臺灣博碩士論文加值系統

本論文探討利用二階段式化學氣相沉積法於二氧化矽/矽基板上成長二硫化鉬薄膜並分析其壓阻特性，利用直流磁控濺鍍系統先在基板上成長厚度為2奈米之鉬薄膜，後續在不同溫度下進行硫化形成二硫化鉬薄膜。以550 °C為基準進行後續實驗，最後試著將二硫化鉬薄膜製作成壓阻元件並使用田口式直交表規劃實驗參數，以應變係數(Gauge Factor)進行最佳化分析，其最佳化參數組合為硫粉重量0.6 g(A3)、氫氣:氬氣為20:200 sccm(B3)、製程時間45分鐘(C3)和製程壓力10 Torr(D3)，所製備樣品的最大GF為37.6、片電阻為496 k。樣品由拉曼光譜解析，A1g與E2g譜峰差約為27.4 cm-1，約為十層的MoS2，且從光學顯微鏡可以觀察到薄膜均勻覆蓋表面。而後使用對甲苯磺酸水化合物(PTSA)摻雜的方式改變其壓阻特性，並以拉曼光譜、霍爾量測以及X光光電子能譜分析其改善原因。發現隨著PTSA莫爾濃度由0.2上升至1.6 M、浸泡時間由1小時增加至16小時，PTSA的表面電荷轉移會使費米能階往導帶偏移，這可從拉曼光譜與XPS峰值的位置得知。MoS2於1.6 M PTSA濃度下摻雜16小時發現摻雜濃度從3.12×1017 cm-3上升至9.44×1018 cm-3，遷移率從2.89 cm2/Vs下降至0.15 cm2/Vs，GF上升至83。

In this thesis, molybdenum disulfide (MoS2) films were deposited on SiO2/Si substrate by two-step chemical vapor deposition and its piezoresistive properties were investigated. First, a 2-nm molybdenum film was deposited on the substrate using a DC magnetron sputtering. After that, the Mo film was sulfurized at various temperatures to synthesize the MoS2 film. The MoS2 film synthesized at 550 oC were appropriate for the subsequent experiments. The Taguchi method was used to optimize the gauge factor (GF) of the MoS2 film. The results indicated that the MoS2 films with sulfur weight of 0.6 g(A3), flow rate of H2:Ar were 20:200 sccm(B3), growth time of 45 minutes(C3), and growth pressure of 10 Torr(D3) had the largest GF of 37.6 and Rsh of 496 k. The Raman spectrum of the optimized MoS2 film had A1g peak of 382.91 cm-1 and E2g peak of 410.31 cm-1. The difference between these two peaks was 27.4 cm-1, indicated the MoS2 film had a 10-layers structure. Optical microscopy also showed the MoS2 film were uniform. The GF of the MoS2 film was improved by chemical doping with Para-Toluene-Sulfonic Acid (PTSA). With increasing the molar concentration from 0.2 to 1.6 M and treatment time from 1 to 16 hours, the shifts of peak position of Raman spectra and X-ray photoelectron spectra were observed. The PTSA treatment caused a relative shift of the Fermi level towards the conduction band edge, suggesting a n-doping effect in the MoS2 films. While the MoS2 film was treated in 1.6 M PTSA for 16 hours, its carrier concentration was increased from 3.12×1017 to 9.44×1018 cm-3, its carrier mobility was decreased from 2.89 to 0.15 cm2/Vs, and its gauge factor was increased to 83.

中文摘要 I
ABSTRACT II
誌謝 IV
目錄 V
圖目錄 VII
表目錄 X
第一章 緒論 1
1-1 前言 1
1-2 動機與目的 1
1-3 論文架構說明 2
第二章 基礎理論與文獻回顧 3
2-1 二維材料簡介 3
2-2 二硫化鉬 4
2-2-1 二硫化鉬簡介 4
2-2-2 二硫化鉬物理特性 4
2-2-3 二硫化鉬製備方式 7
2-2-4 二硫化鉬檢測方法 10
2-3 化學氣相沉積製備二硫化鉬 13
2-3-1 化學氣相沉積原理 13
2-3-2 氣體流量的影響 15
2-3-3 壓力的影響 15
2-3-4 溫度的影響 16
2-3-5 S/Mo比的影響 17
2-4 鉬源對成長二硫化鉬影響 17
2-5 直接成長免轉移二硫化鉬製備 20
2-6 田口方法介紹 21
2-7 壓阻效應 22
2-8 摻雜效應(Doping Effect) 22
2-8-1 電荷轉移摻雜(Charge Transfer Doping) 23
2-8-2 置換摻雜(Substitutional Doping) 24
第三章 實驗步驟與方法 25
3-1 實驗敘述與流程說明 25
3-2 實驗設備 25
3-3 二硫化鉬製備說明 28
3-4 材料分析 31
第四章 結果與討論 35
4-1 低溫製備免轉移二硫化鉬 35
4-2 二硫化鉬化學摻雜 44
第五章 結論與未來展望 58
5-1結論 58
5-2未來展望 59
參考文獻 60

[1]S. S. Prasad, R. K. Mishra, and S. Gupta et al., "Introduction, history, and origin of two dimensional (2D) materials." Advanced Applications of 2D Nanostructures: Emerging Research and Opportunities, pp 1-9. Aug 2021.
[2]H. M. Yehia, A. I. Ali, and E. Abd-Elhameed, "Effect of exfoliated MoS2 on the microstructure, hardness, and tribological properties of copper matrix nanocomposite fabricated via the hot pressing method." Transactions of the Indian Institute of Metals,vol. 76, pp. 195-204,Sep 2023.
[3]C. Liu, Y. Zheng, Z. Zeng, and R. Li, "Polarization-resolved analysis of high-order harmonic generation in monolayer MoS2." New Journal of Physics,vol. 22, p. 073046, Jul 2020.
[4]Y. Xiao, M. Zhou, and J. Liu et al., "Phase engineering of two-dimensional transition metal dichalcogenides." Science China Materials, vol 62, pp 759-775. Feb 2019.
[5]A.Taffelli, S. Dirè, and A. Quaranta et al., "MoS2 based photodetectors: a review." Sensors, vol. 21, pp 2758. Apr 2021.
[6]W. Li, Y. Zhang, and X. Long et al., "Gas sensors based on mechanically exfoliated MoS2 nanosheets for room-temperature NO2 detection." Sensors,vol. 19, pp 2123. May 2019.
[7]S. K. Lee, D. Chu, and J. Yoo et al., "Formation of transition metal dichalcogenides thin films with liquid phase exfoliation technique and photovoltaic applications." Solar Energy Materials and Solar Cells,vol .184, pp 9-14. Apr 2018.
[8]A. K. Gautam, M. Faraz, and N. Khare, "Enhanced thermoelectric properties of MoS2 with the incorporation of reduced graphene oxide (RGO)." Journal of Alloys and Compounds, vol 838, p 155673. Oct 2020.
[9]N. Thomas, S. Mathew, and K. M. Nair et al., "2D MoS2: structure, mechanisms, and photocatalytic applications." Materials Today Sustainability, vol 13, p 100073. Sep 2021.
[10]F. Chen, Q. Lv, and Y. Xia et al., "Two-dimensional bilayer MoS2 flakes with variable size of the upper layer grown by chemical vapor deposition." Micro and Nanostructures, vol 169, p 207358. Sep 2022.
[11]S. Golovynskyi, I. Irfan, and M. Bosi et al., "Exciton and trion in few-layer MoS2: Thickness-and temperature-dependent photoluminescence." Applied Surface Science, vol 515, p 146033. Jun 2020.
[12]H. Cun, M. Macha, and H. Kim et al., "Wafer-scale MOCVD growth of monolayer MoS2 on sapphire and SiO2." Nano Research, vol 12, pp 2646-2652. Aug 2019.
[13]C. R. Wu, X. R. Chang, and C. H. Wu et al., "The growth mechanism of transition metal dichalcogenides by using sulfurization of pre-deposited transition metals and the 2D crystal hetero-structure establishment." Scientific reports, vol 7, pp 1-8. Feb 2017.
[14]C. M. Hyun, J. H. Choi, and S. W. Lee et al., "Synthesis mechanism of MoS2 layered crystals by chemical vapor deposition using MoO3 and sulfur powders." Journal of Alloys and Compounds, vol 765, pp 380-384. Oct 2018.
[15]M. Fang, F. Wang, and Y. Han et al., "Controlled growth of bilayer‐MoS2 films and MoS2‐based field‐effect transistor (FET) performance optimization." Advanced Electronic Materials, vol 4, p 1700524. Mar 2018.
[16]P. Tummala, A. Lamperti, and M. Alia et al., "Application-oriented growth of a molybdenum disulfide (MoS2) single layer by means of parametrically optimized chemical vapor deposition." Materials, vol 13, pp 2786. Jun 2020.
[17]Z. Zhu, S. Zhan, and J. Zhang et al., "Influence of growth temperature on MoS2 synthesis by chemical vapor deposition." Materials Research Express, vol 6, p 095011. Jul 2019.
[18]J. Xu, and D. Ho, "Modulation of the Reaction Mechanism via S/Mo: A Rational Strategy for Large-Area MoS2 Growth." Chemistry of Materials, vol 33, pp 3249-3257. Apr 2021.
[19]S. S. Withanage, M. Lopez, and W. Sameen et al., "Elucidation of the growth mechanism of MoS2 during the CVD process." MRS Advances, vol 4, pp 581-586. Dec 2018.
[20]Y. Jeong, J. Y. Sung, and Y. Choi et al., "Structural characterization and transistor properties of thickness-controllable MoS2 thin films." Journal of Materials Science, vol 54, pp 7758-7767. Feb 2019.
[21]J. Lee, H. Jang, and T. Kwak et al., "Comparison of MoS2/p‐GaN Heterostructures Fabricated via Direct Chemical Vapor Deposition and Transfer Method." physica status solidi (a), vol 217, p 1900722. Dec 2019.
[22]Z. Lin, Y. Zhao, and C. Zhou et al., "Controllable growth of large–size crystalline MoS2 and resist-free transfer assisted with a Cu thin film." Scientific reports, vol 5, pp 1-10. Dec 2015.
[23]J. Li, and M. Östling, "Scalable fabrication of 2D semiconducting crystals for future electronics." Electronics, vol 4, pp 1033-1061. Dec 2015.
[24]J. Pető, G. Dobrik, and G. Kukucska et al., "Moderate strain induced indirect bandgap and conduction electrons in MoS2 single layers." npj 2D Materials and Applications, vol 3, pp 39. Oct 2019.
[25]P.Luo, F. Zhuge, and Q. Zhang et al., "Doping engineering and functionalization of two-dimensional metal chalcogenides." Nanoscale Horizons, vol 4, pp 26-51. Aug 2018.
[26]F. S.Oliveira, R. B. Cipriano, and F. T. da Silva et al., "Simple analytical method for determining electrical resistivity and sheet resistance using the van der Pauw procedure. " Scientific Reports, vol 10, pp 16379. Oct 2020.
[27]D. Collomb, P. Li, and S. Bending, "Frontiers of graphene-based Hall-effect sensors. " Journal of Physics: Condensed Matter, vol 33, p 243002. May 2021.
[28]M. Zhu, K. Sakamoto, and J. Li et al., "Piezoresistive strain sensor based on monolayer molybdenum disulfide continuous film deposited by chemical vapor deposition." Journal of Micromechanics and Microengineering, vol 29, p 055002. Mar 2019.
[29]Y. ZHAO, K. Xu, F. Pan et al., "Doping, contact and interface engineering of two‐dimensional layered transition metal dichalcogenides transistors." Advanced Functional Materials, vol 27, p 1603484. Dec 2016.
[30]C. H. Chen, C. L. Wu, J. Pu et al., "Hole mobility enhancement and p-doping in monolayer WSe2 by gold decoration. 2D Materials", vol 1, p 034001. Oct 2014.
[31]S. Yang, Y. Chen, and C. Jiang, “Strain engineering of two‐dimensional materials: methods, properties, and applications.” InfoMat, vol 3, pp 397-420. Mar 2021.
[32]F. Li, T. Shen, C. Wang, and Y. Zhang, “Recent advances in strain-induced piezoelectric and piezoresistive effect-engineered 2D semiconductors for adaptive electronics and optoelectronics”. Nano-Micro Letters, vol 12,pp 1-44. May 2020
[33]B. Chamlagain, S. S. Withanage, and A. C. Johnston et al., “Scalable lateral heterojunction by chemical doping of 2D TMD thin films.” Scientific Reports, vol 10, p 12970. Jul 2020.