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研究生： 賴文鋒
Lai, Wen-Feng
論文名稱： 利用薄膜沉積技術製作突狀結構應用於具有圖樣化電極的染料敏化太陽電池
Application of protrusive structures made by thin-film deposition technique on dye-sensitized solar cells with patterned electrodes
指導教授： 許渭州
Hsu, Wei-Chou
共同指導教授: 黃家逸
Huang, Chia-Yi
學位類別： 博士
Doctor
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： 2023
畢業學年度： 111
語文別： 英文
論文頁數： 122
中文關鍵詞： 染料敏化太陽電池 、磁控濺鍍 、突狀週期結構
外文關鍵詞： dye-sensitized solar cells, magnetron sputtering, periodic protruding structures
相關次數： 點閱：81  下載：30 
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    • 在傳統磁控濺鍍系統中，電漿產生的離子會持續轟擊靶材，所形成的材料蒸氣會以幅射狀擴散方式附著在試片基板表面，並經由核核過程逐漸聚集而形成薄膜，但此種蒸氣的擴散方式並不易在高深寬比的結構上沉積完整薄膜。本論文所開發的磁控濺鍍系統，藉由改良真空腔體的內部機構設計，包含氣體導流技術與靶材對向配置，可產生「聚焦式電漿分佈」，使本系統能夠在高深寬比的突狀結構上沉積高度完整性薄膜。實驗中先以微影製程製作週期性突狀結構，再使用改良式磁控濺鍍系統個別沉積二氧化鈦薄膜與鉑金屬薄膜，最後將光阻移除後即可留下高度完整性的突狀週期結構，其結構高度為90奈米、線寬為15微米、週期為60微米，以及線長為5毫米。將二氧化鈦突狀週期結構應用於染料敏化太陽能電池之光電極，從實驗數據中顯示二氧化鈦與透明導電電極間的接觸阻抗有明顯降低，且電子生命週期也有增加，表示相較於傳統零維度奈米粒子結構，二氧化鈦突狀週期結構可提供激發態電子特定傳遞路徑，降低電子再結合率，使電子傳導至電極外部的效率增加，進而使得光電流從1.78 毫安培明顯上升至2.26 毫安培。基於光電極使用二氧化鈦突狀週期結構，同時將鉑金屬突狀週期結構應用於染料敏化太陽能電池之對電極，光電流從2.35 毫安培明顯上升至2.60 毫安培，此結果可歸因於鉑金屬突狀週期結構除了可在電解液接面處產生較大接觸面積，有助於電子注入效率，同時產生較明顯的光反射現象，有助於提升元件內部二次光吸收效率，進而提升染料敏化太陽能電池元件之光電流值。預期未來可藉由調整突狀結構參數，進一步優化染料敏化太陽能電池元件之光電效應。

    In traditional magnetron sputtering systems, the ions generated by plasma continuously bombard the target material, and the resulting material vapor adheres to the surface of the sample substrate in a radial diffusion manner, gradually accumulating to form a thin film through a nucleation process. However, this diffusion method is not easy to deposit a complete film on structures with high aspect ratios. The magnetron sputtering system developed in this paper improves the internal mechanical design of the vacuum chamber, including gas flow technology and target opposite configuration, to produce a "focused plasma distribution," allowing the system to deposit highly integrity films on structures with high aspect ratios. In the experiment, periodic protruding structures were first produced using photolithography, and then titanium dioxide thin film and platinum metal thin film were individually deposited using the improved magnetron sputtering system. Finally, after removing the photoresist, a highly integrity periodic protruding structure was left with a height of 90 nm, a line width of 15 μm, a period of 60 μm, and a line length of 5 mm. When the titanium dioxide periodic protruding structure was applied to the photoelectrode of dye-sensitized solar cells, the experimental data showed that the contact impedance between the titanium dioxide and the transparent conductive electrode was significantly reduced, and the electron lifetime was increased. This indicates that compared to traditional zero-dimensional nanoparticle structures, the titanium dioxide periodic protruding structure can provide a specific pathway for excited-state electrons to reduce electron recombination rates, increase the efficiency of electron conduction to the outside of the electrode, and thereby increase the photocurrent from 1.78 mA to 2.26 mA. Based on the use of the titanium dioxide periodic protruding structure in the photoelectrode and the platinum metal periodic protruding structure in the counter electrode of the dye-sensitized solar cells, the photocurrent increased significantly from 2.35 mA to 2.60 mA. This result can be attributed to the fact that the platinum metal periodic protruding structure not only generates a larger contact area at the electrolyte interface, which helps improve electron injection efficiency, but also produces a more significant light reflection phenomenon, which helps improve the secondary light absorption efficiency within the device and thereby increase the photocurrent value of the dye-sensitized solar cell. It is expected that in the future, by adjusting the parameters of the protruding structure, the photoelectric effects of dye-sensitized solar cell devices can be further optimized.

    摘要 i Abstract iii 誌謝 v Contents vi Table Captions ix Figure Captions x Chapter 1 Introduction 1 1.1 Categories of Solar Cells 1 1.1.1 Silicon-based solar cells 1 1.1.2 Dye-sensitized solar cells 3 1.2 Overview of dissertation 5 Chapter 2 Operational Principles of Solar Cell Components 7 2.1 P-N junction in semiconductors 7 2.1.1 Drift current and diffusion current in semiconductor materials 7 2.1.2 Light absorption 9 2.1.3 PN junction under thermal equilibrium 10 2.1.4 Forward bias current of p-n junction 11 2.2 Voltage-current characteristics of solar cells 12 2.2.1 Short-circuit current 12 2.2.2 Open-circuit voltage 13 2.2.3 Fill factor (FF) 14 2.2.4 Power Efficiency 14 2.2.5 Quantum Efficiency 15 2.2.6 Series Resistance and Shunt Resistance in the Field of Semiconductor and Solar Energy 16 2.2.7 Air Mass 17 2.3 Dye-sensitized solar cell (DSSC) 18 2.3.1 Device structure 18 2.3.2 Photovoltaic Conversion Process 19 2.3.3 Dyes in Dye-Sensitized Solar Cells 19 2.3.4 Electron recombination mechanism 20 Chapter 3 Thin Film Deposition Techniques 22 3.1 Plasma 22 3.1.1 Gas atomic structure 22 3.1.2 Formation of plasma 22 3.1.3 Energy transfer in plasma 23 3.1.4 Plasma frequency 25 3.1.5 Plasma characteristic parameters 26 3.1.6 Magnetic force 27 3.2 Plasma System 28 3.2.1 Capacitively coupled 29 3.2.2 Sheath Region 29 3.2.3 Sputtering Deposition 29 3.3 Thin Film Deposition Techniques for Nanostructured Surfaces 31 3.3.1 Magnetron sputtering system 32 3.3.2 Experimental Content 34 3.3.3. Results and Discussion 37 Chapter 4 Study on the Influence of One-Dimensional TiO2 Stripe Array on the Characteristics of DSSC Devices. 41 4.1 Introduction 41 4.1.1 Operating principle of DSSC 41 4.1.2 Issues encountered in electronic transport pathways 42 4.1.3 Patterned electrodes 43 4.1.4 Striped Periodic Structure 43 4.2 Experimental Methods 44 4.2.1 Photoelectrode and Counter electrode 44 4.2.2 Periodic structure of stripe array 44 4.2.3 Porous TiO2 nanoparticle structure 45 4.2.4 Electrolyte Solution 45 4.2.5 Optical Spectral Measurements 46 4.2.6 Measurement of voltage-current characteristics of DSSC devices 46 4.2.7 Quantum efficiency measurement 46 4.2.8 Impedance measurement of DSSC interfaces 47 4.3 Experimental Results and Discussion 47 4.3.1 Measurement and Analysis of TiO2 Stripe Array Periodic Structure 47 4.3.2 Measurement of DSSC Device Characteristics 49 Chapter 5 Study on the Effect of Periodic Spike Structure of Belt-like Platinum Electrodes on the Characteristics of Dye-Sensitized Solar Cells. 53 5.1 Introduction 53 5.1.1 Operating principle of Dye-Sensitized Solar Cells (DSSC) 53 5.1.2 Patterned design of the counter electrode 55 5.1.3 Dye-sensitized solar cells (DSSCs) - Double electrode periodic patterned structure 57 5.2 Experimental method 57 5.2.1 Patterning of periodic photo electrode structures 57 5.2.2 Periodic patterned structure of the counter electrode 58 5.2.3 Porous TiO2 nanoparticle structure 59 5.2.4 Electrolyte solution 60 5.2.5 Measurement of surface characteristics of electrode films 60 5.2.6 Optical spectroscopy measurement 61 5.2.7 Voltage-current characteristics measurement of DSSC devices 61 5.2.8 Quantum efficiency measurement 61 5.2.9 Impedance characteristics measurement of DSSC interfaces 62 5.3 Experimental results and discussion 62 5.3.1 Measurement and nalysis of Pperiodic nanostructures on counter electrode 62 5.3.2 Measurement of characteristics of dye-sensitized solar cells (DSSCs) 64 Chapter 6 Conclusions and Future Work 69 References 110

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