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研究生： 蘇子涵
Su, Tzu-Han
論文名稱： 以溶液法製備鋯鎳酸鎂奈米柱電阻式記憶體之研究
Resistive Switching Behaviors of Magnesium Zirconia Nickel Nanorods by Solution Process for Resistive Random Access Memory
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： 112
中文關鍵詞： 電阻式 、記憶體 、鋯鎳酸鎂 、奈米柱 、溶膠-凝膠法 、水熱法 、燈絲
外文關鍵詞： resistive, memory, magnesium zirconia nickel, nanorod, sol-gel method, hydrothermal method, filament
相關次數： 點閱：92  下載：12 
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    • 本實驗通過使用乙酰丙酮鎳（II）代替鋯酸鎂（MZO）中的乙酰丙酮，利用溶液凝膠法製備鋯鎳酸鎂薄膜做為電阻式記憶體之絕緣層，並已經實現高性能溶膠-凝膠鋯鎳酸鎂基複合材料薄膜電阻式隨機存取存儲器。為有效提高開關行為的穩定性，採用低溫、製成簡單之水熱法製備ITO電極上的鋯鎳酸鎂奈米柱(Nanorods,NRs)作為比較。由FESEM驗證MZN奈米柱約為長10 µm，寬200n，密度約600/mm2 之長方柱，並由EDS mapping鑑定MZN奈米柱之元素組成比。根據不同的製備時間可調整MZN奈米柱薄膜之密度，進而影響元件之電性。Al/MZN NRs/ITO結構呈現雙極性電阻切換行為且為forming-free。與MZN薄膜相比，MZN奈米柱具有較高的開/關比(ON/OFF ratio)與更佳的均勻性(uniformity)。更好的開/關比和均勻性可歸因於MZN奈米柱獨特的幾何形狀導致氧空缺沿著MZN奈米柱的方向形成直線狀可延伸的燈絲。MZN薄膜與MZN奈米柱之切換機制皆為ohmic與SCLC，且再現性高。另外，MZN薄膜亦可應用於二極體，本實驗以驗證W/MZN/ZrO2/ITO具有二極體之電性，且較MIM二極體更為穩定。
    這些結果表明MZN 應用範圍極廣，涵蓋RRAM、diode、並可於未來將RRAM 與diode整合成1D1R結構以期解決3D cross bar array中的漏電問題。

    To effectively improve the uniformity of switching behavior in resistive switching devices, the magnesium zirconia nickel (MZN) nanorods (NRs) on ITO electrodes using the low-temperature and easy fabricated hydrothermal method will be presented. The field emission scanning electron microscope (SEM) image shows the formation of the nanorods, which were 10 µm long, 200nm wide cuboid, and density is around 600/mm2. The Energy Dispersive Spectrometer (EDS) mapping has confirmed the element composition of the MZN nanorods. According to different process time, the density of MZN nanorods can be modified, which will also influence the electrical characteristics of the devices. The Al/MZN nanorods/ITO structure exhibits the forming-free and bipolar resistive switching behavior. Compared to the MZN thin film, MZN nanorods has relative higher ON/OFF ratio and better uniformity. The better ON/OFF ratio and uniformity can be attributed to the distinct geometry of MZN nanorods leads to the formation of straight and extensible conducting filaments along the direction of MZN nanorods. The switching mechanism of both MZN thin film and MZN nanorods RRAM devices are ohmic in LRS and SCLC in HRS, which are highly reproducible. Additionally, MZN thin film can also apply in MIM diode. The diode electrical characteristics of the W/MZN/ZrO2/ITO structure has been demonstrated, which is more stable than MIM diodes. These results suggest that MZN material has a wide range of application, include RRAM, diode, and 1-diode-1-resistor fabricated from combining diode and RRAM to solve the sneak-path current in the 3D cross bar array.

    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 Motivation 3 1.3 Organization of thesis 6 Chapter 2 Literature Survey 7 2.1 Introduction of non-volatile memory 7 2.2 Emerging non-volatile memory 7 2.2.1 Magnetic RAM (MRAM) 7 2.2.2 Ferroelectric RAM (FeRAM) 9 2.2.3 Phase Change RAM (PCRAM) 10 2.2.4 Resistive Random-Access Memory (RRAM) 11 2.3 Resistive Random-Access Memory (RRAM) 12 2.3.1 Resistive switching behaviors 12 2.3.2 Storage media 14 2.3.3 Carrier conduction mechanism 15 2.3.4 Resistive switching mechanism 24 2.4 Fabrication of nanostructures 30 2.4.1 Vapor–liquid–solid method (VLS) 31 2.4.2 Thermal evaporation 32 2.4.3 Anodic Aluminum Oxide (AAO) 32 2.4.4 Hydrothermal method 33 2.5 Sol-Gel Method 35 Chapter 3 Experiment 38 3.1 Fabrication equipment 38 3.1.1 Radio Frequency Sputtering (RF Sputtering) 38 3.1.2 Spin coater 38 3.1.3 Vacuum oven 39 3.2 Material analysis equipment 41 3.2.1 X-ray diffraction (XRD) 41 3.2.2 X-ray photoelectron spectroscopy (XPS) 42 3.2.3 Scanning electron microscopy (SEM) 43 3.2.4 Energy-dispersive X-ray spectroscopy (EDS) 44 3.2.5 Focused ion beam (FIB) 46 3.3 Electrical analysis equipment 48 3.3.1 Current-voltage (I-V) measurement 48 3.3.2 Retention characteristics 48 3.3.3 Endurance characteristics 48 3.4 Sol-gel process 48 3.4.1 Experimental materials 49 3.4.2 Solution fabrication 53 3.5 MZN thin film RRAM device fabrication 55 3.5.1 Substrate cleaning 56 3.5.2 MZN storage media deposition 57 3.5.3 Top electrode deposition 57 3.6 MZN nanorods-based RRAM device fabrication 58 Chapter 4 Results and Discussion 61 4.1 Pure MZN-Based RRAM Electrical and Physical Properties 61 4.1.1 Resistive switching properties of Al/MZN/ITO/Glass 61 4.1.2 Curve fitting 62 4.1.3 Uniformity 64 4.1.4 Data retention 65 4.1.5 Endurance 65 4.1.6 Temperature variation 66 4.1.7 X-ray Photoelectron Spectroscopy of MZN film 66 4.1.8 Focused ion beam (FIB) and thickness of MZN film 67 4.2 MZN nanorods film Physical Properties 76 4.2.1 Scanning Electron Microscope (SEM) of MZN nanorods film 76 4.2.2 Energy dispersive Spectroscopy (EDS) of MZN nanorods film 76 4.2.3 X-ray diffraction (XRD) of MZN nanorods film 77 4.3 MZN nanorods-based RRAM Electrical Properties 83 4.3.1 Resistive switching properties of Al/MZN nanorods-based/ITO 83 4.3.2 Curve fitting 84 4.3.3 Uniformity 86 4.3.4 Data retention 87 4.3.5 Endurance 87 4.3.6 Temperature variation 87 4.4 Resistive switching mechanism analysis 95 4.4.1 Resistive switching model of MZN thin film 95 4.4.2 Resistive switching model of MZN nanorods-based thin film 98 4.5 Diode 100 4.5.1 Single layer insulator diode (MIM diode) 100 4.5.2 Bilayer insulator diode (MIIM diode) 101 Chapter 5 Conclusions and Future prospects 104 5.1 Conclusions 104 5.2 Future prospects 105 References 107

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