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研究生： 梁家瑜
Liang, Chia-Yu
論文名稱： 共濺鍍法合成高熵高介電常數氮摻雜 (Al,Ta,Zr,Hf,Ti)OX 介電層應用於 ZnSnO 薄膜電晶體以及光感測器
Cosputtering Synthesis of High-entropy-high-k N-doped (Al,Ta,Zr,Hf,Ti)OX Dielectrics Applied to ZnSnO-based Thin Film Transistors and Photosensors
指導教授： 張高碩
Chang, Kao-Shou
學位類別： 碩士
Master
系所名稱： 工學院 - 材料科學及工程學系
Department of Materials Science and Engineering
論文出版年： 2024
畢業學年度： 112
語文別： 英文
論文頁數： 109
中文關鍵詞： 共濺鍍 、氮摻雜 (Al,Ta,Zr,Hf,Ti)OX 、ZnSnO 、薄膜電晶體 、可撓式紫外光感測器
外文關鍵詞： Cosputtering, N-doped (Al,Ta,Zr,Hf,Ti)OX, ZnSnO, thin film transistor, flexible UV sensor
相關次數： 點閱：157  下載：0 
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    • 在 ITO/玻璃基板上通過共濺鍍方法使用 Al 和 (Ta,Zr,Hf,Ti) 兩個靶材製備了氮摻雜 (Al,Ta,Zr,Hf,Ti)Ox 薄膜。為確保薄膜的均勻沉積，在沉積過程中旋轉 ITO/玻璃基板。該薄膜的能帶結構通過混合密度泛函理論(hybrid-DFT)進行了理論研究，顯示其能帶結構適合用作薄膜電晶體 (TFT) 的閘極介電層。高通量的 X 射線熒光(XRF)和 X 射線衍射(XRD)結果分別顯示了所有組成元素的均勻分佈以及無結晶結構的形成。
    為研究氮摻雜 (Al,Ta,Zr,Hf,Ti)Ox 薄膜的介電特性，將其應用到金屬 (ITO)-絕緣體-金屬 (Al) 電容器中，並進行合成氣體(FGA)退火處理（350°C，60 分鐘，1 托），以優化薄膜品質並提高性能。利用透射電子顯微鏡 (TEM) 分析評估了薄膜厚度，並確定了相關的 k 值（在 1 kHz-100 kHz 下約為 30）。最大漏電流在 2 V 下約為 10-7.5 A/cm²。
    為評估其在電子器件中的應用，將薄膜製作成 TFT 閘極介電層，並使用 ZnSnO 作為通道層。所製備的 TFT 表現出優異的輸出和轉移特性，具有約 107 的開關比、約 0.085 V/dec 的次臨界擺幅 (S.S.)、約 0.09 V 的閾值電壓 (VT)、約 112.91 cm²/V·s 的飽和遷移率 (μsat) 和約 2.18×1011 eV-1cm-2的界面陷阱密度 (Dit)；其性能優於文獻中報導的基於其他介電層的 ZnSnO TFT。該 TFT 還應用於電子板上的開關，以控制 LED 的開關。
    所製備的 TFT 也用於 350 nm、300 nm 和 253 nm 照射下的紫外光感測器。穩定性由循環研究表明。相關的靈敏度 (S ≈ 106) 和響應度 (R ≈ 1024.2 A/W) 以及響應時間顯著優於文獻中報導的紫外光感測器。
    此外，還在PI 基板上製造TFT，它們在不同的彎曲程度下仍然顯示出卓越的性能，包括穩定性、飽和遷移率 (μsat)、次臨界擺幅 (S.S.)、閾值電壓 (VT)、界面陷阱密度 (Dit)、響應度 (R) 和靈敏度 (S)，支持其在可撓式電子元件中的巨大潛力。
    實驗確定了所製備的 TFT 的能帶結構。氮摻雜 (Al,Ta,Zr,Hf,Ti)Ox 和 ZnSnO 之間的導帶偏移 (約 1.75 eV) 足夠高，可防止不必要的漏電流。由於 ITO 的費米能級低於 ZnSnO，ZnSnO 的導帶和價帶分別向下彎曲（約 0.13 eV）。所得到的能帶圖用於闡明正閘極偏壓應力不穩定性 (PGBSI)、負閘極偏壓應力不穩定性 (NGBSI)、正閘極偏壓照明應力不穩定性 (PGBISI)、負閘極偏壓照明應力不穩定性 (NGBISI) 和正閘極偏壓溫度應力不穩定性 (PGBTSI) 的影響。

    N-doped (Al,Ta,Zr,Hf,Ti)OX films on ITO/glass substrates were fabricated using two targets of Al and (Ta,Zr,Hf,Ti) through cosputtering. To ensure the uniform deposition of the film, an ITO/glass substrate was rotated during the deposition. The film was theoretically studied through a hybrid-density functional theory, which revealed that its energy band structure is suitable for gate dielectrics in thin film transistors (TFTs). High-throughput X-ray fluorescence and X-ray diffraction results revealed that all constituent elements uniformly distributed and the formation of amorphous structures, respectively.
    To investigate the dielectric properties of N-doped (Al,Ta,Zr,Hf,Ti)OX, it was integrated into a metal (ITO)-insulator-metal (Al) capacitor and forming gas annealing (350 °C, 60 min, and 1 Torr) was applied to optimize the film quality and enhance the performance. TEM analysis was employed to evaluate the film thickness and the associated k values were then determined (approximately 30 at 1 kHz-100 kHz). The maximum leakage current was approximately 10-7.5 A/cm² at 2 V.
    To evaluate application in electronic devices, the film was patterned into TFTs as gate dielectrics using ZnSnO as a channel layer. The resulting TFT exhibited excellent output and transfer characteristics, with an on/off ratio of approximately 10⁷, subthreshold swing (SS) of approximately 0.085 V/dec, threshold voltage (VT) of approximately 0.09 V, mobility () of approximately 112.91 cm²/V·s, and interfacial trap density (Dit) of approximately 2.18×1011 eV-1cm-2; the performance was superior to other dielectrics-based ZnSnO TFTs reported in literature. The TFT was also applied to a switch on an electronic board to control a LED turning on and off.
    The resulting TFT was also applied to a UV sensor under 350-, 300-, and 253-nm illumination. The stability is indicated by a cyclic study. Associated sensitivity (S  106) and responsivity (R  1024.2 A/W) and response times distinctly outperform those reported UV sensors in literature.
    Furthermore, the TFTs were also fabricated on flexible polyimide (PI) substrates, and they still exhibited outstanding performances, including stability, sat, SS, VT, Dit, R, and S, under various bending levels, supporting their great potential for flexible electronic devices.
    An energy band of the resulting TFT was experimentally determined. The conduction band offset between N-doped (Al,Ta,Zr,Hf,Ti)OX and ZnSnO is high enough (approximately 1.75 eV), preventing undesirable leakage current. Because the Efermi of ITO is lower than that of ZnSnO, the conduction band and valence band of ZnSnO was then banding downward (approximately 0.13 eV). The resulting energy band diagram was employed to elucidate effects of positive gate bias stress instability (PGBSI), negative gate bias stress instability (NGBSI), positive gate bias illumination stress instability (PGBISI), negative gate bias illumination stress instability (NGBISI), and positive gate bias temperature stress instability (PGBTSI)

    摘要 I Abstract III 致謝 V Contents VI Figure Contents X Chapter 1 Introduction 1 1.1 Overview 1 1.1.1 Dielectric layer 2 1.1.2 Motivation 4 1.2 MIM capacitor overview 5 1.2.1 Capacitance measurement 6 1.2.2 C-V characteristics 7 1.2.3 I-V characteristics 8 1.3 Thin film transistor (TFT) overview 9 1.3.1 TFT structure 10 1.3.2 Operation principle of TFT devices 11 1.3.3 TFT parameter extraction and calculation 13 1.4 High-k Gate dielectrics 16 1.4.1 High-k Gate dielectrics requirement 16 1.5 TFT application to UV sensors 18 1.5.1 TFT-based sensor 18 1.5.2 ZnSnO TFT UV sensor 20 1.6 High entropy oxide 22 1.6.1 High entropy alloys 22 1.6.2 High entropy effect 22 1.6.3 Application for high entropy oxides 24 Chapter 2 Experimental methods 29 2.1 Materials 29 2.1.1 Target for sputtering 29 2.1.2 Substrate 30 2.1.3 Sputtering gas 30 2.2 Equipment 31 2.2.1 Ultrasonic cleaner 31 2.2.2 Magnetron sputtering 32 2.2.3 Tube furnace 33 2.2.4 Muffle furnace 33 2.3 MIM capacitor fabrication 34 2.3.1 Substrate cleaning 34 2.3.2 High entropy oxide deposition 35 2.3.3 Electrode (Al) deposition 35 2.3.4 Forming gas annealing (FGA) 37 2.4 Thin film transistor (TFT) fabrication 37 2.4.1 ZnSnO channel layer deposition 38 2.4.2 Muffle furnace annealing 39 2.4.3 Source/Drain electrode deposition 39 2.5 Characterization 41 2.5.1 Electrical probe station 41 2.5.2 Capacitance-Voltage (C-V) measurement 42 2.5.3 Current-Voltage (I-V) measurement 43 2.5.4 X-ray photoelectron spectroscopy (XPS) 43 2.5.5 Ultraviolet photoelectron spectroscopy (UPS) 44 2.5.6 Focused ion beam (FIB) 44 2.5.7 Transmission Electron Microscopy (TEM) 45 2.5.8 X-ray Diffraction (XRD) 46 2.5.9 X-ray Fluorescence (XRF) Spectroscopy 47 2.5.10 Ultraviolet-Visible (UV-Vis) Spectroscopy 48 Chapter 3 Results and discussion 49 3.1 HEO Film optimization 49 3.1.1 Forming gas annealing (FGA) 49 3.1.2 FGA temperature 49 3.1.3 FGA time 51 3.1.4 FGA pressure 52 3.1.5 Comparison before and after FGA 53 3.1.6 Consistency of the N-doped (Al,Ta,Zr,Hf,Ti)OX thin film 54 3.2 X-ray fluorescence (XRF) analysis 56 3.3 X-ray diffraction (XRD) analysis 57 3.4 X-ray photoelectron spectroscopy (XPS) 58 3.4.1 N-doped (Al,Ta,Zr,Hf,Ti)OX thin film XPS spectrum 58 3.4.2 ZnSnO thin film XPS spectrum 59 3.5 Transmission Electron Microscopy (TEM) 60 3.6 Electrical properties of N-doped (Al,Ta,Zr,Hf,Ti)OX-based ZnSnO TFTs 62 3.6.1 Transfer and output characteristics of TFTs 62 3.6.2 Consistency of TFTs 63 3.6.3 Band diagram 65 3.6.3.1 Theoretical calculation 65 3.6.3.2 Measurement result 66 Bias stress stability 68 3.6.3.3 PGBSI /PGBISI 69 3.6.3.4 NGBSI/NGBISI 70 3.6.3.5 PGBTSI 72 3.6.3.6 Kinetics 73 3.7 N-doped (Al,Ta,Zr,Hf,Ti)OX-based ZnSnO TFT Ultraviolet (UV) sensor 75 3.8 Flexible N-doped (Al,Ta,Zr,Hf,Ti)OX-based ZnSnO TFT UV sensor 78 Chapter 4 Conclusions and future work 82 Chapter 5 References 86

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