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研究生： 李祐安
Li, Yu-An
論文名稱： 以溶液式製備鋇鈦酸鎳奈米結構於電阻式記憶體之應用
Barium Titanate Nickelate Nanostructured Materials Prepared Using a Solution Process for Resistive Random Access Memory Application
指導教授： 王永和
Wang, Yeong-Her
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： 92
中文關鍵詞： 雙極性 、電阻式轉換 、記憶體 、奈米柱 、水熱法
外文關鍵詞： bipolar, resistive, memory, nanorod, hydrothermal method
相關次數： 點閱：49  下載：3 
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    • 本篇研究成功使用水熱法成長鋇鈦酸鎳奈米柱應用於非揮發性電阻式記憶體。過程首先採用低溫製程技術在ITO/玻璃基板上製備非晶BTN奈米柱薄膜做為晶種層，使用溶膠凝膠製程可以有效且輕鬆的掌控化學元素，並且薄膜可以擁有更高的氧空缺密度，使其不需要額外的forming電壓。水熱法成長過程利用不同時間以及溫度上的變化，來調變奈米柱的長度以及密度，進而達到提升電性的目標，其中無需任何複雜的製程即可完成，能有效減少製造時間並降低成本效益。我們在本次研究中成功的觀察到在浸泡溫度50°C，時間為72小時後，可以觀察到BTN奈米柱的形成。透過SEM分析可以觀察到奈米柱的形狀為長柱狀，長度約為30um，寬度為600~700nm，密度為3500#/mm2的奈米柱分布。而EDS mapping以及XPS分析也可以證明其奈米柱中元素確實為本實驗材料所組成。
    在奈米柱成長後，大多數的氧空缺會存在於奈米柱的graind boundaries [1][2][3]，增加了氧原子在此的快速移動和晶界中的導電率[4]，在奈米柱膜層中增強電場，讓氧空缺可以容易的在晶界處遷移[1][4]，因此，奈米柱表面變成了氧原子貯存器的重要作用。在本次實驗中，首次以水熱法生長BTN奈米柱成功應用在RRAM，不需要forming電壓下即可以達到開關比達105以上，在開關週期達到90個週期以上，retention也能達到104，並且HRS的變異係數也成功的從76%提升到48%，LRS的變異係數也能維持在12%，相較於傳統BTN應用於RRAM的元件，set和reset電壓也有效的降低且具有較小的分布，而兩者的元件HRS皆由空間限制電流SCLC以及LRS為歐姆機制所控制。

    Barium titanate nickelate (BTN) nanorod (NR)-based resistive random access memory (RRAM) was demonstrated using the hydrothermal method. The prepared BTN NR materials have the advantages of ease of fabrication, low temperature application, ability to grow various materials, and relative cost effectiveness. In addition, the BTN NR-based RRAM displayed highly repeatable, forming-free bipolar resistive switching behavior with an ON/OFF ratio of over 105. The resistive switching behavior may be related to the oxygen vacancies on the surface of the BTN NRs, giving rise to the formation of straight, extensible conducting filaments along each vertically aligned BTN NR. As compared to its BTN thin film counterpart, superior reproducibility was also observed, demonstrating that the nanostructured material provides an effective way to improve memory properties.

    摘要 I Abstract III 誌謝 V Contents VII Figure Captions X Table Captions XII Chapter 1 Introduction 1 1.1 Background 1 1.2 Non-volatile memory categories 7 1.3 Basic definitions of RRAM 8 1.3.1 Resistive switching phenomena 10 1.3.2 Resistive switching mechanism 11 1.3.3 RRAM Issues 12 1.4 Motivation 13 1.5 Organization of the Thesis 17 Chapter 2 Literature Review 18 2.1 The nano-material growth mechanism 18 2.1.1 VS (vapor-solid) method 18 2.1.2 VLS (vapor-liquid-solid) method 18 2.1.3 SLS (solid-liquid-solid) method 19 2.2 Methods used to grow nano-materials 22 2.2.1 Metal organic chemical vapor deposition (MOCVD) 22 2.2.2 The thermal evaporation method 22 2.2.3 Hydrothermal method 23 Chapter 3 Experiment 26 3.1 Sol-gel process 26 3.1.1 Principle of the Sol-gel method 26 3.1.2 Experimental materials 27 3.1.3 Solution fabrication 32 3.2 Fabrication equipment 34 3.2.1 Spin coater 34 3.2.2 Hot plate/Magnetic stirrer 34 3.2.3 Oven 35 3.2.4 Sputtering 35 3.3 Measurement equipment 39 3.3.1 X-ray diffraction (XRD) 39 3.3.2 X-ray photoelectron spectroscopy (XPS) 40 3.3.3 Scanning electron microscope (SEM) 40 3.3.4 Focused ion beam (FIB) 42 3.4 Electrical analysis equipment 43 3.4.1 Current-voltage (I-V) measurement 43 3.4.2 Retention characteristics 44 3.4.3 Endurance characteristics 44 3.4.4 Resistance-Temperature (R-T) Measurement 44 3.5 Experimental procedures 44 3.5.1 Device fabrication of Al/BTN/ITO structures 44 3.5.1.1 Substrate cleaning 45 3.5.1.2 BTN storage media deposition 46 3.5.1.3 Top electrode deposition 46 3.5.2 Device fabrication of the Al/BTN-NRs/ITO structures 48 Chapter 4 Results and Discussion 50 4.1 Physical properties of the BTN thin film and BTN-NRs films 50 4.1.1 Crystal structure analysis 50 4.1.2 Chemical compositional analysis 50 4.1.3 Thickness and surface morphology 51 4.1.3.1 SEM morphology images 51 4.1.3.2 EDX data 51 4.1.3.3 FIB cross section image 52 4.2 Electrical properties of BTN thin film/nanorod RRAM 60 4.2.1 I-V measurement 60 4.2.2 Conduction mechanism 62 4.2.3 Uniformity 63 4.2.4 Endurance 64 4.2.5 Data retention 64 4.2.6 Dependence between pattern size and current 65 4.2.7 Resistance-Temperature characteristics 66 4.3 Comparison 78 4.4 Resistive switching mechanism analysis 79 4.5 Diodes analysis 81 Chapter 5 Conclusions and Future prospects 84 5.1 Conclusions 84 5.2 Future prospects 85 References 86

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