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研究生： 李承訓
Li, Cheng-Hsun
論文名稱： 以射頻濺鍍法製備ZnGa2O4 薄膜及其光電元件應用
Investigation of Zinc gallate Thin Film Fabricated by RF Sputtering System and Their Optoelectronics Applications
指導教授： 張守進
Chang, Shoou-Jinn
學位類別： 碩士
Master
系所名稱： 電機資訊學院 - 微電子工程研究所
Institute of Microelectronics
論文出版年： 2019
畢業學年度： 107
語文別： 英文
論文頁數： 119
中文關鍵詞： 光檢測器 、光電晶體 、薄膜電晶體 、雙層主動層
外文關鍵詞： Zinc gallate, photodetector, phototransistor, thin film transistor, double-stacked channel layer
相關次數： 點閱：72  下載：0 
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    • 本篇論文為利用射頻磁控濺鍍法沉積ZnGa2O4薄膜，探討不同製程條件下薄膜特性，並將其應用於光感測器之感測層及薄膜電晶體之通道層，並討論元件特性及電性分析。
    在實驗的第一部分，我們以磁控濺鍍法沉積不同氧氣分壓之ZnGa2O4薄膜，並藉由熱退火製程優化薄膜特性。我們從三大面向去討論薄膜的性質，分別是薄膜結構、光學特性、表面及縱深分析。在薄膜結構分析中，ZnGa2O4薄膜表面緻密，且由XRD量測發現隨著退火溫度上升，結晶相強度顯著增加，半高寬越小，顯示薄膜結晶性更好；在薄膜光學特性中，顯示薄膜在可見光區域有85%以上的穿透率，從EDS結果分析，ZnGa2O4薄膜鎵元素的占比很高，使其成為一種寬能隙的材料，主要吸收極紫外光波段；在薄膜表面分析中，藉由AFM量測發現薄膜表面粗糙度很小，對於元件中電子的傳輸十分有利；在薄膜縱深分析中，藉由X射線光電子能譜（XPS）圖發現，當氧氣分壓比例上升時，薄膜之中的氧空缺會因此減少，顯示載子數目降低。
    在實驗的第二部分，將所製備的ZnGa2O4薄膜應用於光檢測器，並改變射頻濺鍍之氧通量、熱退火之溫度作為調變製程的參數，比較其對於元件光電特性的影響。隨著氧流量的提高，元件的光暗電流都顯著下降，因為在濺鍍的過程中薄膜內的氧空缺被製程氧氣填補，造成薄膜載子數目降低，另外，我們也發現氧空缺對於元件開關特性的影響。再來，透過適當的熱退火處理，能提升元件之光電流，並降低暗電流，因此提升光暗電流比，也增強光響應。一般來說，熱退火製程能有效減少薄膜子能隙缺陷，增強晶格鍵結，使原子重新排列。最後，透過製程優化並找到元件製作的最佳參數，發現氧流量比例0%並於真空中進行熱退火200oC的ZnGa2O4光檢測器有最佳的特性，ON/OFF電流比大於108，響應值為0.203 A/W，響應拒斥比為1.23×10^5。
    在實驗的第三部分，實現了以二氧化矽(SiO2)作為閘極介電層的ZnGa2O4薄膜電晶體，藉由調變通道層厚度，製備元件最佳參數。首先，我們發現單層通道層的元件最佳厚度約為30奈米，在室溫下得到場效電子遷移率為0.14 cm^2/V∙s，臨界電壓為3.28 V，次臨界擺幅為0.31 V/dec，ON/OFF電流比為6.48×10^5。最後，將薄膜電晶體的應用延伸到光電晶體，施加偏壓-2 V的情況下，響應拒斥比為2.30×10^4。
    另外，我們利用不同氧比例的薄膜堆疊技術，獲得高性能ZnGa2O4雙重堆疊通道層結構之薄膜電晶體，此結構有更優異的介面品質並減少通道層塊材缺陷，降低電子表面散射，對元件的特性大幅改善。我們也成功利用能帶圖解釋其物理機制。在室溫下得到場效電子遷移率為534 cm2/V∙s，臨界電壓為1.01 V，次臨界擺幅為0.09 V/dec，ON/OFF電流比為1.37×10^8。

    In this thesis, Zinc gallate (ZnGa2O4) is grown by RF sputtering system and the film properties are investigated under different processing ambiences. Next, the ZnGa2O4 thin films will be used as active layer for optoelectronics devices such as UV photodetectors (PDs) and thin film transistors (TFTs). Finally, the electrical analyses and properties of the devices are discussed in detail.
    First, we deposited ZnGa2O4 films with different oxygen partial pressures and optimized the film properties by thermal annealing process. Besides, ZnGa2O4 films are studied from the three aspects such as structural, optical, surface/depth analysis. In the structural analysis, the X-ray diffraction (XRD) reveals that as the annealing temperature increases, the crystalline phase strength increases remarkably and the full width at half maximum (FWHM) becomes narrowly, indicating that the film has better crystallinity. In the optical analysis, the films exhibit a transmittance of more than 85% in the visible light region. Furthermore, according to the EDS results, the ZnGa2O4 film has a high proportion of gallium, making it become a wide-bandgap material. The bandgap is approximately calculated to 5 eV, which absorbs ultraviolet light. In the surface analysis, the surface of the film is very smooth by AFM measurement, leading to lower interfacial trap densities between dielectric layer and channel layer, which is beneficial to the electron transport. In the depth analysis, the X-ray photoelectron spectroscopy (XPS) shows that the oxygen vacancies in the film are reduced as the oxygen flow ratio increased, meaning the number of carriers is decreased.
    Second, the prepared ZnGa2O4 film was applied to a photodetector. By simply adjusting the oxygen flow ratio and thermal annealing temperature, we investigate the influence on the optoelectronics properties of the device. With higher oxygen flow ratio, the dark current and photocurrent drop significantly, since the oxygen vacancies in the film are filled up during the sputtering process, resulting in less carrier concentration. In addition, we also found the effect of oxygen vacancies on the switching characteristics. Furthermore, we can not only increase the photocurrent, but also decrease the dark current by annealing process, thus increasing the on/off current ratio and enhancing the photoresponse. In fact, proper annealing temperature can effectively reduce sub-gap defects, enhance lattice bonding, and rearrange atoms. Lastly, the photodetector manufactured under oxygen flow ratio of 0% and annealed at 200oC for 1 hour has the best performance with on/off current ratio greater than 108, responsivity of 0.203 A/W, and UV-to-visible rejection ratio of 1.23 × 105.
    Third, ZnGa2O4 TFTs with silicon dioxide as the gate dielectric layer were realized. By controlling the thickness of the active layer, we found that the optimized thickness of the devices is 30 nm. The data extracted from transfer characteristics exhibit field-effect electron mobility of 0.14 cm2/V∙s, threshold voltage of 3.28 V, subthreshold swing of 0.31 V/decade, and on/off current ratio of 6.48×105. Moreover, we broaden the applicability of ZnGa2O4 TFTs to phototransistors, and the UV-to-visible rejection ratio was 9.80 × 103 at the bias voltage of -2 V.
    Fourth, we obtained extremely high performance ZnGa2O4 TFTs with a bandgap-engineered double-stacked channel layer structure using different oxygen ratio thin film stacking technology. The homogeneous double-stacked channel layer (DSCL) structure has superior interface quality and fewer bulks traps, reducing surface scattering and improving the characteristics. The mechanism is also successfully explained by the band diagram. The field effect electron mobility was 534 cm2/V∙s, the threshold voltage was 1.01 V, the subthreshold swing was 99 mV/decade, and the on/off current ratio was 1.37×108.

    Keyword：ZnGa2O4 (Zinc gallate); photodetector; phototransistor; thin film transistor; double-stacked channel layer

    摘要 1 Abstract 4 誌謝 7 Content 8 Table Captions 11 Figure Captions 12 Chapter 1 Introduction 16 1.1 Background and Motivation 16 1.2 Background of ZnGa2O4 Material 17 1.3 Overview of Ultraviolet Photodetectors 19 1.4 Overview of Thin Film Transistor 20 1.5 Organization of This Thesis 21 Reference 23 Chapter 2 Relevant Theory and Experimental Equipment 29 2.1 Theory of Photodetector 29 2.1.1 Responsivity of the Photodetector 30 2.2 Theory of Thin Film Transistor 31 2.2.1 Threshold Voltage (Vth) 32 2.2.2 Field-Effect Mobility 33 2.2.3 On/off Current Ratio (Ion/Ioff) 34 2.2.4 Subthreshold Swing (SS) 34 2.2.5 Interface Trap Density (Nit) 35 2.3 Experimental Equipment 35 2.3.1 RF Sputtering System 35 2.3.2 Plasma-enhance Chemical Vapor Deposition (PECVD) 38 2.3.3 X-ray Diffraction Analysis (XRD) 40 2.3.4 Atomic Force Microscopes 42 2.3.5 Energy-Dispersive X-ray Spectroscopy (EDS) 42 2.3.6 X-ray Photoelectron Spectroscopy (XPS) 44 2.3.7 Measurement Systems 45 Reference 46 Chapter 3 Characteristics of ZnGa2O4 thin film 48 3.1 Growth of ZnGa2O4 Thin Film 48 3.2 Structural Characteristics 50 3.2.1 X-ray Diffraction (XRD) Analysis 50 3.2.2 Atomic Force Microscopy (AFM) Analysis 53 3.2.3 Transmission electron microscope (TEM) Analyses 55 3.3 Optical Characteristics 57 3.4 Elemental Analyses 61 3.4.1 X-ray Photoelectron Spectroscopy (XPS) 61 3.4.2 Energy Dispersive X-ray Spectroscopy (EDS) 66 3.4.3 Raman Spectrum 68 Reference 70 Chapter 4 Fabrication and Characteristics of ZnGa2O4 MSM Photodetector 72 4.1 Fabrication of ZnGa2O4 MSM Photodetector 72 4.2 Characteristics of ZnGa2O4 MSM Photodetector 73 4.2.1 Characteristics of Different Oxygen Flow Ratios 73 4.2.2 Characteristics of Different Annealing Temperature 80 4.3 Summary 84 Reference 85 Chapter 5 Fabrication and Characteristics of ZnGa2O4 Thin Film Transistor 86 5.1 Fabrication and Measurement of ZnGa2O4 Thin Film Transistor 86 5.2 Characteristics of the ZnGa2O4 Thin Film Transistors 88 5.3 Characteristics of the ZnGa2O4 Phototransistor 94 5.4 Introduction and Fabrication of the ZnGa2O4 TFTs with double-stacked channel layers (DSCL) structure 101 5.5 Characteristics of the bandgap-engineered DSCL structure for high-performance ZnGa2O4 TFTs 102 5.6 Characteristics of the ZnGa2O4 phototransistors with DSCL structure 107 5.7 Summary 111 Reference 112 Chapter 6 Conclusion and Future Work 114 6.1 Conclusion 114 6.2 Future Work 116 Table 3-1. Characterization of ZnGa2O4 thin film with various partial pressure. 49 Table 3-2. RMS roughness of the ZnGa2O4 films with various annealing temperature. 53 Table 3-3. The bandgap of ZnGa2O4 film under different oxygen flow ratios. 58 Table 3-4. The bandgap of ZnGa2O4 film with and without annealing. 60 Table 3-5. OII/O total ratios for various oxygen flow ratios. 62 Table 3-6. EDS analysis of the ZnGa2O4 films. 66 Table 3-7. Calculated Raman modes for ZnGa2O4 . 69 Table 4-1. I-V characteristics of the ZnGa2O4 photodetectors fabricated under various oxygen partial pressure. 74 Table 4-2. The rejection ratio of the ZnGa2O4 MSM photodetectors fabricated with different oxygen ratio. 76 Table 4-3. Time response of the ZnGa2O4 MSM photodetectors with various processing ambience. 78 Table 4-4. I-V characteristics of the ZnGa2O4 photodetectors with various annealing temperatures 82 Table 4-5. The rejection ratio of the ZnGa2O4 MSM photodetectors with different annealing temperatures. 83 Table 5-1. Transfer characteristics of ZnGa2O4 TFTs. 94 Fig. 1-1. Spinel structures of ZnGa2O4. 18 Fig. 2-1. Transitions in the semiconductor under illumination. 30 Fig. 2 2. Structures of the thin film transistor (a) bottom-gate structure and (b) top-gate structure. 32 Fig. 2-3. The momentum exchange process. 36 Fig. 2-4. Schematic diagram of RF sputtering system. 38 Fig. 2-5. Schematic diagram of PECVD. 39 Fig. 2-6. The X-ray diffraction plot. 40 Fig. 2-7. Seven types of crystal systems. 41 Fig. 2-8. Schematic of EDS system. 44 Fig. 3-1. Schematic diagram of the ZnGa2O4 thin film sample. 49 Fig. 3-2. XRD spectra of ZnGa2O4 thin films with different oxygen flow ratios. 51 Fig. 3-3. XRD spectra of ZnGa2O4 thin films with and without annealing. 52 Fig. 3-4. XRD spectra of ZnGa2O4 thin films are annealed at 700oC, 800oC, and 900oC . 52 Fig. 3-5. AFM images of surface morphology of ZnGa2O4 thin film under different annealing temperature (a)as-deposited, (b) 200oC, (c) 300oC, (d)500oC (e) 700oC. 54 Fig. 3 6. Cross-section image of SEM for ZnGa2O4 photodetectors. 55 Fig. 3 7. The SAED patterns of the ZnGa2O4 film (a) as-deposited (b) annealed at 300oC. 56 Fig. 3 8. Elemental maps of the ZnGa2O4 photodetector. 56 Fig. 3-9. Transmittance spectrum of ZnGa2O4 film as a function of wavelength. 58 Fig. 3-10. Absorption spectrum versus photo energy of ZnGa2O4 film at different oxygen partial ratio. 59 Fig. 3-11. Transmittance spectrum of ZnGa2O4 film annealed at different temperature as a function of wavelength. 60 Fig. 3-12. Absorption spectrum versus photon energy of ZnGa2O4 film at different annealing temperature 61 Fig. 3-13. XPS O1s spectra of ZnGa2O4 thin films with various oxygen flow ratios (a) 0% (b) 2% (c) 4% (d) 6%. 63 Fig. 3-14. XPS full spectra of ZnGa2O4 thin films with oxygen flow ratio of 0%. 65 Fig. 3-15. Cross-section image of the ZnGa2O4 film under different oxygen flow ratio 67 Fig. 3-16. EDS analysis for ZnGa2O4 thin films different oxygen flow ratios (a) 0% (b) 6% 67 Fig. 3-17. Raman spectra of ZnGa2O4 films under different annealing temperature. 68 Fig. 4-1. Schematic structure of ZnGa2O4 MSM photodetector. 73 Fig. 4-2. I-V characteristics curve of ZnGa2O4 MSM PDs measured(a)with oxygen flow ratio of 0% measured in the dark in linear scale;(b) with various oxygen flow ratio in the dark and under illumination. 75 Fig. 4-3. Photoresponsivity of the ZnGa2O4 MSM photodetectors with various oxygen partial pressure. 77 Fig. 4-4. Time-dependent photoresponse of the ZnGa2O4 photodetectors with various oxygen partial pressure for 3 cycles (a) 0%, (b) 2%, (c) 4%. 80 Fig. 4-5. I-V characteristics of ZnGa2O4 MSM photodetectors with various annealing temperatures. 82 Fig. 4-6. Photoresponsivity of ZnGa2O4 MSM photodetectors with various annealing temperatures. 84 Fig. 5-1. Schematic diagram of ZnGa2O4 TFT (a) cross-section; (b) top-view. 88 Fig. 5-2. Output characteristics of ZnGa2O4 TFTs with various active layer thicknesses. (a) 10 nm, (b) 20 nm, (c) 30 nm, (d) 50 nm. 91 Fig. 5-3. Transfer characteristics of ZnGa2O4 TFTs with various active layer thicknesses. (a) 10 nm, (b) 20 nm, (c) 30 nm, (d) 50 nm. 93 Fig. 5-4. Transfer characteristic of ZnGa2O4 phototransistor in the dark and under illumination. 96 Fig. 5-5. Output characteristic of ZnGa2O4 phototransistors before and after illumination. 96 Fig. 5-6. Schematic energy-band diagram of the ZnGa2O4 phototransistors before and after illumination. (a) thermal equilibrium (VG = 0 V ), (b) VG < Vth , (c) VG > Vth 98 Fig. 5-7 Photoresponsivity of ZnGa2O4 phototransistor. 100 Fig. 5-8. Transient responses of the ZnGa2O4 phototransistor 100 Fig. 5-9. Schematic diagram of ZnGa2O4 TFT with DSCL structure. 102 Fig. 5-10. The Valence Band Maximum (VBM) spectra of ZnGa2O4 films with different oxygen ratios (a) 6% (b) 0%. 103 Fig. 5-11 Energy level of ZnGa2O4 films with different oxygen ratios (a) 6% (b) 0%. 104 Fig. 5 12 Energy band diagram of ZnGa2O4 TFTs when the device was operating at VGS> VFB 105 Fig. 5-13. Output characteristics of ZnGa2O4 TFTs with DSCL structure. 106 Fig. 5-14. Transfer characteristics of DSCL TFTs with and without annealing. 107 Fig. 5-15. Transfer characteristics of ZnGa2O4 TFTs with DSCL structure measured in the dark and under illumination. 108 Fig. 5-16. Output characteristics of ZnGa2O4 TFTs with DSCL structure measured in the dark and under illumination of 240 nm UV light. 109 Fig. 5-17. Photoresponsivity spectrum of ZnGa2O4 TFTs with DSCL structure at gate voltage of -1.8 V. 109 Fig. 5-18. Transient responses of the ZnGa2O4 TFTs with DSCL structure. 110

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