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研究生: 吳佳臻
Wu, Chia-Chen
論文名稱: 海膽狀金奈米粒子與氧化物半導體異質接面之表面電漿共振效應與轉換效率結合人工智慧機械學習法建立材料特性預測模組之研究
Transfer Efficiency of Surface Plasmon Resonance between Sea-urchin-like Gold Nanoparticles and Oxide Semiconductor Predicted by Machine Learning of Artificial Intelligence
指導教授: 蘇彥勳
Su, Yen-Hsun
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: 2020
畢業學年度: 108
語文別: 英文
論文頁數: 104
中文關鍵詞: 機械學習海膽狀金奈米粒子成核於花狀氧化鋅之金奈米粒子基因演算法類神經網路
外文關鍵詞: sea-urchin-like gold nanoparticles, Au-decorated ZnO nanoflower, light-to-plasmon, algorithm neural network (GANN)
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  • 機器學習探索材料之特性,並優化合成過程是材料科學發展之主軸。在本研究中,使用基因演算法並結合類神經網絡(GANN),並利用此套演算法對海膽狀金奈米粒子進行表面電將子之活動進行預測並透過所建立之模型對海膽狀金奈米粒子之形貌進行調控。在海膽狀金奈米粒子之調控中,首先利用較低量級的實驗數據驗證了預測模型的準確性,再利用大量的實驗數據證實了預測模型的準確性。了解到此演算法對實驗的優化以及預測有所幫助,本研究中將基因演算法並結合類神經網絡應用於預測氧化物半導體異質接面之共振特性及預測轉換效率,亦得到良好的預測。因此,基因演算法結合類神經網絡具有良好的預測能力,不論是對表面電將共振位置及吸收峰之相關訊息。均方根誤差(RMSE)和回歸線(Regression Line)有助於分析訓練模型的準確性。最後,我們使用TEM和SEM圖像來確認合成產物之形貌,並使用UV-vis測量合成產物的表面電將共振位置。結果表明,利用GANN 所建立之預測模型,我們不僅可以很好地預測電漿共振,並可以優化合成過程以減少化學廢棄物。通過晶種二次成核法結合人工智慧機械學習(Artificial Intelligence-Machine Learning),可調控之海膽狀金奈米粒子及成核於花狀氧化鋅之金奈米粒子已應用於環保替代能源之發展。此外,透過二次成核法,本研究成功將海膽狀金奈米粒子及其雙層衍生結構自組裝於不同氧化物半導體,提升金奈米粒子與氧化物半導體異質接面之應用領域。

    Due to a complexing nucleation of sea-urchin-like Au NPs and the need of a precise predication of its surface plasmon, artificial neural network is utilized with genetic algorithm to comprehend the relationship between synthesis parameters and surface plasmon wavelength of sea-urchin-like Au NPs by seed-mediated growth assisted by machine learning. Herein, low data test is trained by varying the ratio and the concentration of gold seeds, sodium citrate, hydroquinone, and HAuCl4. Moreover, a big data confirmation was established through massive parameter collection from over 684 samples. Thereby, the well-trained genetic algorithm artificial neural network confirmed by a big data can guide a parameter selection for the seed-mediated growth in order to gain the desired surface plasmon wavelength. An optimal model can be obtained after big data evolution, to assist growth method screening of seed-mediated growth of sea-urchin-like gold nanoparticles to achieve a stronger electromagnetic field of surface plasmon. Consequently, machine learning demonstrates an unprecedented advantage, comparing to the empirical science in seed-mediated growth and simulation in surface plasmon prediction, which improves research efficiency and decrease monetary investment. In addition, the performance of sea-urchin-like gold nanoparticles via seed-mediated growth is substantially improved in the visible domain.
    Light-to-plasmon conversion efficiency is an important index affecting by the morphology of nanoparticle, the species of metallic nanoparticles and the distribution of metallic nanoparticles on metal-oxide semiconductors. In this study, different size and different morphology of gold nanoparticles are synthesized, and fabricated on the surface of ZnO nanoflowers. More than 500 experimental parameters are prepared and measured the light-to-plasmon efficiency and plasmon position. The experimental parameters contain precursors, surfactants and UV-treatment time. The understanding of light-to-plasmon and activated plasmon position, especially those far from the coupling state, is relatively limited due to their inherent complexity. Here, genetic algorithm neural network (GANN) is used to build the prediction model with low experimental data containing position of plasmon shifting and light-to-plasmon conversion efficiency. Machine learning (ML) accelerates the fabrication precisely by incorporating all parameters into consideration instead of focusing on one or two parameters in the experimental process. The capability of predicting the target fabrication results has been demonstrated with a successful experimental validation. On the other hand, we can use ML to optimize the synthesized procedure and predict the specific results. In this way, chemical waste can be reduced and explored the characteristics of material more efficiently.
    In addition, through the seed-mediated method, this study successfully assembled sea-urchin-like gold nanoparticles and their double-layer derived structures into different oxide semiconductors, enhancing the application of the heterojunction of gold nanoparticles and metal-oxide semiconductors.

    摘要 i Abstract ii Acknowledgement iv Table of Contents v List of Tables viii List of Figures ix Chapter I : Introduction and Motivation 1 1-1 General Introduction 1 1-2 Motivation 7 1-3 Objectives of Study 8 Chapter II : Literature Review 9 2-1 Machine Learning 9 2-1.1 Artificial Neural Network 11 2-1.2 Genetic Algorithm 13 2-2 Characteristic of Gold Nanoparticle 16 2-2.1 Gold Nanoparticle 16 2-2.2 Surface Plasmon Resonance 18 2-3 Characteristic of ZnO 20 2-3.1 Structure of ZnO 20 2-3.2 Optical Characteristic of ZnO 21 Chapter III : Experimental Section 22 3-1 Material 22 3-2 Experimental Process 24 3-2.1 ITO Cleaning 26 3-2.2 Preparation of Gold Colloid 27 3-2.3 Preparation of Sea-urchin-like AuNPs 28 3-2.4 Preparation of ZnO Nanoflowers 30 3-2.5 Preparation of Au-decorated ZnO 31 3-3 Characterizations 32 3-3.1 High Resolution Scanning Electron Microscope 32 3-3.2 Transmission Electron Microscope 34 3-3.3 UV-visible Spectroscopy 34 3-3.4 X-ray Diffractometer 35 Chapter IV: Results and Discussion 37 4-1 Shaped Control Sea-urchin-like Gold Nanoparticles by Machine Learning 37 4-1.1 Decision Flow 37 4-1.2 Low Data Test 40 4-1.3 Prediction Section 41 4-1.4 Big Data Confirmation 42 4-2 Evaluating Surface Plasmon Resonance of Metal Nanoparticles Coated on ZnO Nanoflowers by Genetic Algorithm Neural Network Machine Learning 55 4-2.1 Characteristics 55 4-2.2 Decision Flow 58 4-2.3 Algorithms Comparison 61 4-2.4 Prediction Section 63 4-2.5 Confirmation 66 4-3 Application of UV-direct Deduction and Seed-mediated Growth in Oxide Semiconductor 71 4-3.1 UV-direct Deduction in TiO2 Nanorods 71 4-3.2 Seed-mediated in ZTO Thin Film 77 4-3.3 Seed-mediated Coupling with Self-assembles in ZTO Thin Film 80 Chapter V: Conclusions 90 5-1 Shaped Control Sea-urchin-like Gold Nanoparticles by Machine Learning 90 5-2 Evaluating Surface Plasmon Resonance of Metal Nanoparticles Coated on ZnO Nanoflowers by Genetic Algorithm Neural Network Machine Learning 91 5-3 Application of UV-direct Deduction and Seed-mediated Growth in Metal-Oxide Semiconductor 92 References 93

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