSe₂ thin films; select electron diffraction patterns for the (002) (c) and (100) (d) planes of MoSe₂ thin film; (e) diffraction ring.

下载: 全尺寸图片幻灯片

图 4 MoSe₂薄膜在900 ℃的XPS图谱　(a)总谱; (b) Se 3d; (c) Mo 3d

Fig. 4. XPS spectrum of MoSe₂ thin film at 900 ℃: (a) Overall spectrum; (b) Se 3d; (c) Mo 3d.

下载: 全尺寸图片幻灯片

图 5 (a) MoSe₂薄膜的吸收光谱, 插图不同温度下MoSe₂薄膜的平均吸收率; (b) MoSe₂薄膜的Tauc关系图; (c)不同硒化温度MoSe₂薄膜的发致发光光谱

Fig. 5. (a) Absorption spectrum of MoSe₂ thin film, insert is the average absorption rate of MoSe₂ thin film at different temperatures; (b) Tauc diagram of MoSe₂ thin film; (c) photoluminescence spectra of MoSe₂ thin films at different selenization temperatures.

下载: 全尺寸图片幻灯片

下载: 全尺寸图片幻灯片

表 1 750—900 ℃ MoSe₂薄膜的各元素原子、质量占比

Table 1. Atomic and mass ratios of various elements in MoSe₂ thin films at 750–900 ℃.

Temperature/℃ Element Atomic/% Weight/%

750 Se 44.46 52.70
Mo 28.30 40.76
O 27.24 6.54
800 Se 55.34 47.25
Mo 38.58 27.11
O 6.09 25.65
850 Se 59.16 54.97
Mo 37.23 26.47
O 3.61 16.56
900 Se 58.06 53.12
Mo 37.88 28.53
O 4.06 18.35

下载: 导出CSV

map

[1]	Monga D, Sharma S, Shetti N P, Basu S, Reddy K R, Aminabhavi T M 2001 Mater. Today Chem. 19 100399 Google Scholar
[2]	Zhou W, Gong H M, Jin X H, Chen Y, Li H M, Liu S 2022 Front. Physics 10 842789 Google Scholar
[3]	Kaur R, Singh K, Tripathi S 2022 J. Alloy. Compd. 905 164103 Google Scholar
[4]	Cui Z, Wang H X, Shen Y, Qin K, Yuan P, Li E L 2024 Mater. Today Phys. 40 101317 Google Scholar
[5]	Li F, Xu B, Yang W, Qi Z Y, Ma C, Wang Y J, Zhang X H, Luo Z R, Liang D L, Li D 2020 Nano Res. 13 1053 Google Scholar
[6]	Yan Q J, Cheng J X, Wang W K, Sun M J, Yin Y L, Peng Y H, Zhou W C, Tang D S 2022 J. Phys. Condes. Matter 34 475703 Google Scholar
[7]	Zhao P, Cheng R, Zhao L, Yang H J, Jiang Z Y 2023 J. Appl. Phys. 134 134302 Google Scholar
[8]	Kalkan S B, Najafidehaghani E, Gan Z, Apfelbeck F A C, Hübner U, George A, Turchanin A, Nickel B 2021 npj 2D Mater. Appl. 5 92 Google Scholar
[9]	邓霖湄, 司君山, 吴绪才, 张卫兵 2022 71 147101 Google Scholar Deng L M, Si J S, Wu X C, Zhang W B 2022 Acta Phys. Sin. 71 147101 Google Scholar
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[17]	Zhan W Y, Zou J P, Xu M, Lei T, Wei H M 2023 Trans. Nonferrous Met. Soc. China 33 2483 Google Scholar
[18]	Zhu X B, Jiang X, Yao X Y, Leng Y X, Xu X X, Peng A P, Wang L P, Xue Q J 2019 ACS Appl. Mater. Interfaces 11 45726 Google Scholar
[19]	Yaqub T B, Vuchkov T, Sanguino P, Polcar T, Cavaleiro A 2020 Coatings 10 133 Google Scholar
[20]	Yaqub T B, Kannur K H, Vuchkov T, Pupier C, Héau C, Cavaleiro A 2020 Mater. Lett. 275 128035 Google Scholar
[21]	Li N, Liu Z T, Feng L P, Jia R T 2016 Surf. Eng. 32 299 Google Scholar
[22]	Mao X, Li Z Q, Zou J P, Zhao G Y, Li D N, Song Z Q 2019 Appl. Surf. Sci. 487 719 Google Scholar
[23]	Wu Q L, Fu X S, Yang K, Wu H Y, Liu L, Zhang L, Tian Y, Yin L J, Huang W Q, Zhang W, Wong P K J, Zhang L J, Wee A T S, Qin Z H 2021 ACS Nano 15 4481 Google Scholar
[24]	Franklin A D 2015 Science 349 704 Google Scholar
[25]	Chang Y S, Chen C Y, Ho C J, Cheng C M, Chen H R, Fu T Y, Huang Y T, Ke S W, Du H Y, Lee K Y 2021 Nano Energy 84 105922 Google Scholar
[26]	Thureja D, Imamoglu A, Smoleński T, Amelio I, Popert A, Chervy T, Lu X, Liu S, Barmak K, Watanabe K 2022 Nature 606 298 Google Scholar
[27]	Chouki T, Donkova B, Aktarla B, Stefanov P, Emin S 2021 Mater. Today Commun. 26 101976 Google Scholar
[28]	Upadhyay S, Pandey O 2021 J. Alloy. Compd. 857 157522 Google Scholar
[29]	Jäger-Waldau A, Lux-Steiner M, Jäger-Waldau R, Burkhardt R, Bucher E 1990 Thin Solid Films 189 339 Google Scholar
[30]	李健, 朱洁 2007 56 574 Google Scholar Li J, Zhu J 2007 Acta Phys. Sin. 56 574 Google Scholar
[31]	毛启楠, 张晓勇, 李学耕, 贺劲鑫, 于平荣, 王东 2014 63 118802 Google Scholar Mao Q N, Zhang X Y, Li X G, He J X, Yu P R, Wang D 2014 Acta Phys. Sin. 63 118802 Google Scholar
[32]	Sharma C, Srivastava A K, Gupta M K 2023 Physica B 669 415290 Google Scholar
[33]	Zeng F, Kong W Y, Liang Y H, Li F, Lvtao Y Z, Su Z H, Wang T, Peng B G, Ye L F, Chen Z H, Gao X Y, Huang J, Zheng R K, Yang X D 2023 Adv. Mater. 35 2306051 Google Scholar
[34]	Mittal H, Raza M, Khanuja M 2023 MethodsX 11 102409 Google Scholar
[35]	Kandar S, Bhatt K, Kumar N, Kapoor A K, Singh R 2024 ACS Appl. Nano Mater. 7 8212 Google Scholar
[36]	Tao S M, Ma J F, Liu J J, Wang Y R, Xiao J R 2024 Int. J. Hydrog. Energy 58 829 Google Scholar
[37]	Ohtake A, Sakuma Y 2021 J. Phys. Chem. C 125 11257 Google Scholar
[38]	Shi N X, Liu G Z, Xi B J, An X G, Sun C H, Xiong S L 2024 Nano Res. 17 4023 Google Scholar
[39]	Wang X, Gong Y, Shi G, Chow W L, Keyshar K, Ye G, Vajtai R, Lou J, Liu Z, Ringe E 2014 ACS Nano 8 5125 Google Scholar
[40]	Zhao S D, Lu M L, Xue S S, Yan L, Miao P, Hang Y, Wang X J, Liu Z G, Wang Y, Tao L, Sui Y, Wang Y 2019 arXiv: 1904.09789 [cond-mat.mtrl-sci]
[41]	Ahmad Y H, Kamand F Z, Zekri A, Chae K J, Aïssa B, Al-Qaradawi S Y 2023 Appl. Surf. Sci. 626 157205 Google Scholar
[42]	Liu H L, Yang T, Chen J H, Chen H W, Guo H H, Saito R, Li M Y, Li L J 2020 Sci Rep 10 15282 Google Scholar
[43]	Wang Z, Chen Y F, Wu P S, Ye J F, Peng M, Yan Y, Zhong F, He T, Wang Y, Xu M J 2020 Infrared Phys. Technol. 106 103272 Google Scholar
[44]	黄静雯, 罗利琼, 金波, 楚士晋, 彭汝芳 2017 66 137801 Google Scholar Huang J W, Luo L Q, Jin B, Chu S J, Peng R F 2017 Acta Phys. Sin. 66 137801 Google Scholar
[45]	Zhang X L, Zhou J, Li S Q, Wang Y Y, Zhang S P, Liu Y L, Gao J F, Zhao J J, Wang W P, Yu R C 2021 J. Phys. Chem. Lett. 12 5879 Google Scholar

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硒化温度对MoSe₂薄膜结构和光学带隙的影响