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研究生： 賴臆升
Lai, Yi-Sheng
論文名稱： 金屬氧化物半導體奈米粒子應用於自旋電子量子計算與產氫
Spintronic Polaron Channel Modulator of Metal-Oxide Semiconductor Nanoparticles in 4 Qubits Quantum Computing and Hydrogen Evolution
指導教授： 蘇彥勳
Su, Yen-Hsun
學位類別： 博士
Doctor
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： 2019
畢業學年度： 108
語文別： 英文
論文頁數： 105
中文關鍵詞： 金屬氧化物半導體 、水分解產氫 、極化子表面態 、自旋電子 、量子計算
外文關鍵詞： Metal-oxide semiconductor, water splitting, polaron surface state, spintronic, quantum computing
相關次數： 點閱：109  下載：1 
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    • 為了解決能源危機和環境污染問題，用於綠色能源發電和儲存裝置的水分解太陽能電池被認為是最佳解決方案。
    鹵化色變性質之染料被視為是二氧化鋯奈米粒子之水分解薄膜電池元件最佳的光敏化劑。鹵化色變性質之染料的激發態能階由具有不同pH值的電解質所控制，作為二氧化鋯之導帶到電子遷移至白金電極端的能階。水分解效率可達約為0.236％，且光誘導之水分解的氫氣產生率可高達1.8 mL / h·cm2。
    在接下來的實驗中，採用天然葉綠素分子作為水分解薄膜電池元件最佳的光敏化劑。馬纓丹（Lantana camara）被視為天然葉綠素的來源，在實驗中作為寬能帶之二氧化鋯的光敏化劑，並為二氧化鋯提供激發態電子遷移的能階。化學發光分子紅熒烯和9,10-二苯基蒽酮通過熒光共振能量轉移（FRET）機制和化學發光輻射為塗有天然葉綠素的二氧化鋯提供更多的光子能量，此過程可使得水分解電池元件之水分解產氫效率高達12.77 ％。
    二氧化鈰奈米粒子之表面由許多氧空缺以及鈰離子的氧化還原過程(Ce+3↔Ce+4)中所形成的極化子所覆蓋。透過具備ħ/-ħ角動量圓偏振雷射光之耦合，可產生單一自旋方向之自旋電子。其極化率可高達75％。而此元件應用於水分解產氫之系統，其能量轉換率高達161％。此外，在該電池元件之電路系統中自旋電子的電荷遷移率提高到2.19×1015m2 /（V·s）。從量子計算和量子層析成像的進一步應用來看，相干ħ/-ħ角動量圓偏振雷射從二氧化鈰奈米粒子之極化子表面態產生自旋電子，實現了4量子位量子糾纏和層析成像系統。過程中水分解的能量轉換效率和自旋電子控制系統得到很好的控制，並在不久的將來帶來實際的用處。

    For solving the problems of energy risk and environmental pollutions, water splitting solar cells for green energy generation and storage devices are considered as the best solution.
    Halochromic pigments sever as the photosensitizers of ZrO2 NPs thin films water splitting cells. The excited energy level of halochromic pigments are acting as the energy level steps of the conduction band energy level of ZrO2 for electrons migrating. The water splitting efficiency is around 0.236 % and the hydrogen generation rate from photoinduced water splitting processing is as high as 1.8 mL/h·cm2.
    Lantana camara is utilized as the source of nature chlorophyll which serves as the photosensitizer for wide band gap ZrO2 as the step of energy level for excited energy level transferring. The chemiluminescence molecules rubrene and 9,10-diphenylanthrance provide photon energy by fluorescence resonance energy transfer (FRET) mechanism and chemiluminescence irradiation. The water splitting efficiency is as high as 12.77 %.
    The small polaron surface state covered CeO2-x NPs thin films water splitting cells operator as the spintronic modulator when redox reaction of Ce+3 ↔ Ce+4 from O vacancy and Ce ions corresponding with coherent ħ and - ħ angular momentum circular polarization laser light injection. The spin polarization is as high as 75 %, the energy conversion from water splitting and hydrogen evolution is up to 161 %. Furthermore, the charge mobility of the spintronic in cell circuit is raising up to 2.19×1015 m2/(V·s). From the furthering application of quantum computing and quantum tomography, the coherent ħ and - ħ angular momentum circular polarization laser light generate the spintronic from small polaron surface state covered CeO2 NPs thin films and achieving the 4 qubits quantum entanglement and tomography system. The energy conversion efficiency and spintronics controlling systems of the water splitting is well controlled and give the actual benefits in near future.

    摘要 I Abstract II Acknowledgements IV Contents VI Table caption X Figure caption XI 1. Introduction 1 2. Theoretical concepts 6 2.1 Orbital angular momentum of light (OAM) 6 2.2 Polaron surface state the spintronic modulators 7 2.3 Basic of water splitting 8 2.4 Mechanism of spintronic injection water splitting cell 10 3. Experimental section 12 3.1 Materials 12 3.1.1 Materials for ZrO2 halochromic pigments water splitting system 12 3.1.2 Materials for ZrO2 FRET water splitting system 12 3.1.3 Materials for CeO2 spintronic water splitting system 13 3.2 Fabrication electrode 14 3.2.1 ZrO2 nanoparticles films matrixed electrode 14 3.2.2 CeO2 nanoparticles films matrixed electrode. 14 3.2.3 Fabrication of Pt films for cathode electrodes. 14 3.3 Pigments coating for anodes electrodes 15 3.3.1 Halochromic pigments coating for anodes electrodes. 15 3.3.2 Nature chlorophyll pigments coating for anodes electrodes. 15 3.4 Electrolytes preparation. 16 3.4.1 ZrO2 halochromic pigments water splitting system. 16 3.4.2 ZrO2 FRET water splitting system. 16 3.4.3 CeO2 spintronic water splitting system 16 3.5 Hydrogen generation from water splitting. 17 3.6 Electrochemical impedance spectroscopy test. 18 3.7 Characterization and experiment equipment. 19 3.7.1 X-ray diffraction (XRD) 19 3.7.2 X-ray Photoelectron Spectroscopy (XPS) 19 3.7.3 Field-emission scanning electron microscope (FE-SEM) 19 3.7.4 Spectrophotometer 20 3.7.5 Electrochemistry analyzer 20 3.7.6 Solar light simulator and laser light source 20 4. Results and discussion 25 4.1 ZrO2 NPs coated with halochromic pigments for hydrogen generation 25 4.1.1 ZrO2 NPs characteristic analyzation 25 4.1.2 UV-vis absorbance spectrum and the excited energy level position of halochromic pigments 29 4.1.3 Halochromic pigments coated ZrO2 NPs water splitting cells and the efficiency 38 4.2 ZrO2 NPs water splitting cell based on FRET phenomena 44 4.2.1 Absorbance spectrum and photoluminescence spectrum analyzation 47 4.2.2 FRET enhanced water splitting cell and the efficiency 54 4.3 CeO2 spintronic water splitting cell for quantum computing 59 4.3.1 CeO2 NPs characteristic analyzation 60 4.3.2 Elemental quantification for CeO2-x surface state 63 4.3.3 CeO2 NPs thin films water splitting cells 65 4.3.4 EIS for CeO2 NPs water splitting cells. 74 4.3.5 Quantum Computing and Quantum Tomography 83 5. Conclusions 89 Reference 91 Author Resume 98 List of Publications 99 Journal publications 99 Seminar publications 101 Awards and Honors 102 Competitions 102 Scholarships 103 Cover Art 104

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